IAEA-TECDOC-362

STUDY OF RADIOACTIVE MATERIALS IN THE

REPORT OF THE FINAL RESEARCH CO-ORDINATION MEETING ON THE STUDY OF RADIOACTIVE MATERIALS IN THE BALTIC SEA ORGANIZED BY THE INTERNATIONAL ATOMIC ENERGY AGENCY AND HEL HELSINKIDN I , 24-28 SEPTEMBER 1984

A TECHNICAL DOCUMENT ISSUED BY THE INTERNATIONAL ATOMIC ENERGY AGENCY, VIENNA, 1986 STUDY OF RADIOACTIVE MATERIALS IN THE BALTIC SEA IAEA, VIENNA, 1986 IAEA-TECDOC-362

Printe IAEe th AustriAn y i d b a January 1986 PLEAS AWARE EB E THAT ALL OF THE MISSING PAGES IN THIS DOCUMENT WERE ORIGINALLY BLANK The IAEA does not normally maintain stocks of reports in this series. However, microfiche copie f thesso e reportobtainee b n sca d from

IN IS Clearinghouse International Atomic Energy Agency Wagramerstrasse 5 0 10 x P.OBo . A-1400 Vienna, Austria

Orders should be accompanied by prepayment of Austrian Schillings 100,- for e for cheque a th f m IAEth f m o n i o n i r Aeo microfiche service coupons orderee whicb y hdma separately MIfroI Se m Clearinghouseth . FOREWORD

The IAEA's activity concerning the radioecology n relatioe Baltii o th a f Se co radiologicat n l safety and environmental protection was initiated in 1980. A Technical Committee was convened at the Agency's Headquarters in Vienna to review the work on radiological investigations under way in the Baltic Sea countries ano discust d a co-operative neer th sfo d e research programme in the Baltic Sea area, which could enhance the evaluation of the long-term behaviour of radionu- clides enterin e Baltith g c Sea, including their transport back to man. Following the recommendations of the Technical Committee, a co-ordinated research programme was initiated in 1981 on the Study of Radioactive Materials in the Baltic Sea. The programme's goals were outlined in the first Technical Committee Meeting (TCM). The results were presented and discussed at the first Research Co-ordination Meeting (RCM) and alse seconth o d Technical Committee Meeting which were hel n i 1982d , Vienna, Austri d 1983an a , Stockholm, , respectively. This document presents an evaluation of the Co-ordinated Research Programme (CRP d som)an e con- clusion d recommendationan s s together wite finath h l reports given by the chief investigators on the activities performed during the entire co-ordinated research programme, from its inception in 1981 to its conclusion (final Research Co-ordination Meeting in , Finland, in September 1984), as well e resultth s f a Intercalibratioo s n Exercisese Th . annually reported release and monitoring data collected for the database are not included in this document. CONTENTS

1. Introduction ...... 7 . 2 Descriptio Baltie areth a f ncao Se ...... 8 . . 3 Source contend san f man-mado t e radionuclide Baltie th a ...... n sci Se 0 1 . 4. Monitoring programmes ...... 11 5. Special studies performed within the framework of the CRP ...... 12 6. Intercalibration ...... 17 P ...... CR resulte e th Th f so . 7 8 1 . . 8 Conclusion recommendationd san s ...... 9 2 .

ANNEXES

1. Research contract agreementd san s ...... 1 3 . Individual reports: 2. ...... 32 . 3 Finland ...... 2 5 . . 4 German Democratic Republic ...... 9 8 . 5. , Federal Republic of ...... 110 6. Norway ...... 3 13 . 7. ...... 141 8. Sweden ...... 152 . 9 Unio Sovief no t Socialist Republics ...... 2 16 . 10. Intercalibration report ...... 176 List of meetings and participants ...... 187 1. INTRODUCTION cleas wa r t I froe beginninth m ge thatth t a , present discharg concentratiod an e n e levelth f o s Whe e Internationath n l Atomic Energy Agency radionuclides, indirect methods had to be used to (IAEA) suggested a co-ordinated research programme achiev e goath e l outlined above e fall-ouTh . t from between the Baltic Sea countries, it was well known nuclear weapons test s howeverha s , mad t i possible e that radiological investigations in the Baltic Sea to measure artificial radionuclides even in the were carried out to a certain extent by all the open sea. Baltic Sea countries. A part of these investigations In evaluatin e radiologicath g l consequences had already been published in different scientific there are a number of factors other than radionuclide papers. However e result, th mos f o t s were given concentration e consideredb o t s , suc s dischargea h s n i national annual reports onld wer n an manyi e y from nuclear facilities, demographic data and consumption case t availablno s n internationaa n o e l level. a foo se y manb df o . In any case, the existing data were not considered The Baltic Sea countries have long traditions sufficient for satisfactory assessments of n océanographii e investigatio e Baltith a f o nSe c area. It was stated that consideration should be e distributioth d transporan n t mechanismf o s given to the océanographie knowledge of the Baltic the different artificial radionuclides in the Sea and to studies going on with regard to non-radio- Baltic Sea active pollutants. dose commitments to man and to other species At its meeting in 1980 the Technical Committee other radiobiological aspects. recommende e IAEth Ao t dtha a co-ordinatet d research programme be established to carry out the co-ordination e studth f f radionuclideo yThereforo m ai e th e s of the most urgent tasks, as follows: o furnist s e e Baltidatwa th th ha an i Se cneede d for intercalibration of sampling and analytical assessment of both individual and collective procedures needed for the monitoring activities radiation doses co-ordination of the radiological monitoring prediction of the long term behaviour of radionu- programme of the Baltic Sea, and clides enterin e Balti th ga owin Se co norma t g l improvemen e exchangth f o tf o informatioe n operations or as a result of accidental releases e radiologicaoth n l studiee Baltith a n i Se sc from nuclear facilities States, including the data of releases into assessmen e radiologicath f o t l impact from the Baltic Sea. such releases from each individual country e environmenth o t f thio t s international water Furthermore e Technicath , l Committee recommended system. that the tasks should be carried out in accordance wit e worth h k planned withi e frameworth n e th f o k convention on the Protection of the Marine Environment 2' ID- 34' 42' of the Baltic Sea Area (Helsinki Convention). •70' 68' 2. DESCRIPTIO E BALTI TH A ARE F SE CO N A

•68' Th a semi-enclosee s Baltii a Se c shallod an d w n whici a hse dissolved substances could remair fo n a long perio f timeo d . This leada greate o t s r -66' accumulation of radioactive materials than in other e Atlantith sea f o s c Basin Baltie a Th wit.Se ch s subregionit transitiod an s n are s i showa n Figi 1 n . -64' together with the drainage areas of the rivers dis- charging into it. Tables I and II give the dimensions and water balance terms of the Baltic Sea.

TABLE I. Dimensions of the Baltic Sea Area and s subareait s Area Volume km2 km3 Baltic Proper 209 200 0 160 3 Gul f Rigo f a 18 100 410 Gul f Finlano f d 29 600 1 130 Bothnian Sea 0 830 0 4 950 Bothnian Bay 36 800 1 490 54- Baltic Sea total 374 000 21 580 e DanisTh h Straits 43 900 800 (Kattegat+Belt Sea) 52-

e approximatTh TABL . II E e water balance termf o s -52' the Baltia Se c 50'-

Precipitation + 200 -50' Evaporation - 200 10' 14' 18' 26' 30- Inflow through Danish Straits + 433 o 17-19) Fig. 1 The Baltic Sea with its subregions and transition Outflow through Danish Straits - 866 (S°/00 8-9) area. Boundaries between the subregions are marked by dashed lines and boundaries between the drainage basins of the rivers Run-off + 433 discharging into the Baltic Sea are marked by thick lines. The largest rivers discharging into the Baltic o d discharga arean Se :m Nevk 0 ea 10 (are 1 28 a 2 600 m3s~1), Vistula (193 900 / 954), Daugava 87 900 / 688), Neman (98 200 / 674), Kemijoki / 581) 0 540 1 , (10 / 526 0 9d Luleäl50 )an v (25 250 / 477). The mean residence e ewateth th timn i f ro e Baltic Sea has been calculated to be 20 to 30 years. The Baltic Sea water is a mixture of the fresh water received e froprecipitatioe riverth th md an s n and the salt water penetrating from the North Sea. Therefore there is a strong salinity gradient in the Baltic Sea, Fig. 2.

A general feature Baltith a f biotao eSe c , like other brackish-water biotas, is the low number f o species numbeA . f marino r e organismt no o d s penetrate intt e Baltialla th oa .Se c Certain marine specie numberw e Baltie founlo th ar s n n i i cds Proper and their number increases toward e Bela th sSe t but does not reach the North Sea levels. There are not enough freshwater and brackish-water species o compensatt e reductioth r fo e n marini n e species. Fish catches in the Baltic Sea are of the order of 1 million tons per year. The most important species caught in the Baltic Sea are Baltic herring, sprat, cod, flounder and salmon. The s Baltii surrounde a Se c y industrializeb d d countries where some nuclear power plant d othean s r nuclear facilities are in operation or under construc- tion e Tablse , e III. Fig. 2. The salinity (°/oo) of the surface water of the Baltic Sea (average situation) 10 TABL majoEe IIITh r .nuclea r facilitie e Baltith a drainagn i Se sc e area 3. SOURCES AND CONTENT OF HAN-MADE RADIONUCLIDES IN THE BALTIC SEA Sitcountrd ean y Typf o e Capacity In operation Release data installation MWe since available since The potential source f man-mado s e radionuclides in the Baltic Sea are: Loviis I Finlana d PWR 420 1977 1977 II PWR 420 1980 a) The worldwide fall-out from nuclear weapons Olkiluoto I Finland BWR 660 1978 1978 testing. The fall-out products reach the sea II BWR 660 1979 by direct depositio y depositn dr (we r o n t o ) 1 GDR PWR 440 1974 1974 f e frowatee of landth th mn rru . surfacy b d an e 2 PWR 440 1975 3 PWR 440 1978 4 PWR 440 1979 b) Liquid discharges from nuclear fuel reprocessing Forsmark F1 Sweden BWR 900 1980 1980 plants in Western Europe. During the past F2 BWR 900 1980 few years transport of radionuclides from the F3 BWR 1060 1985 s beeha Nort na observedSe h e amounTh s . ha t Oskarshamn 01 Sweden BWR 440 1971 1971 been decreasing, however, since 1980. 02 BWR 570 1974 03 BWR 1060 1985 c) Nuclear power reactors. The discharges from Barsebäc 1 B kSwede n BWR 570 1975 1975 B2 BWR 570 1977 the nuclear power stations have been reported e participatin e th IAE th y b Ao t g countries Ringhals R1 Sweden BWR 750 1975 1975 R2 PWR 800 1975 e CRP th a par f s .o a t R3 PWR 915 1981 R4 PWR 915 1982 d) Other applications of radionuclides. Medical, Studsvik Ener- Sweden Research Institute - 1959 1970 industrial and scientific uses may also contribute gitekniB A k e radioactivth o t e contaminatio e Baltith f co n ASEA-ATOM Sweden Fuel fabrication - 1975 1976 Sea. Industry

Leningrad- I USSR RBMK-1000 1000 1973 1974 From a radiological point of view 1 J3'C7 s is I I skaja 1000 1975 III 1000 1979 the most important man-made radionuclide in the IV 1000 1981 Balti a areaSe c . e BaltiIth n c Prope e dominatinth r g source e fall-outh s i s t C froofm 1nuclea ^7 r weapons testing, mainly during the early sixties. The inventories from fall-out are 670 TBq 137Cs (and 560 TBq 9°Sr). However, inflow throug e Danisth h h Straitf o s 137 Cs s beguwa P e ncountrie th BeforCR mos f e o t th e s from nuclear fuel reprocessing plants in Western had thei programmen ow r r monitorinfo s g bote th h Europe have amounte o approximatelt d q "csTB 0 ,15 y open sea and the coastal waters. The programmes i.e. approximately one fifth of the total 13J7'Cs mostly included wate d sedimenan r t sampleo t d an s inventory, sinc e beginninth ee seventiesth f o g . some extent also biological samples. The nuclides e s recenactivitth C Mos f o t s i preseny n i t 137 investigated were often only " Sr and "'Cs. the Danish Straits and in the western part of the A co-ordinated monitoring programm s discussewa e d Baltic Sea. at the first Technical Committee Meeting. The nuclides 7 1 1 on Discharges of 1 37 Cs from nuclear power reactors e determineb s C o t d dan t r shoulonlS no ye b d have contributed approximatele totath o lt q TB 2 y but also nuclides sucs a h Pu and PÜ1 Am. Also 137 Cs inventor e Baltith a area f o Se yc . This i s e includeds oughb C tritiu o J t t d m.an 1 J34 negligible compare o maidtw n wite sourceth h f o s It was decided that each country should try 137Cs. o follot w those recommendations. Another man-made radionuclide in the Baltic The programme for monitoring work now covers Ses i tritiuma , f leswhico s i h radiological impor- the areas and the different samples shown in Table IV. tanc , ehowever Cs tha e fall-ounTh .13 7t inventory of tritiu s mi approximatel 0 TBqcontribue 00 Th 0 . 14 y - TABL . NumbeIV E f samplino r g site n differeni s t parts tion from nuclear power reactors is approximately of the Baltic Sea 0 TBq00 1 . Water Sediment Seston Fish Aquatic The importance of other artificial radionuclides Plants occurring in effluents from nuclear power reactors commercial s i negligibl n comparisoi e n wite abovth h e mentioned Baltic proper 21-48 12-14 5-10catches radionuclides. and Bela Se t 11 commercial 8-9 catches Kattegat and 4. MONITORING PROGRAMMES Skagerrak 8-35 6-{

The term "monitoring" mean l typeal s f investigao s - Greifswalder tion require n ordei d o obtait r n sufficient knowledge 3 3 Bodden commercial 3 e distributionoth f , behaviour fatd f radionuclidean o e, s catches e Baltiith n c Sea. Gulf of Gdansk 4 4 3-4 A monitoring programme includes investigations performed eithe t regulaa r r interval r continuouslyo s , Gulf of Finland 20 5-7 coverin e wholth g e Balti r parto th e f o cs Sea, with e occurrencregarth o t d distributiod an e f differeno n t Bothniad an a Se n 11 radionuclides. Bothnian Bay 2 2-3 e seeb n n ca fro e s mapth A m s, (Figs5) - 3 . \1 investigation e influencth n o s f differeno e t wate d sedimenan r t sample e same th takear set a n environmental parameters (nutrients, salinity, places by many countries whereas aquatic plant samples water temperature, season, etc.e aforth n e)o are taken in coastal waters and in the surroundings mentioned processes of nuclear power plants. Within their own territorial waters the national researc e transfeth n o h r mechanism factord an s s competent authorities are responsible for the measures withi e differenth n t e foolinkth d f o schai n to be taken (including the necessary investigations) to control the releases from nuclear facilities. investigations on the relevant pathways regarding The recommendation to analyse nuclides other the uptake of radionuclides by marine biota (e.g. on 137 than 7 Sr and J'Cs has also been followed. The ingestion, absorption through gill skind an s , results of the monitoring programmes have been reported absorption or uptake by brackish-water flora). e IAE th n ordei Ao t o t makr e them availablr fo e To facilitat e theoreticath e l consideratiof o n compilation in a data bank. various processe n e relatioBaltii th a n i Se cso t n The result e alsar s o publishe e regulath n i dr e aforth e mentioned studies e Technicath , l Committee reporte differenth f o s t laboratorie institutesd an s . Meeting encouraged further elaboration of the models. From the radiation protection point of view, Testing of models on the dispersion and accumulation t presena s i t ti sufficien o perfort t m radiological processes was encouraged on the basis of available measurements, at given time intervals, at a limited data on numbe f stationo r s coverin e differenth g t parts e opeoth f n Baltic Sea. transport processes interaction processes at interfaces 5. SPECIAL STUDIES PERFORMED WITHIN THE FRAMEWORK (bottom - water - air) P CR E TH F O influence of environmental parameters In addition to monitoring, the Baltic Sea countries equilibrium processes, etc. had already carrie t speciaou d l investigations. The first Technical Committee Meeting on the CRP recommended further research. A special reason Further measurement d modellin an se lon th g f o g for encouraging further research was the need for term behaviou d fat an f rradionuclideo e e Baltith n i cs better understanding of the behaviour of radionuclides Sea environment were also considered necessary. Model- in the event of accidents. ling could be performed including either parts of the Baltic Sea, coastal regions, or open sea, or the Baltic suggestes wa t I d that these studies should include: a whole Ses e modela Th . s e use werb o calcu t o dt e - late dosth e e commitments relatee totath lo t dradioac - research regarding the enrichment factors of ra- tivity present in the Baltic Sea. dionuclides in different marine biota V » ' r i' ' • *> ' - A it' ' - A ' V . ' V t ,'<' •' V t ' - u ' V i ' V t ' l-

Poland USSR O Finland

Power Plant (NPP)

I f I ' I« V I < t ' Il

Fig. 3a. The sampling stations (Poland, USSR, Finland, GDR) for water and the sites of the nuclear power plants. 14

FRG .f. Denmark

I I sampline Th Fig. 3b g. stations (Denmark, FRG water )fo r i- ' tV ' iV ' «V ' if ' iV ' t'r ' rf«- ' »V ' if 1

Denmark GDR Poland o Finland O FRG

»^

« 113- l r 13'r a 1 J' Jo M' ' le * IS ' 'i« I «' 7

Fig. 4. The sampling stations for sediment lY '. M* ' tV ' tV ' iV ' i'r ' it' ' iV ' tarl

• Denmark T Finland

Fig. 5. The sampling stations for aquatic plants. In addition to radiological investigations, the e accumulatioTh f radionuclideo n y biotb sd an a results of other relevant studies in the field of e factorth s affectin e discussear t i g n Annexei d , 3 s physical oceanography, marine chemistry and geology e take. 8 on Eve sf d i nan int 4 o accoun wore n th to k were to be taken into consideration. It was stated accumulation of radionuclides by the Baltic Sea biota that this typ f dats o ealread wa a y available froe th m carrien programmei t ou d s other thae presenth n t CRP, ongoing research work being carried out elsewhere. n concludca e on e that further studie e desirablear s . e interestTh possibilitied an s differene th f o s t Modelling wors onlha ky been started (e.g. Annex laboratories determine choice th d f researceo h projects 3) within the CRP. Models have, however, been devel- e carrietb o t withiou de framewor th ne CRPth . f o k e authorizatioope th s para df o t n procedure n couni s - The short time period and the resources available re- tries using nuclear energy e presenTh . t levelf o s stricted the fulfillment of all the recommendations radionuclides discharged from nuclear facilities around made by the Technical Committee. However, essential t offeth no y particularle o an rBaltid a Se c y good pos- studies have been carrie t witou d h basie regarth co t d sibilitie o verift s e dispersioth y - accumulation n information neede o predict d d calculatan t e radiation - dose models. Only very local phenomena can be veri- o radioactivt e du n dosema e o contaminatiot s e th f o n fied around the nuclear power plants. Releases from Baltic Sea. the reprocessing plant n westeri s n Europe have instead e maiTh ne researcareath f o s h projects have been mad t possibli e o calculatt e e transfer coefficients transport of radionuclides into and out of the for certain radionuclides. Baltic Sea Analytical methods have also been developed within factors affectin e accumulatioth g f radionuo n - the framewor e CRPth , f o Annek . 8 x clides into biot d sedimentan a s modelling developmen f analyticao t l method r radionufo s - 6. INTERCALIBRATION clides of interest which have not yet been stud- ied. e TechnicaTh l Committee, recognizin e importh g - tance of analytical quality control in co-operative research involving environmental radioactivity measure- Transpor f radionuclideo t s inte Baltith oa Se c ments, requested the Monaco Laboratory to provide such from nuclear fuel reprocessing plants in western Europe services to the laboratories in the Baltic Sea has been studied by several authors (Annexes 2, 5, . Thes9) d ean studie8 s- folloween e th e fat f th do e countries participatin e CRPth . n i g Four intercalibration exercises were organized hanced releases from Sellafield , durin UK ,perioe th g d 1974 _ 1981. during the period 1981 - 84, using two sea water samp- les of different salinity and of different radionuclide Transport of fall-out radionuclides via precipita- contents e sedimen,on te seaweesamplon d an ed sample. tiod rivean n re differenwateth o t r t water masses The sample codes and the array of the radionuclides 17 is also discussed by several authors, Annexes 3, 4, 5 and 9. measured are shown in Table V. TABL . V EIntel-calibratio n exercises performed during and certain other gamma-emitting radionuclides. Analy- the CRP ses of transuranium elements still present some prob- high sali- lem o certait s n laboratorie t thosbu s e which hav- al e nity Baltic Baltic sediment sea water sea water seaweed ready gained experienc n suci e h measurement n meaca s - SD-N-1/1 SW-N-2 SW-B-1 AG-B-1 sure them reliably at extremely low levels. No se- rious deviations were observed in cases where the refer- Principal ence values were known. The participants have thus radionuclides: proved their competenc n providini e g reliabl d comean - 241 Am X XXX parable datr monitorinfo a g purposes. 239,240 pu X XXX A full account of the intercalibration exercises 238 Pu X XXX is given in Annex 10. 137 Cs X XXX

9°sr X XXX 60 Co X X 54 Mn X P CR E RESULT E TH TH F . O S7 65Zn X Transport of the radionuclides into the Baltic Radionuclides less Sea frequently reported: naturally occuring The ratio 137Cs/9°Sr in the Sellafield discharges radionuclides x (Ra) x (Ra) x (40K) e globath n i l6 compare 6 1. fall-ou 1. ± o 6 t di 9. st 1Cs x from nuclear weapons tests. This, together with the 99Te X information on the presence of 1J 3 4Cs, allows one to X differentiate between the Sellafield 1 -"C37 s and that from global fall-out transfee Th . r factors from Sella- e Danisth fiel o t hd Straits were calculatee b o t d Eleven laboratories froe seveth m n Baltia Se c q (dischargePB r pe 3 dm~ froq arounB m 0 1 Sellafieldd ) countrie e Monacth d oan s laboratory participaten i d a 1 for 137 Cs and surface water. For bottom water it these exercises providing data on one or more of the was around 30 Bq m~3 per PBq (discharged) a . For radionuclides listed in Table V. The overall percent- e valueth r S *s were nearly twic s higa e h (Anne. 2) x age of submitted results was very high, amounting to 13J'C7 s originating froe Sellafielth m d works wa s 91 %. observed in the Deep firstly in 1980 (Annex The result of the intercalibrations was very sat- n Fucui contente c Th s "T spp . f o s5) . suggest that QQ isfactory. The percentage of values loaded with unac- the Sellafield originated radionuclide y havma s e reach- ceptably high erro s negligiblwa r ye grousmalth n pi l ed the southern part of the Swedish East coast (Annex f commonlo y analysed elements, suc s 9C>Sra h , 13?Cs 8). Studies based on observations of fall-out radio- Compared wite ratheth h r homogeneous distribution nuolides clearly shoe higth w h proportio f riveo n r r botS o f9 h verticall horizontallyd an y cons C -, e Gul wateth f Bothni o fn i rGuld f an Finlanao f d with centrations show considerable difference n samplei s s low Cs and high ^H values. Caesium is easily bound collected from the Baltic Proper above and below the o clat y particle d removean s d from water, thus decreas- permanent halocline, i.e. from the surface and bottom 1 37 e transporinth g f Jo t'C y riversb s into seae n I th . layers. Thi s evidentli s e recentla resuly th f o t y areas with a high sedimentation rate, 1 37Cs is effec- increased activity concentratio f Jo n'C s 1foun 37n i d tively deposited on the sea-bed (Annexes 2, 3, 4, 5, the saline water flowing into the Baltic Sea through 7, 9). the Danish Straits, as seen from the high correlation 1 07 Several papers discuss the correlation between between J'Cs concentration and salinity in the transi- 137 d salinityan s •"C , which reflect e mixinth s f differo g - tion zone. ent water masses in the Baltic Sea. As a result of this phenomenon a decrease in the concentration of 137Cs can be observed from the Katte- gat throug e Danishth e hnorther th Strait o t p nu s part Radionuclide concentrations in water of the Bothnian Bay. The tritium activity concentra- tions, however, shoe oppositth w e distribution, with The participants of the CRP have presented data high values in the low salinity water of the Bothnian e activitoth n y levele th 9f °Sr o sn i , H 1373 d Csan Bay and low ones in the high salinity water in the Q Q M -13 water. Figure alse ar so availabl "Ter , fo eCs ,J Kattegat. 11 ,d Figsan 0 1 . 239'240Pu and241 Am. The activity concentrations of 0 '-po24 q17 ' "Pu are also best The values obtained from samples taken at the presented using the values given in Fig. 12. Higher same plac y differenb e t laboratories comply very well values can be observed in the bottom water of the Kat- with each other. The most recent data and the data tegat and the Danish Straits as well as in the Bothnian covering the widest area are those presented in Annexes Bay. A much lower activity concentration was found 5 and 7. The maps presented in Annex 5 are used here e Baltiith n c e GulPrope th f Finland fo d an r . to give an overview of the activity concentrations of 90Sr, 137Cs, 3H and 239'240Pu, Figs. 6 - 12, (taken from Anne. 5) x As can be seen from Figs. 6 and 7 the " Sr level in 198nearls 3 wa e sam th n botyi e h surfac d bottoan e m water ovee entirth r e Balti a areaSe c . Measurements of 137Cs have been carried out by many institutes but the results from the R.V. Gauss expedition provide the best overall picture of the present situation, Figs. 8 and 9. 19 20 18.1 IS.b ÎÎJD 21.f- 19.9 JO.O 20.1 ÄS

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"Results in nus: pagafed etvot I'M% in bmckets Radionuclide concentration n sedimeni s t n contaianca d n higher activity levels than sediments of open sea areas, Table VI (Annexes 2, 3, 4). As the sedimentation rate varies in different The results presented by the participants in the parts of the Baltic Sea the deposition of radionuclides CRP comply well with each other concerning the activity concentration f differeno s t nuclides, even thouge th h TABLE VI. Approximate contents and ranges of radio- samples were taken with different type f equipmento s . 2 nuclide n sofi s t bottom sedimentm r pe s , howeveris t I , diffucul o compart e resultth e s a s in differen a area- se t pe sP durinCR e th g the value e give r ar ssedimen fo n t layer f differeno s t thicknesses 0-1,0-3,0- 0-1d an 5 . Dat0cm a riod . O 5 f\ on naturally occurring radionuclides such as Ra Amount r unipe s 2 t aream~ q B , have been reported (Annex 4, 7). The activity level a areSe a 90Sr 137Cs 239,240pu in sediment e Southerth f o s n Balti a lieSe c s between m layec 5 r - (Anne 0 . e 7) x th q kg- B n i 10 5 d an 0 3 Gul f Bothnifo a Bothniay Ba n There is apparently also a variation in the activity open sea samples 77-79 478-890 41-117 levels depending on the type of sediment. This can river mouths 36-140 590-2700 115-231 be seen in the data in Annex 5 in which values between Bothnian Sea 2.2 and 85 Bq kg-1 dry weight are reported. opea samplese n s 55-87 1390-3100 52-135 coasts and river mouths 41-210 1700-12500 33-252 Radionuclide concentrations in biota Gulf of Finland opea samplese n s 31-190 165-4470 26-283 Data on different radionuclides in biota have coast d rivean s r been reporte e monitorin th s para df o t g programmes, mouths 28-230 700-8000 31-190 and also as part of special investigations. Gul f Rigo f a 1550 e greatesTh t amoun f dato ts reporte i a d regar- Baltic Proper ding aquatic plants in particular Fucus spp. (Annexes open sea samples 38-73 160-1730 23-48 2, 3, 4, 6, 8) but data on other algae and higher coastal areas 15-38 170-1260 36-46 plants are also given (Annexes 4, 7). Danish straits 99-5200 The concentration of 1 37Cs in Fucus is found to vary wite seasonth h . Representative date givear a n e regioth r nfo alon e Norwegiath g n South coast with values between 10.2 and 16.9 Bq kg-1 (1983) and along also varies. The soft bottom will often act as a sink the Swedish coasts 11.8 - 13.8 Bq kg-1 (1983). The e nuclideth r fo s wherea e harth sd bottom e regardear s d data reported from the Danish Straits vary from 5.1 to as transport bottoms with very low accumulation of 13.2 Bq kg"1 dry weight and along the Finnish coast sedimenting material. River mouth areas are more or y q weightkg-B dr 1 e reporte 1 Th d .betwee an d6 5. n 27 less a combination of erosion and transport bottoms 137 Cs concentrationc Fu n i s vesiculosus froe th m 28 south western e Balticoasth a rangef Se o tc d fro8 7. m it to reflect the dispersion of radionuclides on a weighy dr tot g 12.k (Anne q . 2B 4) x large scale. On the other hand it adequately reflects The 3'Cs content in other plants from the south- the local dispersion of releases. er ne Balti coasth a varief Se o tc s d betweean 8 1. n With regard to invertebrates data on molluscs 13.4 Bq kg dry weight (Annex 4). In Annex 6 values from coastal areas are reported in Annexes 3, 4, 8. between 1.8 and 2.9 Bq kg~ dry weight are reported The mean values from different areas are summa- 1 37 for other species. In Annex 7 the -" Cs content in rize n Tabli d e VII. other species frosouthere th m ne Balticoasth f o ct q kg-varieB y weight9 1dr 2. s d betwee.an 8 1. n TABLE VII e summarTh . f meao y n radionuclide concentra- Co has also been analysed in Fucus samples from tions in invertebrates from the Baltic the Norwegian South coas d froe Danisan tth m h Straits Sea. and concentrations between 0.25 and 1.6 and 0.33 and 6.14 Bq kg-1 dry weight have been found, respectively. Bq kg ww The special investigation on Q"TQ c revealed that 137Cs 239,240pu 241Am its concentration in Fucus samples from the Swedish East coas s i vert y constant e kg"Sweq th B n -13 O . 1. , Finnish coastal QQ dish West coas e concentratioth t Fucun i c sT f o n areas (Annex 3) 0.016 is influenced by the inflow of water from the North Macoma baltica 14 0.62 0.039 n increasa e concentratiod th an n a i e Se n from about Mytilus edulis 5.5 <0.14 0.0073 0.0046 3 Bq kg-1 in 1967 - 72 to 50 - 150 Bq kg-1 in 1980 flesh 0.2 0.073 0.0025 has been observed (Anne. 8) x shell 22 <0.13 0.033 The average concentration of 23J3Q' 240Pu in Fucus froe Norwegiath m n Sout, " hkg coasq mB abous i t0 13 t GDR coastal areas that froe Swedisth m h Wes d kg~q t an mB coas 1, 0 10 t (Annex 4) 1 that from the Swedish East coast 170 mBq kg . Corre- Mytilus edulis spending values for 241 Am are 14 and 25 mBq kg-11 for flesh 0.3 0.7 the Swedish West and East coasts respectively. shell 15 3.2 24u0 samples froe Finnisth m h coasts shoa w !" pu con- 1 centration between 100 and 300 mBq kg-' and a Am Swedish coastal^ concentration aroun mB5 3 d q kg-1. areas (Anne) 8 x Fucus ves iculosus is the most common indicator Mytilus edulis 0.01 organism used within the Baltic Sea. The results show, - fles0.8h 7 0.05 however, that it accumulates radionuclides to different shell - 0.330.03 0.02 extents in different parts of the Baltic Sea. This and the seasonal variations make it difficult to use 1) These results are based on a ww/dw ratio of 4 for flesh and 1.1 for shell Q 0 1 37 The concentrations of 7 Sr and Cs have been clusions on the advisability of using different concen- determined in the samples of different fish species. tration factor d distributioan s n coefficient r diffo s - 137, The s concentratioC n varies with both specied san ferent parts of the Baltic Sea or on what bases they catching aret liebu as withi e samth n e orde f magnio r - shoul e selectedb d . This shoul e donb ds para ef o t tude from 1 to 6 Bq kg~l fresh weight of edible parts. on future assessment e giveb d nsan high priorit futurn i y e concentratior S Th ' e edibln i n ee partth f o s work. fishes from different areas and in different species Nevertheless , the data collected within the CRP 1 vary between 0.03 and 0.13 Bq kg- fresh weight. concerning the activity contents in fish and in the e accumulatioTh f certaio n n radionuclides from environmen e satisfactorilb n ca t y use o calculatt d e water into fish and other species is reported in An- the dose from radionuclides in the Baltic Sea, from nexes 3, 4 and 8. It has been found that there are both fall-ou d nucleaan t r fuel reprocessing plants. differences in concentration ratios between water and e dosTh e equivalent commitmen n froma mo t thes - ra e certain fish species in different sea areas. Within dionuclide o annuat e du sl consumptio f Baltio n a Se c the t poslimiteno -s wa d t timi P e CR availabl e th r fo e fish is of the order of 1 uSv. Exposure from other sibl o makt e e extensive studie f factoro s s influencing pathways, eg. swimming, boating etc. is very low in these differences, but attempts were made to study comparison, the influenc f salinityeo , organic matter contend tan The doses of the above-mentioned radionuclides 137 particulate matter content in the case of Cs accumu- to other organism o radiologican f o e smal d ar s an l l lation by pike and Baltic herring (Annex 3). Accumula- concern. 1 37 tion of Cs by pike and Baltic herring shows a nega- Small amount f short-liveo s d radionucliden ca s tive correlation with salinity of the water mass in be detected around the nuclear power plants. The ra- question and positive correlation with organic content diation dose from these sources to people living in of the water. the neighbourhood and eating fish caught locally may e influencTh e potassiuth f o e m conten f wateo t r r yearpe v . uS e Thiorde1 th sf o f o ro tw dos s e i b e 1 37 on Cs uptake is discussed in Annex 4. order f magnitudo s e lower thae dosth n e receivey b d everyone from natural potassium-4 s bodyhi n .i 0 Radiological conclusions . 8 CONCLUSION D RECOMMENDATIONSAN S At present, there are several crude models for calculating doses to man from releases of radionuclides e Co-ordinateTh d Research Programm Baltie th n co e into the Baltic Sea. However, realistic parameters Sea organized by the IAEA terminates in 1984. The Meet- should be used when modelling radionuclide releases ing discusse e progresa positioth d n i s sn wa mad d an e into the Baltic Sea. o statt e thae co-operatioth t d beeha nn very success- Unfortunatel yo opportunit n ther s wa e y within ful. Considerable improvement was made in the under- the CRP to compare all the data available from the standin transporf o g t processes, concentration ratios, 29 Baltic Sea in order to draw more comprehensive con- critical pathways and mass balances of radionuclides. 30 Since radioactive materials are included in Annex e establishmenTh workina f o t g grou radiologif o p - e Helsinkth f o iI I Convention e Meetinth , g recommends cal experts froe Balti th ma countrie Se c s highli s y that the IAEA should request the Helsinki Commission recommended. The tasks mentioned above are mainly to study the possibility of co-ordinating the study aime t improvinga d , inter alia e knowledgth , e th f o e of radioactive materials in the Baltic Sea as performed circulatio f harmfuo n l substance e Baltith a n Se i cs today in the Co-ordinated Research Programme of the as wel s estimatioa l e riskth f so n cause y thesb d e Agency. The IAEA should be associated with the pro- substances to man and marine life. In addition the gramme, n e.gobservera s a . . suggested group could also assess the radiation burden If the Helsinki Commission agrees to co-ordinate populatioe tth o n living aroun s e welBaltia th da l Se c e programmth n radioactivito e e Baltith n i yc Seae ,th as develop model o predict s t radiatione doseth n i s following items wer ee mos regardeth t e b importan o t d t n accidentevena f o t . e continuete establisheb ob o t t alread r no o d f i d y In order to obtain comparable results, further in existence. intercomparison work on various samples is needed. e datTh a shoul e reporteb d a standardize n i d d manner Compilation of available data on radioactive dis- such as that used during this Co-ordinated Research charges. These data should be reported to the Programme. The intercomparison should be performed Helsinki Commission each year. at an interval of 3 - 5 years and should be carried out under the auspices of the IAEA. Special attention Collection of radionuclide data from open sea shoul e intercompariso th e pai b do t d f samplino n g tech- locations, as well as from coastal areas, when niques . appropriate. These data shoul e reporteb d o t d n additioI e internationath o t n l co-ordination the Helsinki Commission in order to gain better of future work on radioactivity in the Baltic Sea, understandin e behaviouth f o g f radionuclideo r s the Co-ordinated Research Meeting wishes to encourage e Baltiith n c Sea r opea .observationFo se n s countrie o continut s e thei n - programmeow ex r o t d an s the Helsinki Commission station network should change data. Seminar n actuao s l problems woule b d preferabl e usedb y . most desirable.

There is an urgent need to establish a data bank r compilinfo e datth g a reporte o facilitatt d an d e a computer-aided evaluation of the data. It would e preferablb o establist e h this data bank within e frame-worth e Helsinkth f o k i Commission, which would also help to use other data collected from e Baltith a withiSe ce Helsinkth n i Commission programme. ANNEX1 RESEARCH CONTRACT AGREEMENTD SAN S

No. Title Institute Chief Scientific Investigator

e th n i 1. r S d an s C Source f o s Risfi National Laboratory, A. Aarkrog Danish Straits. Health Physics Department, Roskilde, Denmark

2. Radiological factors affecting Finnish Centr r Radiatiofo e n . SalA o individua d collectivan l e doses d Nucleaan r Safety, Helsinki, o radionucIidt e du e releases into Finland e Gul th f Finlano f d Gulan f do f Bothnia.

3 . The water/fish concentration National Boar r Nucleafo d r . MoldenhaweF r s influencinfactoit d an r g Safety and Radiation Protection parameters on freshwater fish e GDRoth f , Departmenf o t living under brackish water Nuclear Environmental Protection, conditions. Berlin, German Democratic Republic.

4. Investigations on the distri- Deutsches Hydrographisches H. Kautsky butio f differeno n t artificial Institut, Hamburg, Federal radionuclide e wateth f n o rI s Republic of Germany. the Baltic Sea.

5. Radionuclides and trace elements Institute for Energy Technology, G.G. Christensen in the marine environment along Healt d Safetan h y Division, the Norwegian coast. 1er1 e , j K Norway

6. Monitoring of radioactive materials Central Laboratory for Radio- Z. Jaworowski in the Baltic Sea. logical Protection, Department of Radiation Hygiene, Warsaw, Poland.

7 . Releases, distribution and Lund University, . HolE m pathway f radionuclideo s n i s Department of Radiation the Baltic Sea. Physics , Sweden

31 32 TRANSFER OF RADIOCESIUM AND 90Sr FROM SELLAFIELD TO THE DANISH STRAITS

. AARKROGA . DAHLGAARDH , . BOELSKIFTS , E Risçi National Laboratory, Roskilde, Denmark INDIVIDUAL REPORTS Abstract

A main purpose Danisth f ho e participatio e coordinateth n i n d ANNEX2 research programme on radionuclides in the Baltic Sea has been DENMARK the study of inflow and outflow through the Danish Straits. Applying the effluents of radiocesium and 90sr from the re- processin gs beeplantha nt i possibl: , SellafielUK e eth n i d to calculate transfer factors for these radioéléments to sur- faco bottot s wela e s a l m e Danis wateth n i hr Straitss ha t I . furthermore been possible to estimate the transfer time from a waterborn pollutant in the Irish Sea to the Danish Straits and to calculate the dilution factor. The inflow of radioacti- vity from Sellafield throug Danisthe h h StraitBaltithe to cs somewhas i a Se tdischargese lesth sf o tha% 1 n.

1. INTRODUCTION

The content f 13?co s s an< e wate3 th 90g n ri raroun d Denmark arises from two main sources: fall-out from nuclear weapons testin d waterbornan g e discharges from reprocessin f nucleao g r fuel in Western Europe. In the North Sea the last source is dominant e Baltith a fall-oun e morSe ci ; th e s i importantt . In the Danish straits (The Cattegat, The Sound, and The Great Belt), which connec e Balti th e Nort d th tc an hSeas e botto,th m wate f higo r h salinity correspond o Nort t sa water Se h , while the surface water of lower salinity is a mixture of Baltic and Nort a watersSe h . Hence fall-ou s wel a ts effluent a l s fro- re m 1 processing determine the 90sr and 3"?cs levels in the Straits. 2. METHODS AND MATERIALS Samples of seawater (surface and bottom) have been collected in 8° 9° 10° 11° 12° 13° U° 15° 16° 17° 18° 19° 20° 21° 22° the Danish Straits and analysed for 90Sr and radiocesium. Since 1962 the results have been published in the annual Ris0 Reports in the series: Environmental Radioactivity in Denmark [l],

Radiostrontium was determined by the classical procedure in whic preliminara h y precipitatio uses i ncarbonates a d , followed by fuming nitric acid separations. Radiocesiu s retainewa m n o d an AMP precipitate, which was counted on a Ge(Li) spectrometer. The chemical yield of the radiocesium on AMP is 95-100% and Cs usuallsi a t yieladde no s ya d tracer. This makea s 134 determinatio 134f o n Cs possible e loweTh . r limit f detectioo s n 90 3 137 (LLD)[l] were 0.1 Bq Sr nT and 1.8 Bq Cs m-3 for 50-liter samples.

The quality of the determinations have been checked through participatio n IAEA'i n s intercomparison programmes.

3. SEAWATER Since 197 137e 3th C s concentration Danise th n hi s Straits have been proportional to the salinity in o/oo: Bq 137Cs m~3 = 29.6 -0.16 o/oo (1972) 137 3 Bq Cs m~ = 22.2 +0.44 o/oo (1973) go 100 12» 130 u° 15° 16° 17° 18° 19» 20° 21° 22" Bq = 20.0 +0.67 o/oo (1974) Bq 137Cs '3 =23. +0.37 7 o/oo (1975) Bq '3 =19.6 +0.70 o/oo (1976) 3 Bq 137Cs m- 15.2 +1.00 o/oo (1977) Fig. 1. Caesium-137 in surface seawater collected in 1983 in the Bq 137Cs itT3 -10.4 +2.85 o/oo (1978) e Straitsth d e erroBaltian Th . a re mea Se 1 cS.Eth ter n s f i mo . Bq 137Cs m"3 =-33.3 +4.44 o/oo (1979) of a summer and a winter sampling. 13 Bq _= 9-73 C- 1sm +3.26 o/oo (1980) Bq 137Cs m-3 = -5.0 +3.04 o/oo (1981) 13 3 Bq 7Cs HT = 4.11 +2.56 o/oo (1982) Bq 137Cs m"3 = -1.73+2.19 o/oo (1983) The regression analysis showed significan r probablo t y signi- 33 ficant regressio yearl al n si n except 1972. 34 ° 22 » 21 ° 20 » 19 ° 18 " 17 ° 16 ° 15 « K ° 13 ° 12 ° 11 ° 10 » 9 l« 125 60 Nort watea Se h r Salinity 3i%o (bottom water from 100 the Danish Straits) The Danish Straits x--137Cs Surface water 75 - 90o Sr Surface water

m

25

i i i i i i i i i i i i i i i i i i i i i 65 70 75 80 00 YEAR

. Caesium-133 Fig. e Danis th 90d Sn an 7rhi Straits 1962-1983.

53° » 22 ° 21 ° 20 » 19 ° 18 » 17 ° 16 ° 15 » U ° 13 ° 12 0 ,, o 10 o g o 8

Furthermore, we have found that the 13?cs concentrations in 35 o/oo seawater froe Danisth m h Straits during 1972-1983 were relateSellafiele th o t d d discharge 137f o s Cs (PBq y"1) year4 s Fig. 2. Caesium-137 in bottom seawater collected in 1983 in the earlier (1968-1979) (cf. fig: .4) Baltic Sea and the Straits. The error term is 1 S.E. of the mean

of a summer and a winter sampling. 1 Bq 137Cs m-3 = 24.1 + 17.4 PBq 37Cs yr-l 150 The 90sr concentrations in the Straits may also be related to 137, IJq 'Csm-B 24." = 3 yr 1 17.* q 4PB the salinity:

790 Bq 90Sr m"3 = 34.8 -0 .67 o/oo (1967-1971) Bq 9^Sr m-3 = 29 .6 -0 .16 o/oo (1972) 90 -3 100 Bq Sr m = 35.9 0.74 o/oo (1973) Bq 9^Sr m-3 = 34 .4 -0 .37 o/oo (1974) Bq 90Sr m— 3 = 29 .2 -0 .22 0/00 (1975) U) 9 o Bq ^Sr m-3 = 26.3 -0.074 0/00 (1976) Bq 9^Sr m-3 = 26 .3 -0.056 o/oo (1977) CT CD Bq 90Sr m-3 = 27 .8 -0.107 o/oo (1978) -77, 9 50 Bq "gr m-3 = 27 .8 -0 .31 o/oo (1979) Bq 9^Sr m-3 = 20 .8 + 0.159 o/oo (1980) Bq 90Sr m-3 = 25 .9 +0.098 o/oo (1981) Bq 9^Sr m-3 = 26 .8 -0.197 o/oo (1982) Bq 90Sr m-3 = 27 .6 -0.083 o/oo (1983) J_ 12345 However, the regression analysis showed only significant regres- 90 PBqyr-1 sion in 1967-1971, 1972, and in 1974.The contribution of Sr

from reprocessin s thui g s much less thar 137£fo n S. howeverf i , Discharge Cofs 137 from Sellafield four years earlier ther d bee o 90gha en n n Sellafieli r d effluents e woulw , d have see negativa n e correlatio e yearsl observe th al w n r s i ,a nfo t i e first part of the period.

Fig . Caesium-134 . n bottoi 7 m seawate 4 0/0(3 r 0 salinity) collected In open oceanwate 13e 7cs/th r 90Sr rati s 1.5i o , i.e. closo t e Danise ith n h Straits 1972-1983 relate o discharget d s from Sellafield that observed in fall-out [l] . In the first part of the four years prior. seventies before effluents from reprocessing had entered the

Danish Straits in significant amounts the 137cs/90sr ratio was approximately 1 [ l] . This lower ratio in shallow coastal waters is due partly to runoff e.g. from rivers, where the

137cs/90gr ratio is in the order of 0.1 [ l] and partly to a

greater sedimentatio e seabeth f 13?cn o do n s than 90sre th ,

137cs/90sr ratio in coastal sediments being in the order of 5 [ l] . Cesium-137 is to a larger extent than ^Sr retained by clay minerals o mainuclidee tw d th thi n ,an e s i reasosth s y wh n 35 show a different environmental behaviour in shallow coastal waters. Table I.A. Strontium-90, Cesium-137 and Cesium-134 in sea water collected around Zealand in May 1983

Position Depth 90Sr Sal inity N E in m Bq m~3 Bq 3 m~ 3m q B o/oo

Kullen 56°15' 12°25' 0 24. L . D . B 11.8 n 17 23 74 2.7 33.3 Hesselß* 56°10' 11°47' 0 26 45 . L B. .D 20.1

n 23 60 2.4 A 31 .2

Kattega W S t 56°07' 11°10' 0 31 . L B. .D 14.7 " 27 18.966 2.4 33.4 Asnae v re s 55°38' 10°47' 0 26 24 . L B. .D 12.4 „ 32 67 2.2 32.9

Halskov rev 55°23' 11°02' 0 24 B. D. L. 11.8 n 19 27 70 2.1 32.2

Langeland bait 54°52' 10°50' 0 26 18.8 B. D. L. 9.6 „ 29 67 1.79 31.0 Femern baelt 54°36' 11°05' 0 19.8 . L B. D 9.6

n n 21 25 59 2.3 A 28.9

Gedser odde 54°28' 11°59' 0 26 18.9 . L B. .D 9.2

n n 17 45 1.28 20.0 Maen 54°57' 12°41' 0 16.5 . L B. .D 8.3

» 22 25 21 . L B. .D 10.0

The Soun Sout- d h 55°25' 12°37' 0 30 16.7 . L B. .D 7.8

I I M N 10 16.4 . L B. .D 8.0 The Soun North- d A 55°48' 12°43' 0 16.6 . L B. .D 8.7

„ 14 25 42 B. D. L. 18.9 The Sound - North B 55°59' 12°42' 0 25 19.5 . L B. D 9.7 n n n 25 76 2.3 31.6

Mean Surface 26 23 11.1 S.D. 1 .76 8. 15 3.45 S.E. 0.72 2.35 1.00 Mean Botto4 2 m 55 26.0 S.D. 2.79 19.98 9.30 S.E. 1.14 5.77 2.69 •Collected in August. Table l.B. Strontium-90, Cesium-13 d Cesium-13an 7 a watese n ri 4 collected around Zealand in November 1983

Position Depth 90Sr '«Cs initl Sa y N E in m Bq m Bq m~3 Bq m~3 o/oo

Kullen 56°15' 12°25' 0 23 B.D.L. 11.3

- 22 59 1.8 A 27.3

Hessel» 56°10' 11°47' 0 51 1.8 A 25.0 « 23 26 60 B.D.L. 26.8 Kattega W S t 56°07' 11°10' 0 n 35

Asnas rev 55°38' 10°47' 0 32 B.D.L. 16.8

« 23 28 44 B.D.L. 23. 1

Halsko v re v 55°23' 11°03' 0 31 B.D.L. 15.8

« 18 41 B.D.L. 21.2

Langeland bait 54°52' 10°50' 0 30 B.D.L. 14.8

n 29 44 B.D.L. 21.6

Femern bœlt 54°36' 11°05' 0 24 29 B.D.L. 15. 1

., 22 39 B.D.L. 19.2

Gedser odde 54°28' 11°59' 0 21 B.D.L. 11.3

n 15 28 26 B.D.L. 13.5 Maen 54°57' 12°41' 0 29 18.0 B.D.L. 9.9

n 20 21 B.D.L. 10.4

The Soun Sout- d h 55°25' 12°37' 0 18.9 B.D.L. 10.2 n 1 1 19.4 B.D.L. 10.7 The Sound - North A 55°48' 12°44' 0 25 18.6 B.D.L. 10.5 n H n 14 22 B.D.L. 11.1 The Soun Nort- d B h55°59 ' 12°42' 0 21 B.D.L. 10.8 i t t i n 25 56 B.D.L. 27.3 Mean Surface 26 27 13.8 S.D. 2.65 9.66 4.49

S.E. 1.53 2.91 1.35 Mean Botto7 2 m 39 19.3 S.D. 1.15 15.33 6.79 S.E. 0.67 4.62 2.05 Tabl . KC Radlonuclidee a watese n ri s collecte Danise th n i hd straits e Balti th e Nort th d ,c an hSea n 198i s 3

, 239,240 241 Position Date Depth Salinity 9°Sr '"es134C s JH Pu Am N E el. W in m 3 m~ q 0/0B 03 m q B Bq m kBq m mBq m mBq m

Barseback 55045129 12°52'77E 9/5 0 8.0 16.8 B.D.L. 18 33.0 74 2.0 A

55°46'01 12°52'68E 14/4 2 10.4 19.1 B.D.L. " " " « 11 10.6 21 B.D.L.

Ringhals 57°155 '1 12°03'60E 14/4 0 18.2 37 B.D.L. " " " " 24 33.7 65 2.3 A • 57°15' 17 12°03'55E 10/8 0 20.5 44 B.D.L. • " " " 18 28.3 55 B.D.L.

Dana Tog t 1 54°45' 0°30' E 15/2 0 34.9 171 5.6 • 5S°15' 0°30' E 21/2 0 35.0 31 157 5.1

. 56°15' 0°30' E 15/2 0 34.5 189 6.7

. 57°45' 0°30' E 15/2 0 35.5 10.6 48 2.1

. 59°45' 0°30' E 13/2 0 35.1 34 B.D.L.

. 60°45' 0°30' E 14/2 0 35.4 3.8 B.D.L. • 59°15' 1°30' E 13/2 0 35.3 6.9 28 B.D.L. . 60015' 1°30' E 14/2 0 35.7 3.7 8.3 B.D.L. " 61015- 1°30' E 14/2 0 35.5 2.8 3.5 B.D.L. • 58°45' 2°30' E 13/2 0 34.5 69 2.2 A " 55°15' 3°30' E 22/2 0 35.0 136 4.1

• 58°15' 3°30' E 12/2 0 35.3 7.2 28 B.D.L. " 58°15' 4°30' E 12/2 0 34.2 85 2.4 . 53°45' 5°30' E 25/2 0 33.8 31 98 4.1

. 55°15' 5°30' E 22/2 0 35.t 3 18.11 8 4.1 " 57°15' 5°30' E 11/2 0 35.4 39 B.D.L.

M M 57°45' 5°30' E 11/2 0 34.8 11.1 47 B.D.L. . 57°15' 6°30' E 10/2 0 35.0 106 3.6 • 55°15' 7°30' E 22/2 0 33.9 34 2.9 . 57°15' 7°30' E 10/2 0 34.9 15.3 64 2.3 Dana Tog t 7 57°18'3 8°20'5 E 10/5 0 33.2 7l 2.4 A

K N 57°57'5 7°51E '0 9/5 0 23.6 46 B.D.L.

' 58°15'8 9°17' 2 E 15/5 0 29.7 60 2.8

• 58°00' 9°26' E 16/5 0 32.6 87 3. 1

8 t Dang To a 55°00' 7°50' E 27/5 0 29..6 20 2.9 " S4°I6' 7°38' E • 0 30.,5 24 18.21.,0

. 55°40' 7°47' E 28/5 0 29..6 25 24 2.,4 A

. 56°09' 7°52' E " 0 29.5 23 2.,2

" 55°53' 7°59'' E 29/5 0 30.6 27 30 2.,4 Dana Tog t 9 57°10'60 7°36 '42E 6/6 0 31 .6 73 2.9 • 57°09'96 6° 17'29E 7/6 0 32 .2 20 71 3.1 . 57°10'79 5°27 '41E 7/6 0 34 .9 89 3.2 . 57°09'87 4°28 •34E 7/6 0 34 .9 16.3 87 3.4 N n 57°09' 10 3°26 •07E 7/6 0 35 .0 92 3.4 . 57°10'60 2°30 '20E 8/6 0 34 .8 26 139 5.2 . 57°09'94 1°26 '33E 8/6 0 34 .7 136 3 .9 • 57°08'30 0°29 '86E 8/6 0 34 .9 19.0 95 3 . 1 Dana Hanstholm 57°10'10 8°26 •8 E 10/5 0 30 .6 31 36 B .D .L. " Mandai 2 57°49'6 7°57 '6 E 9/5 0 32 .0 22 68 2.8 A • Arenda1 l 58°21'4 8°58 '9 E 15/5 0 19 .7 23 43 1 .4 A " Arenda3 l 58°08'5 9°36 '4 E 15/5 0 30 .0 27 60 3.0 " Skagen 57°48'1 10°52 '5 E 14/5 0 28 .3 30 61 3.1 Hals Limfj. 56°59'51 10°18 '20E 2/8 0 26 .0 31 37 B .D .L. 2.3±0.2 Table I.e. (continued)

, 1 239,2424 . 013,, 3 Position Date Depth Salinity 90Sr 137C *Cs H Pu Am l e E N H . in m 3 o/om" o q B 3 Bqm Bq m"3 kBq m~3 roBq m"3 mBq m~3

Gjal " 57°03'74 9°42'05E 2/8 0 24 .6 29 27 . 2.1*0.L B. .D 7

Amtoft " 57°00'32 8°56'70E 3/8 0 26 .2 27 25 B. D. L.

Sillerslev Lim. 56°40'83 8°44 '05E 3/8 0 29 .1 29 31 B. D. L.

Thyboran 56°42'78 8°13 '76E 3/8 0 32.0 32 77 2.6 A

Hanstholm 57°07'29 8°36 •20E 4/8 0 32.0 74 3.8 Hirtshals 57°35'80 9°57 •83E 4/8 0 31 .3 71 2.9 Skagen S7°43'85 10°35 '52E 4/8 0 3t .6 26 76 2.6

L*sa East 57°19' 11°08 • E 10/8 0 22 .4 25 45 B.D.L.

• West 57°18' 10°56E • 10/8 0 21 .5 44 B.D.L.

Anholt 56°43- 11°31 1 E 10/8 0 20 .1 31 40 1 .8 A

Kessele 56°11'70 11°42 '55E 11/8 0 19 .7 41 B.D.L.

GAUSS 8 55°00'08 10°06 •11E 26/5 0 11 .9 25 26 B.D.L. 4.7* 0.67 A*

• • » " 34 25 .7 35 56 B.D.L.

GAUS2 2 S 54°46'2 12°45 •8 E 27/5 0 8.3 26 17.7** 0.108** 3.4* 0.21 B*

- " It • 17 8.5 31 19.B1.D.L. 24 55°49'89 10°48 •29E 28/5 0 13 .5 3.2* 0.60 A« 27 56°30'03 11°29 '97E 29/5 0 15 3.2« 0.28 A* • 30 57°30'02 11°29 •99E • 0 "16 3.0 A* 0.24 B* 33 56°15' 12°22 ' E 30/5 0 14 .5 2.8* 0.26 B* . . 55°10'06 16°00 •04E 1/6 4 8 26. 1A 1 0.53. 16.8B 2Spiked Polarstern 2+3 57°54' 4°07 1 E 30/6 5 32 .6 18.8 62 2.8 A 1.210.4 17.1« 1.75*

" 4 60°33' 4°0E 0 1 30/6 10 30 .2 19.7 53 2.0 A 1.810.4

Dana Tog t 14 60°1S' 2°1W 0 ' 16/9 0 34 .6 10.7 45 B .D.L.

• 60°04' 2°01W 1 " 0 35 .2 33 B .D.L.

" 59°55' 2°18W 1 H 0 35 .2 37 1 .9 A

" S9°45' 2°0W 9 1 " 0 34 .7 8.5 31 B .D.L.

• 59°35' 2°14W 1 17/9 0 35 .1 88 2.9 A " 58°35' 2°5W 0 1 29/9 0 34 .9 147 5.6 m m 58°34' 2°58 1 W " 0 34 .9 157 5.7

. 58°46' 2°4W 9 ' • 0 35 .0 148 5.0 • 58°56' 2°2W 9 1 " 0 35 .0 134 5.6 . 59°05' 2°2W 5 ' M 0 34 .8 164 6.9

. S9°15' 2°10W 1 " 0 34 .2 159 6.6 Dana Tog t 16 54°46' 13°3E 1 ' 20/10 0 11 .1 23 B.0.L.

• 55°38' I5°1E 5 1 21/10 0 9.4 20 B.D.L. 2.6** • " " " 60 9.6 18.6 B.D.L. 2.8** • 54°48' !5°34 1 E 27/10 0 8.3 17.6 B.D.L.

. " • • 60 8.4 17.3 B.D.L.

. 55°03' 16°2E 9 1 22/10 0 8.2 14.4 B.D.L.

" 56°07- 17°05 ' E 24/10 0 7.8 16.5 B.D.L.

m • " " " 30 7.9 16.2 B.D.L.

. 55°21' 18°37 ' E 25/10 0 7.7 14.9 B .D.L.

• 56°20' 20° 1E 51 • 0 7.7 16.4 B.D. L.

• " " • 45 7.7 14.4 B.D. L. . 55°3C' 20°2E 5 ' 24/10 0 7.8 27 15.B.D7. L. e GolTh f fo Finland 60°15'14 25°48•95E 23/10 0 5.8 1 1.5 B.D. L.

Rise 15/5 0 10 .9 19.3 B.D. L. " 16/5 0 18.3 B.D. L. • 18/5 0 18.3 B.D. L.

Bolund at Rise 6/6 0 10.3 20 B.D. L. Rame 55°05' 8°3E 4 1 10/1 0 25 .9 20 1 .91

Esbjerg 5S°29' 8°25 1 E 10/1 0 27 .9 18.2 1.44 A

3 m 2 0. * 3 m 7 «*1. ~ all other samples were ~ 0.05 m . 3 40 During the period 1974-1981, when the Cs discharges from rected to mid-1983 they are: 137 Sellafield in the OK have been enhanced, the 137Cs/9Osr mean 137 6 (1SD,N=8)5/1. e discharge± rati th 6 n 9. i o n seawates i . wa s r 3278 ± 758 (N = 8, rel. SD = 23%) T Bq Cs sample se 137 collecte th Cs/90se Nort a th Se hn i rd ratis ha o 72.5 ± 12.8 (N = 8, rel. SD =18%) T Bq ^4Cs 90 been lowe e dischargesr th tha n i n ; typicall e ordeth f o n ri y =27%D S q SB l rT re ) , 8 = N ( 341 3±9 60-70% of the expected ratio 1.6). We have assumed a fall-out background in the North Sea of 3 Bq 137Cs m~3 and 2 Bq 90Sr m~3 e assumW e Danise thae wateth th tn hi r straits during 1980/1983 seawater e concentration,th whic e ar h s observee Nortth n hi d has been in equilibrium with the discharges. Hence we will Atlantic surface water. Close to the coast of North Scotland relat e decath e y corrected mean concentration e radioth f -o s the 137Cs/9Osr ratios come e expectecloseth o t r d valuet bu , nuclide e e straitsabovth th foun n o ei t sd dischargen i s thee stil ar o ylow to l . order to calculate the transfer factors from Sellafield to the straits. However, before we make this calculation we have We conclude that some of the radiocesium discharged from to make some correction r non-Sellafielfo s d activities. Sellafiel s removei d d froe wateth m r column whe t passei n s along the British coast before it enters into the central part e assumW e thae fall-outh t t backgroun e straitth n i ds varies of the North Sea. Jefferies et al [7] have stated that <10% of proportionally with the salinity and that the backgrounds in the total ^37Cs discharged has entered the seabed compartment theq NortB a (salinity2 Se hd an 137q B 3 Co/oo5 3 sm~ 3 : e ar ) 903 of the Irish Sea. According to Livingston et al [3] only less e westerth n i n d Baltian a (salinitySSe crm~ 8 o/oo: 5 1 ) than 3.5% of the 137Cs from Sellafield is found in the sediments. Bq 137Cs m~3, and 23 Bq 90Sr m~3. The equations used are: In an earlier report during this Baltic programme [8] we assumed Bq 18.= 137 3 C5snT -0.4 4 o/od oan that unknown sources of 90gr Were responsible for the lower 90 3 than expected ^ Cs/ Sr ratios. This may still be a factor of Bq Sr iïT = 29 -0.78 o/oo 37 9u importance, however e believw , e that ' Cs from Sellafiels i d 37 Furthermore e assum,w e that other nuclear facilities (Cae d p deposited in the coastal waters of Britain and in the North Sea la Hague in Prance and Dounreay in the UK) contribute with o suct extenn a h t tha1e 37th tCs/ seawatee 9th Os n ri reduces i r d 17% while Sellafield yields 83% of the non-fall-out 90sr in significantly. In other words, we suppose that on the order of the straits. This assumption was based upon the discharge one-third of the radiocesium discharged from Sellafield is perioe th datr d fo a1976-198 0 [9J. deposited in coastal sediments. We know from measurements of At the four permanent stations in the southern Cattegat (55°38'N- sediments in the Cattegat [ l] that 13^Cs is present and this 56°15'N, 10°47'E-12°25'E e fall-out-correcteth ) d mean concen- proves that radiocesium from Sellafield is deposited in the trations of surface water (mean salinity 15 o/oo) during 1980- straits and hence undoubtedly also in the North Sea. 1983 (decaycorrected to mid-1983) were 6.4 ± 1.2 (1SE,N = 7) Bq 90Sr nr3, 0.91 ± 0.11 (1SE,N = 5) Bq 134Cs m~3 and 23.6 ± 2.3 (1SE,N =16) Bq 137Cs m~3. Hence the transfer factors become: . CALCULATIO4 TRANSFEF O N R FACTOR O SSAWATEST R Les consideu t e annuath r l mean discharge f radiocesiuo s d an m 6.4 x 0.83 = 16 Bq 9USr m~3 pr. PBq a~l Sr from Sellafield during the period 1974-1981 [5]. Decaycor- 90 0.343 0.91 Darrs Sill of 12.3 x 472 x 109 = 5.8 TBq 137 pr PBq 137 = 13 Bq 134Cs m~3 pr. PBq 134Cs a"1 Cs Cs 0.0725 discharged from Sellafield or approximately 0.6 %. This means thae totath t l inventor f Sellafielo y de Balti 137th a Cn si Se c 23.6 at presen ordee t th : 100-20 r (1984aboun of ro i q s t)0i TB one- 37 373 q 1 PB Cl - s. a 1q pr B C7 =s m" e inventorfiftth f o h y from fallout. 3.278

Ie transfea nsimila th y wa rr factor r bottofo s m water (mean 5. SEDIMENTS salinity: 33-34 o/oo) were calculated: In the Danish Straits a considerable part of the 137cs inven- tor s e presensedimentsi y th n i t . Froe dat n th tablmi a 2 e we notice that the deposition vary between approx 100 and 5200 x 0.8 4 32 90 3 1 2 37 = 58 Bq Sr nT pr PBq 90Sr a" Bq 13?c:s m~e mediaTh . n valu s approximateli e q !B C0 s90 y 0.343 totae th m~ Danise lS 2 A .th are f ho a Straits (The Cattegad an t the Belt Sea) is 43 900 km2 the total inventory in the sedi- 2.09 ment s approximateli s q !37TB Cs e wate0 e volum4 .th yTh rf o e 134q 1 CPB sa" . pr 134q B 3 C 9 snr 2 = 0.0725 e meath n d Danise concentratioian th n 3 hkm Strait0 80 n s i ni s s approx198 137q wa B 33 C . Henc(cf0 sm~ 2) 5 . e .d w e figan 1 s 84 may conclude that the total inventory in the Danish Straits 137q 1 CPB sa' . pr 137q B 3 C s6 nT 2 = was approximatelky 80 TBq 137c and that this activity was 3.278 s nearly equally divided between sediments and water.

As expected the transfer factors (TP) were lower for surface In "Dybe Rende" (57°30'N 11°30'E) s determinecwa s d down water thar bottofo n m r waterSfo r d valueP werT an , f eo s 134 90 e sedimentsth n i e totam c Th . 13q 2 B lt4c1 o deposi2 7 s wa t nearly two times those of radiocesium. For 134c they should be s s m~ . This is (corrected for decay) 2.5 times more than found the sam s thos a er 137 fo eCs t thi s apparentl,bu wa se th t no y 2 in 1979 (Ris0-R-42 9 [l]e 6 annua Th .. p 1 l deposit since 1979 case for surface water. If, however, we take the uncertain- of Sellafield 137Cs may from this information be estimated at ties into consideratio t o significantlfigureno tw e e ar th ns y 400-500 Bq 137Cs m~2 in "Dybe Rende". different. e Iassumw f e that "Dybe Rende" represent a ssedimentatio n rate Froe transfeth m r factor f radiocesiuo s o surfact m d bottoan e m water in the Danish Straits it is possible to calculate the of Cs: 5200 ~ 6 times that of the mean for the Danish Straits, 137 13 900 net inflof o w7c s from Sellafiel e Baltith o ct d e w Sea f I . this mean becomes 75 Bq ^ Cs m~ a~-'-. This corresponds to a assume thate transfeth r factors vary proportional wite th h 37 2 salinit d thae salinit an ye th inflowin t th f o y g wate s 17.i r 4 mean sedimentation rate froinventore th m overlyin e th f yo g water e n infloa th t t a ge w3 [10 km e ]w 4 1 2 e volum47 th o/os d i ean o colum . yearf 5-1o npr 0% . Table 2.A. Cesium-137 in sédiments collected in inner Danish waters in May 1983 by GAUSS. (HAPS) (Area: 0.0145 m2)

Location Station Date Df>pth Bq kg"y dr 1 Bq m~2 no. in cm

54°46'N 12°46'E 22 27 0-3 A 0 1. 46 « « n 3-6 1 .2 53

0-6 J. 99

54°39.68'N 10°45.41'E 23 A 28 0-3 16.7 420

N H H 3-6 9.1 350

0-6 L 770

23 B 28 0-3 19.4 440

Hl* H 3-6 8.6 280 n « « 6-9 2.8 100

0-9 1. 820

23 C 28 0-3 15.6 530 „ 3-6 6.7 250 " 6-9 2.7 110

0-9 l 890

55°50'N 10°48'E 24 28 0-3 20 430 . 3-6 8.3 260 .. " 6-9 5.1 180 " " 9-12 1.96 70

0-12 £ 940

56°30'N 11°30'E 27 29 0-3 6.1 230 i« w n 3-6 7.6 270

0-6 E 500

56°15'N 12°22'E 33 30 0-3 18.1 540

M H « 3-6 14.9 510

Ml« H 6-9 6.1 250 H N n 9-12 1.54 54

0-12 £ 1350

57°30'N 11°30'E 30 29 0-3 62 780

M H M 3-6 65 970

MM «1 " 6-9 64 1080

M H M 9-12 55 990 n » M 12-15 40 770

» 15-18 32 620

0-18 !• 5200 Table 2,B. Cesium-13 d Cesiurn-13an 7 sedimentn i 4 s collecte n Limf^ordei d n 198i n 3 (HAPS) (Area: 0.014) 2 5m

Location Depth Date q ]DeptB 37Csh 134q B 2 "«CCq sB «T B qs 137 2 CSm' m ic n kg"y 'dr y kg"dr 1

56°59'N 10°18'E Hals 7 m 2/8 0-3 2.4 130 " " 3-6 1.64 92

0-6 t 220

6 5. 56°60' 3 0- N 8°57' 8 3/ E Amtof m 6 t 191

3-6 4.2 178

0-6 J 370

56°38'N 8°17'E Nissum Bredning 5.5 m 3/8A 8 1 0-3 A 12. 8 0. 1 0 27

6 3- 15.2 360

" ... 9 _ 6 ,.6_ 9 370

. .... 9_,2 15.3500

0-12 1. 1500 1 18

Table 2.C. Cesium-13 sedimenn i 7 t samples collecten i d Roskilde fjord, 1982. (HAPS) (Area 0,014) 2 m 5

Location ^ m Dept q B h q kg~y B Datde ^ e in cm

3 7. 6 6/ 7 A0- t Bolund 520

55°40'N 12°05'E 25/7 16.6 2400

Table 2.D. Gamma-emitting radionuclides in sediment samples collected at Barsebäck location 38, in 1983.

Depth 60Co '«Sb U'cs Date in m Bq kg"1 d.w. Bq m~* Bq kg"' d.w. Bq m"^ Bq kg"' d.w. Bq m"2

9/5 0-3 14.9 88 4.2 A 25 A 86 510 0 5 3 5. 6 3- 50 470 6-9 38 300 9-15 7.6 191

8 13 t 0-15 £ 25 r 1470

14/11 0-3 150 11619.09 151 79 600 6 3- 1.83 2 8 43 520 6-9 10.5 132 9-12 3.6 50 12-15 1.6 A 24 A

0-15 44 Table 2.E. Gamma-emitting radionuclide sedimenn i s t samples collecte t Ringhalsa d , locatio 1983n i , 2 .n (Area: 0.0145 m2)

Depth 54«n 60Co 125Sb l"cs 1 1 m n i Date q kg"B * kg"q 1B d.wm~ Bq kg"' qB 'q d.wm" B kg"' .1 q d.w B m~ * . ' q d.wm~ B . q B .

3 13 4 9. 17.0 825 3 0- 14/4 A 0 4 12.0 543 A 1 1. 0 22 4 6. B 9 B 3 0. 6 3- 6 18 7 4. A 2 3 A 8 0. 9 6- "

9-12 0.6 A 29 A 2.8 123

0-12 £ 9 E 410 £ 40 I 990

3 0- 10/8 A 0 7 19.0 142 A 1 3. 10. 0 323 3-6 8.8 330 4.6 170 8.4 310 6-9 1.93 96 " 9-12 0.9 A 37 A

0-12 £ 560 I 240 I 860

c , 6. BIOTDANISE DOSED TH AAN O HST POPULATION Data from 198 seaweedn 3o , fish and mussels are shown in tables 3, 4 and 5 respectively, • Garpike d Co o Fig. 5 summarizes the 137Cs c oncentrations in fish caught in the Danish Straits since 1962. û Plaice a Mackerel vl HerrinEe o g From the 134Cs/137C s rati n ^ fisi have o w he estimated tha- ap t proximately 90 % o fe l37th Cn fisi s h consume? jj n Denmari d k come from Sellafieldn I . 1983 the mean concentration in Danish fish 5" 0 137q B waC 4 ss kg"1 . The annual intake of fish flesh is 10.9 8 k g° m o , o o e o capitth pr d an e - , ; populatio£ f Denmaro nx 10 5 b .s i Henck e th e 137 collective dose fro m Sellafield Cs become , si.e Sv 2.4 n . 5ma 0° ° /\°/r/\* »£* approximatel% 0 4 y of the total dose from radiocesium in the D A : X\/ 5^-— ssJLl Jr Danish diet in 1983[1]. n ^H~§~^ ° y " ' A J 0 i i ivi i i i°i i IAI i i i r i i l i i i i i Compared with the rlatural occurring background radiation (in- 65 70 75 80 85 YEAR 0.25 o/oo o concern , i.ef o .n fro a mhealt h hazard poinf o t Fig . Caesium-135 . fisn i 7 h froe Danismth h Straits 1962-1983 line Th e. view. s drawi n throug e mediath h n values. Table 3.A. Strontium-9 d Césium-13an 0 n Fucui 7 s vesiculosus from Roskilde Fjor n 198i d 3

Location y dr Dat% e Bq 9C 'sr (kg 90q Ca)SB r ~1 kg"q B ' 137Cs (kg K)~1 Bq 137Cs kg"1 matter y weighdr t dry weight

At Bol und 25/1 24.3 250 7.4

21/3 18.4 191 5.6 230 6.9

- " - « ' 11 11.6 Î40 11.6

_ tt _ 20/12 16.9 410 5.8 206 7.2

IX 12/12 18.0 189 7.2 220 8.0

X 12/12 16.2 390 6.1 230 9.5

Tabl. B . 3 e Radionucl ides in brown algae collected in inner Danish waters in 1983 (Uni q kq~B t' dry)

Species Position Date % dry matter Salinity 40K' «Mn 58co '«Co "zn E N o/oo

Fu. sp. 57°44' 10°36' 4/8 21 .8 35 1.05

La . sp. 57°36' 09°58' 4/8 20.0 38 0.4 B 1 0.42A

Fu.ve. 57°2T 10°33' 2/8 25.1 30 0.95

Fu.ve. 57°20' 10°32' 2/8 22.9 32 0.67 A

Fu. se. 570,91 J,0OB. 10/8 27.6 24 1.98

Fu. ve. 57°19' n008' 10/8 21 .2 33 1.37

Fu.ve. 57°19' 11°08" 15/4 21 .4 25 1.70

Fu. se. 57°18' 10°56' 10/8 24.8 32 2. 1

Fu.ve. 57°18' 10°56' 10/8 23.7 29 0.3 A 2 1.30

Fu. be. 57°18' 10°56' 15/4 21.6 26 0.2 A 8 0.83

Fu.ve. 57°18' 10°56' 15/4 20.1 27 0.3 A 3 0.74

F uv. e. 57°09' 10°26' 2/8 19.5 33

Fu.ve. 57°07- 12°11- 1/12 17.5 37 1.04 8.3 3.1

Fu.ve. 57°07' 12°11' 2/6 19.1 28 0.6 B 1.99

Fu. sp. 57°07' 08°36' 4/8 26.1 28 1 .37

Fu. sp. 57°04' tfl°22' 2/8 20.5 29

Zo.ma . 57°04' 09°42' 2/8 19.1 27

Fu.ve. 57°00' 10°18' 1/8 29.2 22

Zo.ma . 57°00' 10°18' 1/8 24.8 19

Fu.se. 57°00- 08°57- 3/8 26.9 25 0.41 A 0.50

Fu.ve. 57°00' 08°57' 3/8 28.7 29 0.43 A

Fu.ve. 56°54' 10°16' 2/8 22.3 31 1.06 A 0.44 A

Fu.ve. 56°54' 10°16- 2/8 23.5 25.4 32 0.51 B

Fu . ve . 56°4S' 10°18' 2/8 21 .0 24

Fu. ve. 56°45' 10°18' 2/8 22.9 28 0.36 A

F uv. e. 56°45' 10°18' 2/8 22.6 24.8 28 0.40 B

Fu.se. 56°43' 11°31' 10/8 22.6 28 1 .65

Fu.ve. 56°43' 11°31' 10/8 19.5 3 2. 32 0.4 A 6

Fu.ve. 56043' 11°31' 23/5 13.2 35 1. 15 A

F uv. e. 56°43' 11°31' 17/1 22.2 39 0.25 A 1.11

Zo.ma. 56°41' 08°44' 3/8 20.7 25 1.13

Fu.ve. 56°36' 10°19' 2/8 19.8 30

Fu.ve. 56°31' 10°27' 2/8 23.4 22.8 25 0.59 B 0.52 A

Fu.ve. 56°27- 10°58' 2/8 23.3 29 0.89

Fu.ve. 56°27' 10°58' 2/8 23.3 30 0.96

Fu.ve. 56°23' tO°56' 2/8 22.1 28 0.80 A

Fu.ve. 56°22' 08°07' 3/8 19.0 22.5 35 1.00

Fu.se . 56°12' 11°43' 1 1/8 24.6 22 0.65 A 2.8 Table 3. B. (continued)

40 "Mn 58 60 65 O o C n Z Species Position y dr Dat% e matter Salinity K* C N E o/oo

Fu.ve. 56°12' 11°43' 11/8 21 .2 31 2.3 Fu.ve. 56°12' 10°40' 2/8 23 .2 40 0.82

Fu.ve . 56°12- 10°40' 19/1 24 .0 32 0.74 Fu.ve. 56°07' 12°19' 29/7 24 .4 16.3 28 2.0

Fu..ve . 56°06' \2°28' 29/7 23 .6 17.8 21 6 3. 0.5 6B Fu. ..ve 56°04' 12°33' 29/7 20 .4 17.5 32 0.59 A 3.0 Fu.. se. 56°03' 12°36' 29/7 22 .3 16.3 . 6 24 0.4 B 5 1 . Fu.se. 56°03' 12°36- 17/2 21 .6 30 0.76 4.6 Fu. ..ve 56°00' 12°36' 29/7 23 .0 14.9 2 4. 25 0.5 6A Fu., ve. 56°00' 12°35' '7/2 20 .4 27 0.44 A 3..8 Fu.. ve. 56°00' 08°08' 3/8 11 8 . 23.8 32 0.82 Fu..ve. 56°00' 08°08' 3/8 17 .4 23.8 29 0.81 Fu..ve. 56°00' 08°08' 8/3 19 .6 32 0.32 A 0.86 Fu., ve. 55°59' 11°21 ' 14/2 19 .8 32 1.40 Fu.ve. 55°58' 11°17' 25/7 24 .4 . 0 24 0.5 A 1 68 Fu.ve. 55°58' 11°17' 14/2 22 .8 22.8 25 0.50 0.73 Fu.ve. 55°56' 10°04' 27/7 26 .0 27 Fu.ve . 55°56' I0°03' 6/6 19 .1 24 0.3 B Fu.ve. 55°55' 12°40' 13/9 19 .2 20.7 32 0.5 A 7. 6 0.4 6B 1 Fu.ve. 55°55' 12°40' 13/9 19 .1 20.7 31 0.41 B 5.2 Fu.ve. 55°55' 12°40' 13/9 24 .2 20.7 30 0.43 A 0.38 B 5. 1 Fu. se. 55°55' 10°39' 27/7 23 .9 29

Fu.ve. 55°55' 10°39' 27/7 23 .5 21.0 29 0.34 B 0.53 A Fu.ve. 55°53' 12°43' 13/9 18 .6 20.9 32 0.55 5.6 Fu.ve. 55°53' 12°43' 13/9 18 .6 20.9 32 0.63 A 6.5 Fu.ve. 55°53' 12°43' 13/9 19 .9 20.9 31 0.68 A 6.3 Fu.se. 55°52' 10°03' 27/7 26 .2 28 Fu.ve. 55°521 10°03' 27/7 24 .3 26 Fu.ve. 55°49' 10°39' 27/7 23 .0 28 0.70 A Fu.ve. 55°48' 10°32' 27/7 25 .2 20.8 24 0.47 Fu.ve. 55°46' 12°36' 28/7 22 .7 . 3 14.1 2B 2 4 0. 4

Fu.ve. 55°45' 10°57' 27/7 25. 1 20.8 33 0.67 Fu.ve. 55° 4 1 '11°05' 27/7 23 .1 28 Fu.ve . 55°35' 12°55' 1/12 16 .3 26 0.6 B 2.1 Fu.ve. 55°31 ' 09°46' 4/8 19 .8 29 Fu.ve . 55°27' 08°28' 3/8 24 .6 29.7 32 0.64 Fu.ve. 55°27' 08°28' 3/8 22 .9 29.7 40 0.61 A Fu.ve. 55°27' 08°25' 3/8 20 .7 29.1 28 0.36 B 0. 74 Fu.ve. 55°21' 11°07' 4/8 22 .9 25

Fu.ve . 55°18' 10°51' 4/8 22.2 22.2 36 0.53 A Fu.se. 55°05' 15°09' 17/11 18 .6 28 0.91 0.33 A Fu.ve. 55°05' 15°09' 25/5 20 .0 23 0.66 Fu.ve. 55°05' 08°34' 3/8 26 .6 29 0.48 A Fu.ve. 54°40' 11°44' 29/12 22 . 1 32 1.37 Fu.ve.** 53033' 08035' 28/6 lost 20 Table 3. C. Radionucl ides in brown algae collected in innée Danish waters in 1983 (Unit: Bq kg dry)

95 Species Position Date % dry matter salimty Nb ">«Ru 125sb 131j 134Cs 137Cs N E o/oo Fu .sp. 57°44' 10°36' 4/8 21.8 0.37 A 9.9 La .sp. 57°36' 09°58' 4/8 20.0 6.8 0.85 A 0.51 A 8.1 Fu .ve. 57°27' I0°33' 2/8 25.1 9.1 Fu . ve. 57°20' 10°32' 2/8 22.9 9.3 Fu .se. 57°I9' 11°08' 10/8 27.6 8.8 Fu.ve. 57°19' n°08' 10/8 21 .2 9.3 Fu . ve. 57°19' 11°08' 15/4 21 .4 6.7

Fu .se. 57°18' 10056' 10/8 24.8 11 .6

Fu . ve. 57°18' 10°56' 10/8 23.7 9.0 Fu .se. 57°18' 10°56' 15/4 21 .6 B 3 A 5 0. 0.28 7A .5

Fu .ve. 57018' 10°56' 15/4 20.1 8 0.3 A 2 .0

Fu .ve. 57°09' 10°26' 2/8 19.5 10 .1

Fu . ve. 57°07' 12°11' 1/12 17.5 10 .3

Fu .ve. 57°07' 12°11' 2/6 19. 1 12 .0 Fu .sp. 57°07' 08°36' 4/8 26.1 A 7 4. 0.37 6A .7 Fu .sp. 57°04' 10022' 2/8 20.5 9.6

Zo .ma. 57°04' 09°42' 2/8 19.1 5.9 1.4 A

Fu .ve. 57°00' 10°18' 1/8 29.2 4.6

Zo .ma. 57°00' 10°18' 1/8 24.8 7.2 Fu .se. 57°00' 08°57' 3/8 26.9 0.61 A 6 .3

Fu .ve. 57°00' 08°57' 3/8 28.7 4.9

Fu .ve. 56°54' 10°16' 2/8 22.3 12 .7

Fu .ve. 56°54' 10°16' 2/8 23.5 25.4 13.2

Fu .ve. 56°45' 10°18' 2/8 21 .0 10.1

Fu . ve. 56°45' 10°18' 2/8 22.9 14 .2 Fu . ve. 56°45- 10°18' 2/8 22.6 24.8 11.0

Fu .se. 56°43' 11°31 ' 10/8 22.6 10 .4 Fu . ve. 56°43' 11°31 ' 10/8 19.5 7.3

Fu .ve. 56°43' 11°31 ' 23/5 13.2 11 .3

Fu . ve. 56°43' U°31 ' 17/1 22.2 2.2 B 0. 16 B 9.3

Zo .ma . 56°41 ' 08°44' 3/8 20.7 5.7 2.5

Fu .ve. 56°36' 10°19' 2/8 19.a 1.9 A 11.1 Fu . ve . S6°31 • 10°27' 2/8 23.4 22.8 8.5 Fu . ve. 56°27' 10°58' 2/8 23.3 10 .7

Fu .ve. 56°27' 10°58' 2/8 23.3 9.5

F uv. e. 56°23' 10°56' 2/8 22.1 9.1 0 Fu .ve. 56°22' oaS 07' 3/8 19. 0B 3 4. 22.5 .2

Fu .se. 56°12' U°43' 11/8 24.6 10 .0

Fu .ve. 56°12' 1I°43' 11/8 21 .2 9.8

Fu . ve. 56°12' I0°40' 2/8 23.2 5. 1

Fu . ve. 56°12' I0°40' 19/1 24.0 0.18 B 8.3 Fu .ve. 56°07' 12°19' J9/7 24.4 16.3 7 .4

Fu .ve. 56°06' I2°28' 29/7 23.6 17.8 8 1-3 9A .9 Fu . ve. 56°04 • 12°33' 29/7 20.4 17.5 » .8 Fu .se. 56°03' 12°36' 29/7 22.3 16.3 8.5 Fu .se. 56°03' 12°36' 17/2 21.6 2.2 A 7.9

Fu .ve. 56°00' 12°36' 29/7 23.0 14.9 8.6 FU .ve. 56°00' 12°35' 17/28 20. 4A 1 2. 0.4 B 2 .1 Fu .ve . 56°00' 08°08' 3/8 18.1 23.8 5.1 A 1.45 A 7 .7 Fu .ve. 56°00' 08°087 ' 3/8 A 1 1. 17.4 A 5 1. 23.8 .1 Fu .ve. 56°00' 08°08' 8/3 19.6 2.8 A 0.76 3.1 Table 3.C. (continued)

Species Position Date « dry matter Salinity 95Nb 106Ru 125Sb I3'j '3«Cs 137Cs E N o/oo

0 ,,o i Fu.ve. 55 591 2] 14/2 19 .8 8 0.8 A 3 .8 Fu.ve. 55°58' 11 017' 25/7 24 .4 9.5 Fu.ve. 55°58' 1t 017- 14/2 22 .8 8 0.2 A 2 .1 Fu.ve. 55°56' 10O04' 27/7 26 .0 9.3 Fu.ve. 55°56' 10o03' 6/6 19 .1 9.6 Fu.ve. 55°55' 12o40' 13/9 19 .2 20.7 3.3 3.2 A 9.8 Fu.ve. 55°55' 12°40' 13/9 19 .1 20.7 1.4 3.4 9.2 Fu.ve. 55°55 ' 12o40' 13/9 24 .2 20.8 7 B 0 3. 3.6 .7 Fu.se. 55°55' 10o39' 27/7 23 .9 13 .7 Fu.ve. 55°55' 10°39' 27/7 23 .5 21.0 0.44 A 10.8 Pu.ve. 55°53' 12043, 13/9 18 .6 20.8 9 A 2 4. 0.9 A 6 .9 Fu.ve. 55°53' 12043, 13/9 .0 2u.» .3 Fu.ve. S5°53' 12°43' 13/9 19 .9 20.9 9 A 5 4. 1.A 0 .1 Pu.se. 55°52' 10o03' 27/7 26 .2 11 .8 Pu.ve. 55°52' 10o03' 27/7 24 .3 9.1 Fu.ve. 55°49' 10o39' 27/7 23 .0 8.9 Fu.ve. 55°48' 10o32' 27/7 25 .2 20.8 0.23 B 8.5 Fu.ve. 55°46' 12°36' 28/7 22 .7 14.1 10 B 8.8 Fu.ve. 55°45' 10°57' 27/7 25 .1 20.8 2 0.31 A 4 .4 Fu.ve. 55°41' 11 0OS- 27/7 23 .1 10 .1 Fu.ve. 55°35' 12o55' 1/12 16 .3 8 1. A 5 .2 Pu.ve. 55°31' 09o46' 4/8 19 .8 1 1 .0

Pu.ve. 55°27' 08o28' 3/8 24 .6 29.7 4.5 A 5.4

Fu.ve. 55°27' 08o28' 3/8 22 .9 29.7 1.28 A 4.8

Fu.ve. 55°27' 08°25' 3/8 20 .7 29.1 0.25 A 10.4

Fu.ve. 55°21' 11 007- 4/8 22 .9 8.6 Fu.ve. 55°18' 10°51' 4/8 22 .2 22.2 10 .8

Fu.se. 55°05' 15o09' 17/11 18.6 7.5

Fu.ve. 55°05' 15°09' 25/5 20 .0 6.4 Fu.ve. 55°05' 08°34' 3/8 26 .6 4 0.7 A 9 .5

Fu.ve. 54°40' 11 044' 29/12 22 .1 B .2

Fu.ve.** 53°33' 08o35' 28/6 lost 3.5

Fu.,ve. Fucus vesiculosus

Pu..se. Fucus serratus Pu.sp. Pucus spiralis Zo.ma. Zostera marina La.sp. Laminar i a species * Unit: g K kg"1 dry weight. ••Collected at Bremerhaven. Tab ^6^3, D. Radionucl ides in the hrown altjae FUCUB vesictilosus (Fu.ve.) and Fucus serrât us (Fu.se.) collected at Klint (55°58'N 11°35'E) in 1982(Unit q kg"B :y weight1dr )

,,c ,,. ,17 239,240 241

Species Date » dry Salinity K* Mn «°Co 90Sm r A "TC u P Sh CsCs

)25 IJ4 )37

54 matter o/o o40

Fu.ve. 14/224.9 21 0.4 A 1.32 7.5

Fu.se. " 24.6 30 0.69 2.6 1.47 9.5 Fu.ve. 24/319.3 B 4 0. 24 0 5 0 1.35. 2 0.4 A 8.1 0.29 0.057

Fu.ve. * 18.0 24 0.4 A 1.26 6.0 151 7.9 0.29 0.035

Fu.ve. ** 19.0 23 0 18 0 1.05. 6 7.6 0.23 0.023 " F uv. e. 19.2 25 7 13 7 1.45. 5 8.3 0.32 0.042 Fu . ve . " 17.4 A 4 0. 6 2 1.28 5.1 187 8.7 0.24 0.030 Fu.se. " 19.7 27 0.61 8 4 0 1.99. 6 1.28 9.7 0.54 0.057

Fu.se. " 18.6 29 0.95 2.1 10.3 871.22 9.0 0.62 0.046

Fu.se. " 19.2 3 39 2 8 0.8. 7 A 3 2. A 3 1. 11.4 0.50 0.039

Fu.se. " 20.0 29 0.86 1 2. 11.6 8 1 1.45 0.4 A 9.9 0.35 0.110 Fu.se. ** 18.6 31 0.84 2.1 9.8 79 1.0 A 9.7 0.61 0.073

Fu.ve. 25/718.3 19.0 27 2.3 9.8 Fu.se. " 22.7 19.B 05 0. 26 2.3 9.9

Fu.ve. 18/818.9 20.3 32 2.8 8.1 Fu.se. 22.1 20.3 26 3.0 7.6

Fu.ve. 16/920.5 22.4 39 0.4 B 2.7 11.0

Fu.se. " 24.0 22.A 45 0. 19 2.6 6.9

Fu.ve. 21/10 18.6 26.4 30 3.0 7.7 Fu.se. " 24.4 26.4 27 3.0 6.6 Fu.ve. 24/1119.7 24.9 31 2.8 7.2 Fu.se. 20.6 24.9 34 3.7 8.6 Fu.ve. 21/1221.4 29 1.92 7.7

" •Unitkg K g : ' dry weight.

Table 4. A. Strontium-90, Cesium-13d an 7 Cesium-134 in fish froe Nortth ma Se h purchasen i d Ringkabing in September 1983

Species Bq 9°Sr kg'1 Bq 90Sr (kg Ca)"' Bq 137Cs kg"' Bq 137 g K)~C(k s ' 134Cs/'37Cs

Cod 0.022 30 (16.3) 5.1 1450 0.028

Plaice 0.0152 23 (16.6) 0.91 360 Herring 0.009 A 29 A( 6.0) 4.1 1320 0.032

Bone levels are shown in brackets. Table 4.B. Strontium-90, Cesium-137 and Cesium-134 in fish from inner Danish waters purchased in Hundested in September 1983

9 1 9 1 1 Species Bq °Sr kg" Bq °Sr (kg Cap Bq 137 Cs kg' Bq 137 g K)~C(k s 1 134Cs/137Cs

Cod 0.052 64 (47) 4 .9 1190 0.014

Flounder 0.056 40 (30) 3 .8 840 0.027 Herring 0.026 51 (8.4) 5 .2 980 0.024

Bone level se showar n in brackets.

Table 4.C. Strontium-90, Cesium-13 Cesium-13d 7an fisn i 4 h collectee th n i d Cattega d Roskildan t e fjor n 198i d 3

Species Location Date Bq 9°Sr Bq 90Sr Bq 137Cs Bq 137Cs 134Cs/137Cs kg-1 (kg Ça)"1 kg'1 (kg K)"1

Herring Roskilde f j . April 0.028 64 (14.3) 4.6 1060 Garpike Kikhavn 5/5 9.3 2300 0.022

Bone level showe ar s n in brackets.

Table 4.D. Strontium-90, Cesium-13 d Cesium-13an 7 n fisi 4 h meat e caughth n i t Baltic Sea in 1983

90 9 137 137 1 37 Species Location Date Bq Sr Bq °Sr Bq CS Bq Cs 34CS/1 CS kg'1 (kg Ca)~1 kg'1 (kg K)"1

Flounder Bornholm 17/11 0.047 78 2.4 580 Herring* 54°52'N 13°27'E 20/10 0.010 A 24 A 1.82 530 Herring* 55°00'N 13°58'E 27/10 0.015 A 42 A 3.4 910 0.027 Cod* 55°44'N 20°10'E 24/10 0.057 72 2.5 690

«Caught from the R/V DANA.

Table 4.E. Gamma-emitting radionuclide n fisi s h meat O collecte Barsebäckt a d , locatio 0 (55°45'933 n N 12 52'72E)( 1983. (Unit: Bq kg"1 fresh)

Species Date 137Cs

Dab 3/5 0.084 A 3.5 Cod 3/5 0.180 6.7 REFERENCES:

Table 4.F. Gamma-emitting radionucliden i s . Environmentaal . Aarkrot 1 e . A g l Radioactivit n Denmarki y . fish meat collecte Ringhalst a d , locatio, 14 n April 15, 1983. (Unit: Bq kg"1 fresh) Riso Report s, 107 85 Nos , 63 .130 , 154, 180, 201, 220, 245, 265, 291, 305, 323, 345, 361, 386, 403, 421, 447, 469, 487 (1962-1984) . Species 65Zn 137Cs 2. Harley J.H. (editor), HASL procedures manual HASL-300 (1972). Dab 6 2. 0.2 A 9 Flounder 1 .85 Livingsto. 3 n H.D., Bowen V.T Kupfermad .an n S.L. Radionuclides from Windscale Discharges II: Their Dispersion in Scottish and Norwegian Coastal Circulation. Journa f Marino l - Re e search, Nov. 1982.

4. National Research Council of Canada, Radioactivity in the Tabl . 5 eCesium-13 d Cobalt-6an 7 Hytilun i 0 s edulis flesh collecte n innei d r Danish waters in 1983. tUnit: Bq kg~1 dry weight) Canadian Aquatic Environment NREC No. 19250 (1983)

Location Date % dry Depth 1 37Cs 106Ru 60Co 40K. . Carabra5 y R.S., Annual Discharge f certaio s n long-live- ra d matter in m dionuclides to the sea and the atmosphere from the Sella- field Works, Cumbria 1957-1981. AERE-M 3269. Harwell 1982. 57°00'N 10° 18'E Hais 1/8 13 .3 2.7 A 8.9 57°03'N 9°42 •E Gjal 2/8 12 .2 0.5 3.6 A 8.8 . Deutsche6 s Hydrographisches Institut, Uberwaschun Meeress de g . 57°00'N 8°57 'E Aratoft 3/8 12 .1 0.5 2.0 7.9 1981981d un 0 , Hamburg 1982 & 1983 . 56°41 'N 8°44 'E Sillerslev 3/8 15 .6 0.5 1 .72 7.8

57°07'N 8°36 'E Hanstholm 4/8 17 .4 0.5 3.2 6 6. 7 0. < 7. Jefferies, D.F., Steele A.K., and Preston A. Further Stu-

57°36'N 9°58 'E Hirtshals 15/3 16 .0 0.5 4.5 20 0.8 17.6 Distributioe th die n o s f 137co n Britisn i s h coastal

57°44'N 10°36 'E Skagen 4/8 15 .8 0.5 2.4 1.1 A 6.0 water . IrisI s- h Sea. Deea researcse p , 713-7329 h 8 (1982)

57°18'N 10°56 'E Läse W 15/4 16 .1 0.5 4.2 < 1.1 11 .0 8. Aarkrog A & Dahlgaard H. Sources of 137Cs and 90Sr in the 57°19'N 1 1°08'E L*s0 E 15/4 15 .8 0.5 3.9 0.66 A 10.9 Danish Straits. Progress Report by 1981 (Rise» National 4.1 57°18'N 10°56 'E Laeso W 10/8 10 .8 0.5 1 .6 A Laboratory 1981) . 55°58'N 12°01 'E Frederiksvsrk 24/3 10 .6 5.1 11 .7 9. Luykx F. and Fraser G. Radioactive Effluents from Nuclear Power Community (March 1983).

. Voipio10 . (editorA , e BaltiTh ) c Sea. Elsevier Océanographie 51 Series. 1980. 52 FINNISH STUDIES ON RADIOACTIVE MATERIALS IN THE BALTIC SEA

Abstract

During several years monitoring programmes have been carriey Finnisb t ou dh scientist e Baltith n i sc Sea, especially in the Gulf of Finland and the Gulf of Bothnia. More detailed information than that avail- abl, howeveris e , neede n ordei d o built r d locad an l ANNEX 3 regional model r predictinfo s e radiatioth g n burden FINLAND e Baltith a aren Se i c a n tfroma o m different potential sources of contamination. n additioI e monitorinth o t n g programme opet a s n around se an ae nuclea th d r power plants, special stud- ies were designe n ordei d o improvt r e informatioth e n on factors influencing the accumulation of 90Sr and 137Cs by fish and on the availability of 9°Sr, 137Cs, po3*o ' pirn Pu and ?U1 Am to biota at lower trophic levels. This report summarize e speciath s l studies above, 9 13Y 239 240 and the present inventory of °Sr, Cs and > pu e Baltith n i c Sea site-specifiA . c hydrodynamic model is also outlined. PART 1 Simultaneously, the input with the saline component INVENTORIEE TH CERTAIF SO N LONG-LIVED RADIONUCLIDES e Baltith a wate f s o Se cbecom ha r e more important. BALTIE TH A N CI SE Consequently s beeha n t i necessar, e morus e o t y accurate estimates for the inflowing and outflowing . SALOA . TUOMAINEK , N water masses transported through the Danish Straits Finnish Centre for Radiation and Nuclear Safety than those in the earlier papers for the mass balances of these nuclides in the Baltic Sea. A. VOIPIO As in the earlier papers, we have considered Institut f Marineo e Research e differenceth s between annual storage estimates Helsinki, Finland (A) based on measurements of the radionuclide concentra- a watetionse n ri s samplee "calculateth d an s d values" n 196I 0 a modest monitoring programme concerning e estimate e th summinbase th f o n r o p varioudu fo gs s e content th e long-liveth f o s adionucr dn i s e d 1i balanc s inventorieC e d terman r ssS (A" e 1)Th . the Baltic Sea was started by Finnish scientists. of 1961 were used as basic values to which the annual Later this project has constituted an important contributions by different balance terms were added. part of a wider monitoring programme of the aquatic These terms includ e contributioth e direcy b n t deposition environment being carried out by the Finnish authorities a surfacse e oth ne (precipitation), runof d infloan f w responsible for radiation protection. throug e Danisth h h Straits, whil e outfloth e w through The other countries roun e Baltith da hav Se ce e Straitth d radioactivan s e decay were negativth e e one after another also established their own national terms. The difference between these two quantities research and monitoring programmes. evidently reflect other factors removing radionuclides The resulte Finnisth f o s h programme have froe wateth m r phase. been published and discussed in several papers /1-3/, Tabl I elist e differenth s t volume aread an s s in addition to the original data included in the e varioufoth r s subregion e Baltith a /4,5 f Se o cs / various volumes of the STL Reports (see e.g. refs. an e dradionuclid th Figs 5 1- . e concentrations used 6-9). in the calculations. For run-off of 1 ^7 Cs only Durin e firsth g te studyearth f yo s period, e concentrationth hal f o f n Figi s .2 were used, the deposition directly on the sea surface was the becaus e weighe th x elarges si e d th t mea r riverfo n s 1 S7 most pronounced source of the radionuclides Cs discharging into the Baltic Sea yields half of the QQ r originatinS and g froe nucleath m r weapons tests. weighed mean for Finnish rivers. The values are However, its share has decreased from the amount given together with a reference to sources of original of 80-90Î of the total annual increase of these s dataC , d somdataan e n r additioI S . o t n 7 1^ QQ p-jq 240 nuclides to the present share of some 10-20Ï only. dat n £--o a);7 > t™pe alsar u o availabl a waterse r ,fo e 53 54 TABL . I EVolume d areaan s e calculationss th use n i d .

a areSe a volume soft bottom hard bottom (km3) (km2) (km2)

Gulf of Bothnia Bothnian Bay 1500 16000 21000 Bothnian Sea 5200 40000 39000

Gulf of Finland 1100 16000 14000

Baltic Proper 99000 110000 above halocline 10000 below halocline 3500

Gul f Rigo f a 7000 12000

Total 21300 178000 + 196000 = 374000

Annual Volumes (km3) 3 43 Inflow Outflow 866 Run-off 433 4 -6 2 -6 0 6 -70 -72 -74 -76 -78 -80 -82

Fig. 1. Strontium-90 and caesium-137 deposition (Bq m ) showing concentrations from 0.00 o t 0.05m q 3B in Finland. (References 2,3,6-9). between 1979 and 1982 79,10,117. In thi se ablpape ar o report e w r t also several 137 9 23 2f40 data on the contents of Cs, °Sr and 9> pu e sedimenth n i t samples collected from various parts of the Baltic Sea and consider their importance e materiath n i l balance estimates together with some other data available from various sources 79,16, 19-287. Bqnr3

137 3 o BOTHNIAN BAY 50 Cs Bam' 70 - « BOTHNIAN SEA RUNOFF D GUL F FINLANFO D 40- 60 - o 90 D» O °rm* g CD to) tat 137, n Cs 30 50- 20 to) ° 8 18> • . . ,_,<-•» . >8 8 40 10-

30-- -J—i—i—i—i—l—i—l—l—i—i—l—l—i—i—h 2 -8 0 -8 8 -7 6 -7 4 -7 2 -7 0 -7 8 -6 6 -6 4 -6 2 -6 0 -6

0 20 Sr 50- a n o o o (o) 10-- 40- (O) (CD)

30- • (•) (•) (t) (•) (o; (O) D D -I—i- 2 -8 0 -8 8 -7 6 -7 4 -7 2 -7 0 -7 8 -6 6 -6 4 -6 2 -6 0 -6 '•> («i ; «

20 O (O)

Fig. 2. Estimated average concentrations of strontium- 10 -8 90 and caesium-137 given in Bq m in run-off from Fin- land inte Baltith o cr calculatin SeaFo . e inventorth g y -60 -62 -64 -66 -68 -70 -72 -74 -76 -78 -80 -82 f caesium-13o e valueth 7 n Figi s . were devideo tw y b d e text)(seth e . (Reference , 6-9)3 , 2 .s Fig. 3. Estimated average concentrations of strontium- 90 and caesium-137 given in Bq m in the Bothnian Bay, Bothnian Sea and Gulf of Finland. Years 1960 - 1967 based on the Finnish values only, years 1968 - 1973 USSR values for Gulf of Finland and the years 1974 - 1982 are based on the Finnish, Polish, USSR and GDR e valuevaluesth r n bracketi sFo . direco n s t measure- ments were availabl d thee estimatean e ar y e basi th n so d of nuclide ratios. (References 2,3,6-9,11-14). 55 56 3 m- 137 q CB s BALTIC PROPER 3 - 137 OD 0S„ bq m DANISH SOUNDS. 50 50 o below halocline • bottom o surface o above halocline • o _ • • • o • o 40 0 0 40 Co) • C*) « »

) (0 • 0 o o C»° )• C») C«) 30 * ) (« (« ) ) (• C») (8 ) - 0 O 30 • • . • ) (o * o C») o 0 0 - ) (o ) (o ) Co ) (o 20 • 20 -0 * 00 °0-*«»- ° 0 0 ° o~ 0 8 5 0 («) . 0 0 0 0 0 * 10 10

* 1 . • 1 1 1 1 1 1 1 1 t 1 t l 1 1 1 I t -60 -62 -64 -66 -68 -70 -72 -74 -76 -78 -80 -82 6 4 '-7-7 -6 8 4 2 -7 -6 '-8 2 0 2 0-7 -6 -8 0 -7 8 -6 6 -6

3 - 90g g 50 m r 50 - 30Sr Bq m'3

_ 40 40 g G» o O 30 0 ° ° Co.) 30 - C» 0 * . ° 0 . ° 00 ° • ° ° ° ° o ° ° (a • ° 808 . * 8 ° o • o * II o ö _ " ° 2 » ° • * 20 ') t« l H • • 20 ~ c§ (») C«) • CO • • 0 ° . . " 10' 10 .

-60 -62 -64 -66 -68 -70 -72 -74 -76 -78 -80 -82 -60 -62 -64 -66 -68 -70 -72 -74 -76 -78 -80 -82

Fig. 5. Estimated average concentrations of strontium- Fig. 4 Estimate. d average concentration f strontiumo s - 90 and caesium-137 given in Bq m~^ in the Danish St- d caesium-13 e Baltian th 0 9 n i c Pro m 7 -q giveB n i n raits. Years 1961-196 e base ar 7n Danis o d d Finnisan h h per. For the basic material see text for Fig.3. Since values and years since 1968 on Danish values. Stations 1978 additional values measure y scientistb d s from Fede- o witrepresen/o h 0 salinitie 2 inflowine - th t 5 1 f go s ral Republi f Germano c y were used. (References 2,3,6- wate °/o9 r- o8 (bottom represen f o d outflowe an ) th t - 9,11-19). ing water (surface). (References 2,3,19-22). We have useo differentw d t type f calculationo s s sedimentation rates, which would yiel e amountth d s to estimate the total amounts of these radionuelides of radionuelides estimated to be present in sediments bound to bottom sediments. by the other methods. Firstl e content th e ynuclide e th sof th f to sn i s To check the importance of biota in removing and hard sediment samples per square meter from or binding these radionuelides, and to estimate differen a arease t s were multiplie e areath y sb d the total amounts of radionuelides likely to be f d sofharo an dt bottoms respectively e areaTh .s bound to biota the rough estimates of the annual f o sofd haran dt bottoms were estimated froe th m eateh of fish of 10 tons and a very crude estimate maps provide Winterhaltey b d l /4/a t e r. of total biomass of 50x10 tons were used with the Secondly, the average nuclide contents per kg highest radionuclide concentrations in biological dry weight of sedimenting material for three periods samples. This calculation yields at the most a couple Q 0 137 f o years (8a+10a+10a) since 1955 were estimated d -''C an a coupl r d S sf an GBqo ef o TBq r s fo s and these concentrations were then multiplied by for 239'240Pu. the total masses deposited in the respective sea Tables II-V show the more or less processed areas n additionI . e estimatew , e (virtualth d ) data.

TABLE II. Strontium-90 inventory in the Baltic Sea.

Year Total Deposition -i- Runoff + Inflow - Outflow - Decay = 1961+ A' A1 - A storage in water A P R I 0 D = A' (TBq) (TBq) (TBq) (TBq) (TBq) (TBq) (TBq) (TBq) 1960 210 1961 283 1962 319 58.0 11.3 8.2 16.5 6.8 337 18 1963 437 101 .0 11.3 13.0 26.0 7.7 429 -8 1964 593 159.3 33.8 14.3 28.6 10.5 597 4 1965 686 55.4 29.0 16.0 32.0 14.2 651 -35 1966 637 29.2 22.5 11.3 28.6 16.5 669 32 1967 765 18.0 22.5 11.3 26.0 15.3 680 -85 1968 662 10.5 18.6 (8.2) 20.8 18.4 678 16 1969 601 7.9 16.0 (8.2) 20.8 15.9 673 69 1970 563 7.9 14.7 (6.5) 18.2 14.5 670 107 1971 550 11 .6 12.1 6.5 20.8 13.5 666 116 1972 546 7.1 12.1 9.5 19.9 13.2 661 115 1973 501 4.5 13.4 6.5 18.2 13.1 654 153 1971 525 5.2 10.4 9.5 23.4 12.0 644 119 1975 517 6.0 10.0 8.2 26.8 12.6 629 112 1976 567 1.3 9.1 7.4 19.9 12.4 614 47 1977 544 2.0 8.2 10.0 22.5 13.6 598 54 1978 537 6.4 8.7 11.3 25.1 13.1 587 50 1979 478 3.3 7.4 9.5 19.9 12.8 574 96 1980 483 1.6 6.9 10.4 19.1 11.5 562 79 1981 475 2.5 7.4 10.0 19.1 11.6 552 77 57 r valueFo n bracketi s s data missing TABLE III. Caesium-137 inventory in the Baltic Sea.

Year Total Deposition + Runoff + Inflow Outflow Decay = 196A 1 - +' A û < storage in water A P R I 0 D = A' (TBq) (TBq) (TBq) (TBq) (TBq) (TBq) (TBq) (TBq)

1960 198 1961 302 1962 379 92.8 3.2 9.5 22.5 6.9 378 -1 1963 629 161.9 1.0 19.1 28.6 8.7 526 -103 1961 717 219.9 7.1 17.8 38.1 11.5 718 -29 1965 (596) 95.1 1.0 16.0 35.5 (17.2) 781 185 1966 711 11.1 3.2 11.3 35.5 13.7 793 19 1967 757 23.6 2.1 13.0 28.6 17.1 787 30 1968 711 11.6 2.2 (11.3) (19.1) 17.1 778 61 1969 672 10.1 1.7 (11.3) (19.1) 16.1 769 97 1970 615 10.5 1.7 (11.3) (19.1) 15.5 761 116 1971 517 16.5 2.3 (11.3) (22.5) 11.8 751 207 1972 191 10.2 1.7 (16.0) (19.1) 12.6 750 256 1973 192 5.5 1.1 13.0 21.7 11.1 737 215 1971 192 1.6 .3 18.2 29.1 11.3 720 228 1975 163 8.2 .2 15.6 23.1 11.3 710 217 1976 381 2.0 .0 16.9 26.0 10.6 691 310 1977 131 2.2 .0 18.2 26.0 8.8 680 219 1978 351 6.1 .0 16.5 17.3 9.9 677 323 1979 362 1.0 .2 15.6 16.5 8.1 673 311 1980 361 2.1 0.9 16.5 16.5 8.3 668 301 1981 316 3.3 1 .0 22.5 17.3 8. U 669 323

For values in brackets data missing

TABLE IV.

QO 1^7 23QP40 Sr, Cs and ' Jy Pu per unit area in the soft bottoms and their total amounts e differen if th n1970'so d en t. e sub-areath t e Baltia th a f o Se cs

Amount r unipe s t~ aream q B , Total amountsq TB 3, soft bottoms hard bottoms0 9 137 Sea area °Sr Cs 239,210pu 90Sr 137Cs 239,240pu 90Sr 137Cs 239,210pu

Gul f Bothnifo a Bothniay Ba n all samples 96 1300 130 1.5 21 2.0 0.10 5.6 0.26 open sea samples 78 500 76 river mouths 106 2200 150 Bothnian Sea all samples 100 3800 100 opea samplese n s 71 2100 98 3.0 95 3.9 0.59 19 0.39 coast d rivean s r mouths 86 3600 88 Gulf of Finland l sampleal s 88 2700 130 opea samplese n s 83 2000 120 1.3 32 2.0 0.23 5.1 0.17 coast d rivean s r mouths 92 3100 130 Baltic Proper l sampleal s 21 550 18 open sea samples 38 710 51 3.7 70 1.7 0.81 15.7 0.60 Gul f Rigo f a (90) 1500 (120) 9 9. 0.70.599 0.2 1 0.13. 1 1 8 22 13.10.1 3 12. 19.6 1. 1

calculation e basear s open a o sampled se n l ssample e al Bothnia excepth n o r y fo st Ba n values used for hard bottoms are 1/5 of soft bottom values for Sr and •''Cs and 1/10 for 239,210 anapw u fe base iya sen o ds evaluated fro e e valueGul th mth f Finlan o ff o s d 9 137 2 CONCLUSIONS TABL . CalculationV E amounte th f f °Sro so s , d 39,240Csan pu in bottom sediments base n estimateo d f concentrationo s s in sedimenting material and the assumed sedimentation In this preliminary report we would like to rates of 0.3 mm a for Baltic Proper and 4 mm a list the following conclusions without too deep for the Gulf of Finland and the Gulf of Bothnia. discussions . 1. The good agreement between the annual changes in the inventories of 90 Sr and 1 JI37Cs calculated Gulf of Bothnia Gulf of Finland Baltic Proper Total on the basis of sea water analyses and input-output (sedim. rate (sedim . rate (sedim. rate inventory ) i ) ~ ma m « mm a'1) 0.3 mm a ) data support the reliability of our basic data and (Bq kg"1) (TBq) (Bq kg"1) (TBq) (Bq kg~1) (TBq) (TBq) estimates of the radionuclide contents in various compartments of the Baltic Sea as well as of the various mass balance terms. 1955-62 0.13 0.52 0.61 0.19 0.37 0.07 e differencTh . 2 e betwee e quantitieth n s 1963-72 1 .3 2.0 2.5 0.95 1.8 0.10 A1 - A excluding one or two years has all the time 1973-82 3.3 5.0 2.3 0.87 3.6 0.79 been positive thus reflectin n additionaa g l mechanism 11 f removao f nuclideo l s froe watemth r phase. 3. The main mechanism referred to under paragraph s evidentli 2 y sedimentation, sinc e totath e l amounts 1955-62 5.3 6.1 13.« 1.2 8.1 1.5 1963-72 31 51 98 37 50 11 found on the basis of sediment analysis are of the 1973-82 73 110 133 51 83 18 same orde f magnitudo r s differencea e . A - ' A s The first approximation used in calculations, i.e. 290 the sediment values from the deepest parts of the 239,210Pu different basins, representing often also the greatest 1955-62 0.12 0.15 0.65 0.20 0.23 0.01 sedimentation rate, most probably yield too high 1963-72 5.1 7.7 5.1 1.9 6.6 1.5 estimates for the total amounts found in sediment. 1973-82 6.2 9.1 5.0 1.9 3.9 0.86 The radionuclide amounts r bouno remove o t dy b d 21 biota are of minor importance. e deviatioTh . 4 n betwee e A value th - n 1 A s e wateith n r phas n comparisoi e e totath o lt n amount QO in sediment is greater for Sr than for ICs. on It may reflect the easier mobilisation of Sr from the sediment surface than tha f Jo t'C s 1whic 37 s i h rather firmly bound to the clay particles. The remova0 l24 oQ f3 2 -"'Pu from the water phase seems to be most efficient of the three nuclides studied, 59 the total inventory of plutonium in water phase bein whilq e gsedimenTB th e onl 2 0. y t analyses yield the sedimentation rates t I woul. d also explain abou 0 time10 t s higher inventorie n bottoi s m sedi- e sometimeth s significant difficultie o repeat s t ments. Caesium-13 s i nearl7 y equally distributed observations of radionuclide concentrations in sediment between water and sediment phase, while more than samples taken with different sampling devices. 90? of strontium was in the water phase at the end Often e differenth , t samplers var n collectini y g of 1970's. e softesth uppermosd an t t sediment. 5. The amount of radionuc1 ides deposited a floo n alsse e estimateca e b ro o th ne basith n so d ACKNOWLEDGEMENTS of the mean rate of sedimentation and the mean concentra- tion of nuclides in the sedimenting material, estimated We wis o exprest h r l thankthoseal ou s o t s , e sedimenth f o t cores e calculationsTh . , using and especially to Mrs. Marketta Puhakainen and Mrs. Ritva e meath n e valueannuath f o sl rat f sedimentatioo e n Saxèn, who have provided the original Sr and (a few tenths of millimeter) given in the literature, dat e areport th use n i d . yield much lower values than those given in Table V. Sedimentation rates of as high as 4 mm a" for the Gul f e Finlano Gul fth f 3 o Bothnid f0. an dd an a mm a" for the Baltic Proper are needed to yield REFERENCES similar inventorie e estimateth s a s s base n sedimeno d t analyses. 1. d VoipioSaloan . , 1966 A ,e A. ', th J'C n .O s 137, 6. One factor likely to influence the situation QQ and ^ Sr ratio in Baltic waters. In Radioecologi- mentioned under paragraph 5 could be the following. cal Concentration Processes, ed. Aberg, B. & The primary deposition of radionuclides on the sea Hungate . F ,Pergamo n Press, Yorkw OxforNe ,& d floo s greatli r y regulate y scavenginb d g processes pp. 827-833. together with biological or other organic material. . 2 Voipiod Salo , an 1971e balance A. . th , A n , O . s When this organic matte s decomposei r e radionuclideth d s of e Balti 90137d th S an Cn ri cs Sea. Nordic are evidently liberated into water. Depending on Hydrology 2 (1), pp. 57-63. their "affinity e sedimenth o t " t material e radionuth , - . 3 d VoipioSaloan . , 1981A A. , , . Balancf o e clides however e minerae bounth ar ,o t d l particles 1 37 Sr-90 and Cs-137 in The Baltic Sea revised present in the sediment. Thus, Cs will be bound 1978. Marine Pollution Bulletin, Vol 12, No o clat y particles e enricheb y , ma n whili r dS e QO . 218-224pp , 6 . the temporarily sedimented material very rich in . 4 Winterhalter , FlodénB. , , IgnatiusT. , , H. , water organic matter. This rather mobile matter Axberg, S. and Niemistö, L., 1981. Geology s i absent both froe permanentlmth y sedimented material e Baltioth f c e BaltiSeaTh n cI . Sea. ,ed and from the water phase. The latter mechanism Voipio . A Elsevie, r Océanographie Serie, 30 s should result in much more even areal distribution Amsterdam, pp. 1-121. f depositeo d nuclide s coula s e expecteb d d from . 5 Melvasalo , PawlakT. , , GrasshoffJ. , , ThoreilK. , , 13. Study of strontium-90 and caesium-137 concentration d Tsibanan . . A L (Eds., ) 1981. Assessment e open coastath i nd n i Baltian la waterSe c s e effectth f f o pollutioo s e naturath n o n l of the GDR in the period 1975-79. National resources of the Baltic Sea, 1980. Baltic Board-for Nuclear Safety and Radiation Protection Sea Environmental Proceedings No 5B. of the GDR. Presented at the IAEA Technical . 6 Studie n environmentao s l radioactivit n Finlani y d Committee Meeting Vienn 9 Jul5- a y 1982. 1978. Annual Report STL- . Institut32 A f o e 14. Study of radioactive contamination in the open Radiation Protection, Helsinki. n coastai d Baltian la e waterSe GDcth Rf o s . 7 Studie n environmentao s adioacitivitr l n i y e perioth n i d 1980-81. National Boarr fo d Finland 1979. Annual Report STL-A 34. Institute Nuclear Safet d Radiatioan y n Protectiof o n f Radiatioo n Protection, Helsinki. e GDRth . Departmen f o Nucleat r Environmental 8. Studies on environmental radioactivity in Finland Protection. Presented at the IAEA Technical 1980. Annual Report STL- . Institut38 A f o e Committee Meeting Vienna 5-9 July 1982. Radiation Protection, Helsinki. 15. Ivanova, L.M., 1978. Investigations on the . 9 Studie n environmentao s l radioactivit n Finlani y d radioactive pollution in the Baltic Sea (in 1981. Annual Report STL-A 40. Russian). V.G. Khlopin Radium Institute, Leningrad. 10. Miettinen, J.K., Leskinen, S. and Jaakkola, 16. Radiological Investigations in the Southern , 1982T. . Studie n distributioo s f actinideo n s Baltic Sea during the years 1975 to 1981. between seawate d particulatan r e fractions Presente . BaranskDr y b d i (Polande th t a ) in the Baltic Sea and its gulfs. In Transuranic IAEA Technical Committee Meeting Stockholm cycling behaviou e marinth n i er environment. 22-26 August 1983. IAEA-TECDOC-265. IAEA, Vienna. 17. Kautsky , 1981H. , . Radiological investigations . 11 Lazarev, L.N., Gedeonov, L.I,, Ivanova, L.M., in the Western Baltic Sea including Kattegat Oleneva, N.A., Orlova, T.E., Vakulovsky, S.M., durin e yearth g s 197 5o 1980t . Deutsche Hydrograp- Nikitin, A.I. and Chumishev, V.B., 1982. The hische Zeitschrift, Jahrgan , Hef. 34 g4 t conten f strontium-9o t d caesium-13an 0 n i 7 . 18 Kautsky Eicked an . H , , H-F. Radiological investiga- the water of the Baltic Basin 1979-81. L82- e westertion th e Balti n th i s n d Baltican a Se c 22057. English translation froe originath m l Proper, includin e Danisth g h Straits, During paper published in Radiohimija No 5, 1983 pp. 669- 1981. Deutsche Hydrographische Zeitschrift, 675. Jahrgang 35 pp 211-221. 12. Lazarev, L.N., Gedeonov, L.I., Ivanova, L.M., 19. Aarkrog, A., Better-Jensen , L., Dahlgaard, Orlova, T.E., Tishkova, N.A., Vakulovsky, S.M., H., Hansen, H., Lippert, J., Nielsen. S.P. and Salo, A., Puhakainen, M., Saxén, R and Tuomainen, Nilsson, K. 1979. Environmental Radioactivity K., 1983. Study of the Radioactive Contamination n Denmari n i 1978k . Ris«5-R-403. Risrf National of the Baltic Sea in 1979-80. STL-B-TUTO-23. Laboratory, Denmark. El Institute of Radiation Protection, Helsinki. . 20 Aarkrogß2 , Better-JenA. , , DahlgaardL. , n se , 25. Aarkrog, A. and Lippert, J. 1977. Environmental H., Hansen , LippertH. , , J. Nielsen, , S.Pd an . Radioactitivy in Denmark in 1976. Ris<5 Report Nilsson, K. 1980. Environmental Radioactivity No 361. pp. 92-96. n Denmari n 1979i k - Risrf-R-42 1. Risrf National 26. Aarkrog, A., B«Stter-Jensen , L., Dahlgaard, Laboratory, Denmark. H., Hansen, Heinz, Lippert , NielsenJ. , , S.Pd an . . 21 Aarkrog , Bitter-JenseA. , , DahlgaardL. n, , Nilsson, Karen. 1978. Environmental Radioactivity H., Hansen, H., Lippert, J., Nielsen, S.P. and in Denmark 1977. Risrf Report No 386. p. 38 Nilsson . K 1981, . Environmental Radioactivity and 109. in Denmark 1980. Ris«5-R-447. RiseS National . 27 Bojanowski , SkibaR. , , TomzakD. , . J ,1976 . Laboratory, Denmark. On the Recent Levels of 90Sr and 1^7Cs in the . 22 Aarkrog , Better-JenA. , , DahlgaardL. , n se , Baltic Sea. Proc. X-th Conf. Baltic Oceanogr. H., Hansen , LippertH. , , J. Nielsen, , S.Pd an . Göteborg, 2-4 June 1976. Nilsson. K. 1982. Environmental Radioactivity . 28 Lazarev, L.N., Gedeonov, L.J., Ivanova, L.M., in Denmark in 1981. Ris«S-R-469. Ris«S National Orlova, T.E., Stepanov, An.VI., Flegontov, Laboratory, Denmark. V.M. The Content of Strontium-90 and Caesium- . 23 Aarkrog Lippertd an . A . ,J , 1974. Environmental 137 in Some Areas of the Baltic Sea in 1982. Radioactivity in Denmark in 1973. Danish Atomic Presente e IAEth At a dTechnica l Committee Meeting Energy Commision. Ris<5 Report No 305. Stockholm 22-26 August 1983. 24. Aarkrog, A. and Lippert,J. 1976. Environmental Radioactivity in Denmark in 1975. Research Establishment Risrf. Ris<5 Repor 345- .No t PART 2 In this study the influence of several hydrographi- s C J l factor e ca accumulatiod th an n r o sS f o n QO 137 ACCUMULATION OF CERTAIN LONG-LIVED RADIONUCLIDES n s studiefisi wa h n differeni d t areas alone th g FISY B H Finnish coast. Special attention was paid to seasonal variation in water quality.

E. ILUS, R. SAXÉN, T.K. TAIPALE MATERIA D METHODAN L S Finnish Centre for Radiation and Nuclear Safety, Helsinki, Finland Sea water samples (100 1) were taken five times a year from three areas alon e coastth gsampline Th . g areas were Oulu, Tvarminn d Loviisan e a (Fig) 1 . and the sampling times March, May, August, September The brackish water characte e Baltith f o cr and November in 1982 (Table I). The sampling station Sea is extraordinary clear in the inner parts of e Gul th f Bothnio f d Gul f an Finlandao f , where th e at Oulu was rather exposed, whereas those at Tvarminne and Loviisa were situated mor r leso e s inside th e inflow of river waters is significant. Especially QQ 13J 7 in late winter and early spring, when there is plenty archipelago. Apart from Sr and ' Cs, the water samples were also analysed for salinity, pH, colour, of thawing water flowing into the sea and the gulfs particulate material and organic carbon. Furthermore, are mostly ice-covered, the river waters are spreading in the Olkiluoto area, sea water samples were taken on extensive areaa thi s na s fresh water layer under QO 137 four times a year for ' Sr and 'Cs analyses in the ice. Except in the water salinity values, this J connection with the surveillance programme by the can als e seenb o , among other thingse colouth n i ,r power station. numbers of water, which usually are caused by humic Baltic herring (Clupea harengus d pikan )e (Es.ox substances transporte y riversb d . lucius) were chosen for the fish species to be studied, Since 1977, radionuclide analyse f piko d s an e becaus f theio e r economic importanc differend an e t Baltic herring have been included in the continued living habits. a stationarPik s i e y predatory fish monitoring programme by the Institute of Radiation living almost all of its lifetime usually within Protection in the coastal areas of Finland. According a smal ls originalli area t I . a yfres h water fish, r earlieou o t r results /1/, some areal differences have been found in the accumulation of QQ Sr and but in Finland it is common in the whole country bot n fres i hbrackisd an h h water t I prefer. s shallow 13 7y fishCb s . However s beeha n t i obvious, , that on 137 coastal areas with rich vegetation. The young individ- our previous knowledge of ' Sr and -"Cs concentrations ualt evertebrateea s e adultth d san s mostly other e influenc a th wate se d an n ri f wateo e r quality fish species, like roach, perch and Baltic herring. on the accumulation have been inadequate to decide f piko Normally s e i beloe ag 0 yeare 1 wd th an , s whether one and the same or various concentration the catching size 1-3 kg. In 1982, the total catch factors e (CFentir th e vali r ar ) efo d coas n modei t l f piko n Finlani e 0 tonss abou 70 f wa whic do 7 , t h calculations. 63 0 ton70 1s were froe seath m . 64

TABL . I E Resulta watese f ro s samples taken five time a yeas t Oulua r , Tvàrminne Oulu and Lovus n 1982i a .

1 40K Sampling °/oS statioo n pH Colour Particulate Org.C 9°Sr 3TCs material mg Ptl"1 mgl mgl Bqm"

Oulu March 1 .02 6.7 35 1 .0 8.0 17 7.8 380 Tvàrminne " 1.80 7.0 22 1 .9 5.4 16 4.8 640 Lovusa " 0.43 6.9 32 4.8 7.0 21 1.3 190

Oulu May 2.09 6.9 26 2.3 5.5 16 8.9 710 Tvàrminn6 e " .50 7-7 12 0.3 3.8 25 14 2400 Lovusa 3.47 7.2 15 3.0 5.0 22 10 1300

Oulu August 2.72 7.4 12 1 .2 4.6 17 10 920 Tvàrminn5 e " .69 8.1 6 0.9 4.4 25 12 2100 Lovusa " 4.60 8.0 7 10 .7 5.2 24 10 1600

Oulu September 3.41 7.6 8 2.5 3.8 21 13 1500 Tvàrminne " 6.31 7.5 5 2.1 4.1 24 13 2300 Loviisa " 5.13 7.7 8 0.8 4.8 25 10 2200

Oulu November 3.80 7.3 8 2.5 4.6 22 11 1300 USSR Tvàrminn6 e " .88 7.7 6 0.8 3.8 24 16 2700 Lovus5 a " .03 7.3 8 2.3 5.4 25 9.9 1900

Fig . 1 Locatio. f samplino n e gaverag th area d ean s salinities in surface water (°/oo). Q _ Y 1o Baltic herring is a small sized form of herring. TABLE III ., e averag) Th s contentC m a wate se eq n (B ri s s i als d oe Baltian e wholt th I livea th f o Se n eci s the 1 37Cs contents in the edible parts of Baltic herring l e commoFinnispartal th f n i o ns h coast contrasn I . t " e flesfreskg th f pikano n q hi hd(B e weightd )an to the pike, Baltic herring is a pelagic shoal fish, the corresponding CF values in eight areas along the principall a yplankto n feeder, which makes regular Finnish coast. migrations between the coast and the open sea, but Area Average contents Baltic herring Pike returns ever e ysam th yea e o t coastar l are o spawnt a . in sea water 5 1 1 f Baltio e Thag ce herrin s i usuallg y less tha6 n Bq m"- Bq kg - CF Bq kg' CF e normath year d an sl size belo 0 grammsw5 . Economically Oulu 9.6 3.0 310 6.0 630 _ _ seen, Baltic herring is the most important fish Kokkola 9.8a 2.6 270 Vaasa 11*> 2.5 230 5.6 510 species in Finland. In 1982 the total catch was Olkiluoto 12° 1.96 160 3.3S 280 85 000 tons. However, a marked proportion (about Seili 12d 2.1 180 4.1 340 Tva'rminne 11 1.8 160 3.8 350 50-60 %1 from the catch goes to feed fur animals. Helsinki 10e 1.7 170 _ _ The fish samples (5 kg) were taken from eight Loviisa 7.4 1.78 230 3.38 450 areas alon e coasth g t e pik(Figth , e 1) .sample s a n April-Mai e Baltith d can y herring sample n Septemberi s - = sea water values of Oulu used in calculations b = interm«2diate sea water viîluef o s Ould Olkian u : Luoto used in November 1982 e exceptionTh . s from this practice calculations are presented in Tables II and III. averag= ° a watese e r monitorine valueth f o s g programme used in calculations = intermediat d a watese e r value f Olkiluoto s d Tvarminnan o e used in calculations = intermediat e a watese e r value f Tvarminno s d Loviisan e a used TABLE II. The average Sr contents in sea water (Bq m~-^), in calculations f = average value of the monitoring samples in 1979 /1/ the Sr contents in the edible parts of Baltic S = average value of the monitoring samples in 1982 e flesg k th f fres pikn o hq i herrin (B ed h an g weighte correspondinth d an ) F valueC g n eighi s t e e ediblflesth Th f pikd o he an epart f Baltio s c areas along the Finnish coast. herring were analysed for yQ OS r and 13-"7 Cs. The pre- treatmen d analysinan t g method f boto a swate se h r Area Average contents Bait Pike and fish samples have previously been described in sea water -1 -1 Bq m Bq kg CF Bq kg CF e earlieith n r reportr Centrou f o es /2,3/. Oulu 18 0.13 7.2 0.041 2.3 Kokkola 188 0.093 5.2 b Vaasa 19 0.068 3.6 0.043 2.3 RESULTS Olkiluoto 21° 0.081 3.9 0.032f 1.5 Seili 22d 0.064 2.9 0.028 1.3 Tvarminne 22 0.068 3.1 0.026 1.2 The results of the sea water samples taken Helsinki 23e 0.070 3.0 Loviisa 23 0.092 4.0 6 0.0371. f five time a yeas r from Oulu, Tvarminn d Loviisan e a e givee samplinar Th n Tabli n . I eg statio t Oula n u For upper indexes see the list below Table III. 65 represents the northernmost end of the Gulf of Bothnia (jß wit a hsignifican t inflo f wriveo r water from northern e principlth e mentioned above, using mean values parts of Finland and Sweden. This can be seen in e 198oth f 2 monitoring result s basia s c datan I . e salinityth , colou d organian r c carbon values. the other areas, the nearest available concentration The Tvarminne area belongs to the most marine part values and local ice duration data were used (cf. Tables e Finnisoth f h coast. However e effecth , f thawino t g III)d an .I I water s i cleas n earli r y spring even theree Th . The 9°Sr and 137Cs concentrations in fish (given sampling station at Loviisa lies in Hästholmsfjärden, IIId n Tablei an e mainl) I ar I s y base n sampleo d s a semi-enclose n i nea y e nucleaba dth r r power station, e presenth take r fo nt stud n 1982i y . Howevere th , where the effect of rivers is evident e.g. in salinity, results of Olkiluoto and Loviisa are mean values colour, particulate material and organic carbon o samplintw e th g f o periods (Ma d Septemberan y ) values, especially in March and May. used in the monitoring programmes and the 'QO Sr results The averag7 13 e QO Sr and J'Cs contents evaluated for pike are from 1979 /1/. for sea water in the different areas are given in a waterIse n e annuath , l mean concentrations d III Tablemeae an Th .nI I svalue r Oulufo s , Tvarminne of Q' OSr were lowest in the Gulf of Bothnia and highest 137 and Loviisa were calculated by dividing the year in the Gulf of Finland, whereas the Cs concentrations into three periods: were e innelowesth n ri e tgulfs partth f o s. However, the concentrations of both nuclides in fish and 1) froe formatioth m e disappearancth o t n f o e valueF C e sth wer n generai e l e higheinneth n ri r permanen e coveic t r (the winte e period)ic r , parts of the gulfs, especially in the northernmost 2) from the disappearance of permanent ice cover e Gul f th Bothniao e enentirf o th d n I e . material, QO to the end of August (the summer stratification the CF values of y Sr were 3-7 for Baltic herring periodd an ) r pikd fo thos an e2 f an137o e1- dC s 150-30r fo 0 3) froe beginninth m f Septembeo g e formatioth o t r n Baltic herrin 300-65d an g r pikefo 0 . of permanen e coveic t r (the autumn mixing period). Representative concentration values were chosen DISCUSSION r eacfo h e annuaperioth d an ld means were calculated n relatioi e numbeth e differen f o th t dayno r n i s t In spite of adjustments in the average 90,Sr 137 periods. The results for March were chosen to represent s content C a wateranse d e f concentratioo th s, n the first period, the intermediate values of May factors for fish were in a rather good agreement and Augus e seconth t d perio d thosan df Septembeo e r witr previouou h s results /1/. Accordine th o t g and Novembe e thirth r d e duratioperiodic e Th n. present calculations valueF C e e sth ,th wer n i e data is based on the average dates given by Palosuo inner parts of the gulfs somewhat higher than those /4/ for the different parts of the Finnish coast reported earlier. It seems obvious that the areal during 1931-1960. difference se concentratiofounth n i d n factore ar s For the Olkiluoto area the average contents e samth ed t valivaluan no reathud e ds i an eon ls Q 0 137 a watese n i r wers C e calculate d an r S d wit f o h for the entire coast. Due to different living habits, the CF values Sr Pike of 3'Cs for pii

The areal difference valueF C e sth sho n i sw 4 2 4 thae accumulation th d t ^'Can e connecter ar S s * f o ds with other environmental factor e samoun th suc s a ht 1 2 of river water flowing into the sea areas. Some -CF -CF -CF correlations between hydrographical parameters and 234 e concentratioth n factor o pikBaltid t s an e c herring Baltic herring

e meae presenteTh ar n - value3 d n Figsi dan s 2 . mgPftal Colour mg/l Particulate material mg/l Organic carbon 10 e parameteroth f n differeni s t area e calculatear s d 25 5 with the same principle described earlier for the (r.0.97) (r .0.0008) (r.0.79) on i -37 s concentrationsC d averagan correlatione r S Th .e s should be regarded as very rough trends only, because 6

we have only three points (Oulu, Tvarminn Loviisad an e ) 4 in the diagramms. For both radionuclide d botan sh fish species, 2 valueF C e s th see o correlatmt e rather well with -CF -CF colour numbers and values of organic carbon and salinity. The CF values had a positive correlation with colour number d organian s c carbon valued an s Fig. 2, Relationship between some hydrographical parameters and concentration their correlation with salinit s negativewa y o N . factor f ^°So r s pik Baltid fo r an e c herring. Open circl Oulue= , triangl Tvarminne= e correlatio s founwa n d betwee e concentratioth n n and filled circl Loviisa= e . factors and particulate material. However, all e threth e samplin t gfull no area e y ar scomparable . For instance Oulu, with its relatively low content of particulate material n offshora s ha , e character, whereas the two others are inside the archipelago. e o partlcorrelatioThiy reason th y ma se b wh yn n was found betwee e concentratioth n n factord an s particulate material. 67 68 The colour numbers and concentration factors correlated best. As mentioned before, humus is 137Cs Pike e maith n factor affectin e colouth g r r valueou n i s o/oo Salinity mgPr/nl Colour mg/l Porticulate material mg/l Organic carbon waters e resulTh . t could mean that humus increases 10 25 10T the availability of 9°Sr and 137Cs to fish. A very (r-099) (r-0151 (r-087) (r»-095) clear correlatio alss owa n found betwee e concentrath n - tion factors and water salinity. 6 When considerin e resultsth g t i shoul, e b d

4 borne in mind that the hydrographical parameters are not independent, but for instance salinity, 2 colou d organian r c carbo e oftear n n associaten i d different water masses. Thus, one of the parameters -CF -CF -CF 300 400 500 600 300 400 500 0 6060 0 0 50 0 3040 0 0 60 0 50 0 3040 0 can have a predominating influence on accumulation, Baltic herring whil e otherth ehav n ca se onl a quasicorrelatioy n.

o/oo Salinity mgPr/rnl Colour mg/l Particulate material mg/l Organic carbon 5 Wt 10 ACKNOWLEDGEMENTS (r--098) MOO) (r-027) (r-093) The authors wish to thank Jaakko Ojala and 3 Kari Sinkko for performing the gammaspectrometr ic analyses thankr o Markettt Ou e alse .ar s odu a Puhakainen 2 and Kirsti-Liisa Sjoblom for their valuable comments

1 during this work.

0 40 0 30 0 20 100 0 40 0 30 0 20 100 100 200 300 400 100 200 300 400 REFERENCES 1. Koivulehto, M. and Saxén, R., 1981. Accumulation of 90 Sr, 137 Cs and some stable elements in some Fig. 3. Relationship between some hydrographical parameters and concentration Baltic fishes. Report STL-B-TUTO 11, Institute factors of '"GS for pike and Baltic herring. Open circle = Oulu, triangle = of Radiation Protection, Helsinki. Tvarminn d fillean e d circl Loviisa= e . 2. Studies on environmental radioactivity in Finland 1976-1977. Report STL- , InstitutA26 f Radiatioo e n Protection, Helsinki. 3. Studies on environmental radioactivity in Finland 1979. Report STL-A 34, Institute of Radiation Protection, Helsinki. U. Palosuo , 1965E. , e alon.ic Duratio e g th f o n the Finnish coast 1931-1960. Merentutkimuslai. t Julk./Havsforskningsinst. Skr . 219No . . PARTS MATERIAL AND METHODS

Fucus vesieulosus has generally been used as ACCUMULATION OF CERTAIN LONG-LIVED RADÎONUCLIDES a bioindicato e Baltith a arean i Se rc . Undee th r BY LITTORAL ALGAE AND BOTTOM ANIMALS joint Fucus Project of the Nordic Countries the Institute of Radiation Protection has studied the K. TUOMAINEN, E. ILUS, T.K. TAIPALE 0 4 2 Q 3 2 contentu P e Fucutf-nuclid\>th - > n si J7 s sample d an e s Finnish Centre for Radiation and Nuclear Safety, collected from the southern and western coast of Helsinki, Finland Finland in 1980-81 /5,6/. n 1982I , Fucus vesieulosu d unfilterean s a se d In the Finnish coastal areas of the Baltic water samples were collected from eight locations e Sewateth a r salinit s i very y 1-o- 6°/oo 3 w(< ) in the southern and southwestern coast of Finland /?/. and consequently biota is poor in species and the Additional sampling was carried out from 8 locations at Loviisa and from 6 locations at Olkiluoto. The individual e smalar s n sizei l . Furthermore, such -1-37 J 240 e humuth s sa e contenturbiditth d an t f wateo y r samples were analysed for 'Cs , d partlPan u y 241 Q 0 are high. Thus the factors affecting the accumulation r fo Am. s analysewa r S d from samples collected of radionuclide diffey ma s r from e othethosth n i re n 198i d 1980an 1 froe sammth e locations l thesAl . e parts of the Baltic Sea. samples also belonge e Nordith o t dc Fucus Project Since 1975 the Institute of Radiation Protection (Fig. 1) . has carried out radioactivity investigations of mM_o a balticac a benthi s i a e mussel, endemic on 137 some seaweed and bottom animal species. Sr, Cs, for the Baltic Sea. As a link between sediment 1 24 , partlPu 23924y ' 0somd Aman e stable elements an transfey d fishma t i r, radionuclides from sediment have been analysed from annually collected samples back to biological cycle. Different bottom types e environment inucleao th n tw e rth powef o s r stations may affect the accumulation of radionuclides. t Loviisa Olkiluotd an a o /1-4/. n I 198 d 1982an 3 Macoma samples were collected n I 198 d 1982an 3 additional samplee th f o s from eight locations alon e Gul th f gFinlano f d an d seaweed Fucus vesiculosu d bottoan s m animals Macom.a the Gulf of Bothnia (Fig. 1). Additionally unfiltered baitic Mvtilud an a sa wateedulise f rs o wela ss a l and filtered near botto a watemse s wela rs bottoa l m and sediment were collected alon e Finnisth g h coasts. sediment were collected. Sea water was filtered The aim was to complete the earlier studies and through a 0.45 urn Millipore disc filter using a to examine whether the same concentration factors submersible pumpe sampleTh . s were analyser fo d 90*- 137IJI , could be used in model calculations concerning the 'Sr, Cs, '^»""P d "'AmUan determino T . e entire Finnish coast of the Baltic Sea. To explain the character of the sediment, parameters such as e possiblth e areal differencevalueF C e s th n i s organic carbo ignitiod an n n loss were analysed. some water and sediment parameters were also compared. Mytilus edulis is a bioindicator organism of 09 international interest a filte s A .r feede t i feedr s 200k 70 on particulate matter of water and on the Finnish coasts it is important only as a link of food chains. In the northern parts of the Baltic Sea Hytilus is very small in size (0.5 - 2 cm) and occurs only in areas of a salinity of above 4 °/oo. It lives attached to stones, algae etc. In 1982-83 Mvtilus samples were collected from three different types of areas: Olkiluoto (the Bothnian Sea), Houtskari (the d Tvärminn)an e (the Gulf of Finland) (Fig. 1). Larger Mvtilus samples were collected froe Olkiluotth m Houtskard an o i areas for separate analysis of shells and soft tissues. Unfiltered surface sea water was collected from the same locations. Samples were analysed for QQ Sr, 137CSj 239,240pu and 241Am> Salinity as well as organi ce amouncarboth d f particleo an nt s were also determined from water samples.

SWEDEN Analytical methods Gammaspectrometric measurement d determinatioan s n of strontium-90, plutonium-239,240 and americium- 241 were carried out by the methods described /4,8/. Organic carbo s determinewa n a titrimetri y b d c method. Organic matter was oxidized with potassium dichromate in a sulphuric acid solution and the

USSR excess chromat s titratewa e d with ferroammoniumsulphate solution using diphenylamine as an indicator /9/. The ignition loss was determined by igniting 1. Norrskär (Fu) . 8 Tvärminne, Langskär (Fu,My) 2. Vaasa, Bergöfjärden (Ma) 9. Station LL-11a, Hanko (Ma) e t samplhours3 a 550°th r g fo C5 e . 3. Olkiluoto area (Fu,My,Ma) . Helsinki10 , Katajaluoto (Ma) 4. Station Eros-1 (Ma) 11. Pellinki, Lökskär (Fu) 5. Houtskari, Fiskö (Fu,My) 12. Loviisa area (Fu,Ma) RESULTS 6. Seili; Orhisaan (Fu), . Kaunissaar13 i (Fu) Högholmen (Ma) 14. Haapasaari (Fu) 7. Jurmo (Fu) 15. Tammio, Harvajanselkä (Ma) Fucus vesiculosus . Ulkotammi16 o (Fu) e samplinIth n g e pointGul th f Finlando ff o s , • nuclear power station site QQ • other sampling areas , Sr e e ArchipelagBothnia th e th th d a an Se na Se o 137 239 240 2l|1 Fig. Locatio1 . f samplinno g areas. Cs, ' pu and Am contents ranged from 15 to 26, from 5.6 to 11, from 0.10 to 0.30 and Hvtilus edulis from 0.011 to 0.070 Bq kg-1 dry wt, respectively In intact Hytilus samples the 7U90S,r contents p s q pun (Table I). The mean activity ratio of Pu-238/Pu- varied from 5.1 to 6.1, oy> Pu contents from 239,24 s abouwa 0 te entir0.0th n i 5e material. 0.0034 to 0.012 and Am contents from 0.0026 to o "2 Q 240 1 1 37 The mean '--13''- "Pu contents were lower in the Both- 0.0056 Bq kg fresh wt . J'Cs concentrations were nian Sea samples and QO Sr contents higher in the usually below detection limit, 0.13 Bq kg fresh 9 137 2 Gulf of Finland samples than in those of the other e meaTh n . contentwt f o °Srs , d 39,240Can s pu sea areas (Tabl. I) e in shells were 22, <0.13 and 0.033 Bq kg"1 fresh The activity concentration f unfiltereo s d seawater wt, respectively (Table III). There was no significant collected froe samth m e location s Fucua s s were difference in the average contents of the radionuclides used for calculation of concentration factors (Table in the different sea areas. IV). The mean CF value on dry weight basis was The mean concentration factors on fresh weight 137 9 23 90 137 239 2 40 241 r fo r 84 Cs°Srfo 0 0 , 67 ,3900 r fo 9,2400 pu basis for Sr, Cs, ' ' Pu and Am for the and 19000 for 241Am. intact mussel were 240, <9.1, 1300 and 4300, respectively (Table IV). Strontiu d plutoniuman m see o maccumulatt e Hacoma baltica mainly into the shells. In the Hacoma baltica samples the activity 90 137 2 241 concentrations of Sr, Cs, 39,240pu and Am varied from 9.5 to 18, from <0.2 to 1.9, from 0.016 to 0.097 and from 0.007 to 0.029 Bq kg fresh wt, respectively. The average concentrations were nearly the same in the different sea areas (Table II). Using concentrations of near bottom sea water, the concentration factors were calculated (Table IV). The mean CF value on fresh weight basis was 9 137 239 240 650 for °Sr, 48 for Cs, 5800 for ' pu and e factore ArchipelagTh th . n i s Am o200 r fo 0 ?4 1 Sea appear to have the lowest values. Accumulation from sediment was also evaluated by calculating concentration ratiot s we (CR n o ) weight basis t samplin(TablA . V) e g point4 , 3 s 137 239 240 241 and 6 the ratios for Cs, ' pu and Am appear to be higher than the other CR values.

71 Table I. 90Sr, 137Cs, 239'240Pu and 241Am in Fucus vesiculosus (Bq kg"1 dry wt) and surfac secollecte) a m wate q (B rd frosame th me locations alon e Finnisth g h coast.

Fucus vesiculosus 137 239,240 241 Locations Date 90SrC Cs pu Am a wt y dr g Bk q 1. Ulkotammio 28.9.82 26 7.2 0.20 0.030 . 2 Haapasaari 29.9.82 26 6.8 0.20 _e . 3 Kaunissaari 28.9.82 24 7.3 0.20 0.045 4. Loviisa area 25.8.-2.9.82b 26+3 8.6+2.0 0.24+0.05 0.052 5. Pellinki 22.8.82 25 8.8 0.24 0.028 6. Tvarminne 23.8.82 23 7.2 0.19 0.011 7 . Jurmo 18.8.82 18 7.0 0.29 0.028 8. Seili 17.8.82 17 11 0.13 0.017 9. Houtskari 29.7.82 16 11 0.30 0.070 10. Olkiluoto area 5.-9.8.82tp 19+2 8.0+0.3 0.10+0.09 0.035 11. Norrskar 11.8.81 15 5.6C 0.11° -

MeaS.D1 + n . 27 0 1. + + 4 4 8. 0.19 + 0.07 0.035 + 0.018 Median 23 7.3 0.20 0.030 Range 15 - 26 5.6 - 11 0.10 - 0.30 0.011 - 0.070

Sea water (unfiltered) Location Date 9°Sr 137Cs, 239,240pu 241Am Salinity J Bq m o/' oo

1 . Ulkotammio 28.9.82 27 11 0.0059d _ 4.2 2 . Haapasaari 29.9.82 30 9.3 - - 4.3 3. Kaunissaari 28.9.82 29 12 - - 4.5 . 4 Loviis3 a 22.7.82 24 7.6 0.011 0.0026 4.5 5. Pellinki 22.8.82 26 12 - - 5.5 . 6 Tvarminnne 23.8.82 25 14 0.0099 0.0012 6.3 7 . Jurmo 18.8.82 25 13 - - 6.7 . 8 Seili 18.8.82 23 12 - - 6.4 9. Houtbkari 29.7.82 24 17 0.003 - 6.6 10. Olkiluoto 2 15.9.82 24 16 0.005 0.0008 6.2 11. Quark 28.9.82 23 14 - - 3.6 weight/wy a dr mea f o n eweight 0.1s i t 8 ^ mean of 8 locations at Loviisa and 6 locations at Olkiluoto (+1 S.D.) c analysed from samples collecte n 198i d 0 frosoute th m h198n i coas d 1 froan twese th mt coasf o t Finland5^6 d near bottom water e not analysed 90 137 239 240 241 Tabl. SrII e, Cs, - pu an(j MacomAn mi a baltica, near botto watea d se m an r sediments collected from the same locations along the Finnish coast in 1982-83

au iJ Location Date Sr 'Cs . zja,-^upu '""Am Bq kg 1 fresh wta (dry wt)

1. Tammio, Harvajanselka 14.09.83 18 (44) <0.2 1«0.5) 0.019 (0.048) 0.010 (0 .026) 2. Lovusa, stenorarna 13.10.83 15 (42) 0.41 (0.97) 0.016 (0.043) 0.011 (0 .029) 3. Helsinki, Katajaluoto 23.11.83 15 (36) 0.40 (1.1) 0.046 (0.11) 0.015 (0 .035) 4. Hanko (LL-lla) 28.06.82 9.5 (20) 1.9 (3.9) 0.071 (0.15) 0.029 (0 .061) 5. Se 1 1 1 , Ilogho Ime n 10.08.83 11 (32) 0.54 (1.6) 0.019 (0.057) 0.008 (0 .023) 6. Eros-1 29.06.82 - - - - 0.097 (0.19) 0.026 (0 .049) 7. Olkiluoto 2 29.07.83 11 (29) 0.52 (1.4) 0.020 (0.054) 0.007 (0 .019) 8. Vaasa, Bergofjarden 23.08.83 15 (37) 0.40 (1.0) 0.025 (0.066) 0.019 (0 .047)

Mean + 1 S.D. 14 + 3.0 0.62 + 0.57 0.039 + 0.03 0.016 ± ° .008 (34 + 8.2) (1.5 ± 1.1) (0.090 + 0.055) (0.036 •f 0 .016)

Sea water (unfiltered) 2 Location Date 9°Sr 137Cs 239,240pu 41Am Salinity Bq m~3 °/oo

1. Tammio 14.09.83 27 8.3 0.0059 - 3.8 2. Lovi isa 13.10.83 19 8.5 0.017 0.010 5.6 -"- (filtered) 19 12 0.0030 0.0004 5.6 3. Helsinki 23.11.83 25 14 0.013 0.002 6.a 4. Hankob 28.06.82 25 11 - 0.0039 6.4 -"- 09.06.83 - - 0.0060 0.0015 - 5. Seili 10.08.83 25 14 0.012 0.007 6.5 6. Eros-1 29.06.82 22 13 0.020 0.003 6.7 7. Olkiluoto 03.08.83 23 14 0.010 0.006 6.2 -"- (filtered) 15 13 0.003 0.006 6.2 8. Vaasa 23.08.83 19 13 0.0044 0.003 5.5 - (filtered-" ) 18 17 0.0041 0.006 5.4

Sediment (0-10 cm) 239, Dry- Ignition Location Depth 9C>Sr 13<7Cs 240pu 241Am matter loss Org.C cm Bq kg"1 dry wt % % %

1. Tamraio c.0-5 0.43 9.1 0.42 0.21 58 .1 2.2 0.76 2. Lovusa 0-5 2.22 112 5.15 1.39 12 .7 _ 5.6 5-10 2.73 97 5.21 1.25 17 .9 16 .4 5.2

3. Helsinki 0-6 0.15 5.6 0.16 0.07 55 .3 2.3 4.3 4. Hanko-Inkoo 0-5 0.94 98 3.23 _ 19 .4 10.6 3.3 5-10 0.95 56 2.53 - 26 .6 8.1 2.4 5. Seili 0-5 0.80 72 1.69 0.47 19 .0 8. 5 2.2 5-10 0.75 43 1.06 0.37 42 .3 7.0 1 .6 6. Eros-1 c.0-5 0.21 14 0.72 0.13 65.3 1.5 0.54 7. Olkiluoto 0-5 2.1 81 .9 3.44 0.82 17. 4 15,.4 5. 1 5-10 2.3 80.5 4.66 1.46 31. 9 13,.7 4.8 8. Vaasa 0-5 1.8 89 5.1 1.26 23. 4 11,.3 3.1 5-10 2.3 62 6.7 1.50 33. 3 10..2 3.0 a fresh wt/dry wt 1.9 - 2.9, mean 2.4 surface water sample 90 137 239 240 241 Table III. Sr, Cs, ' pu an

Mytilus edulis Location Date 90Sr 137Cs 239,240pu 241n ^ Bq kg fresh wta (dry wt)

1. Olkiluoto A 09.08.82 5.1 (20) .1<30 (<0.5) 0.010 (0.040) 0.0051 (0.020) OlkiluotoB 09.08.82 5.1 (20) .1<30 (<0.5) 0.0046 (0.018) 0.0026 (0.010) 2. Olkiluoto, Puskakari 12.08.82 6.1 (240 < ) .13 (<0.5) 0.0067 (0.026) 0.0056 (0.022) shell 23 (28) <0.13 (<0.15) -b flesh 0.075 (2.09) - - 3. Houtskari, Fiskö 29.07.82 5.3 (210 ) .18 (0.73) 0.0034 (0.014) 0.0039 (0.016) shell 21 (25) <0.13 (<0.16) 0.033 (0.038) flesh 0.21 (5.9) 0.071 (1.95) 0.0025 (0.070) 4. Tvärminne, Langskär 03.08.82 5.7 (21) .1<30 (<0.5) 0.012 (0.043) 0.0026 (0.0096)

Mean + 1 S. D. whole organism0 < 4 5.50. + .10.0+ 4 2 0.007 0.003+ 3 0.0040 + 0.0014 (21 + 2) (<0.55 + 0.10) (0.028 + 0.013) (0.016 + 0.006) shell 22 + 1 <0 .1+ 3 0.033 (26 -1- 2) (<0 .16 + 0.01) (0.038) flesh 0.21 0.07 0.00+ 3 3 0.0025 (5.9) (2.02 + 0.10) (0.07)

watea Se r (unfiltered) 239 ' Org.Part, Location Date 90Sr 137Cs 240Pu 241Am Salinity carbon mat. 3 Bq m~ 0/OQ rag !-l mg 1~1

1. Olkiluoto 2 15.09.82 24 16 0.005 0.0008 6.2 0.78 Olkiluoto 2 03.08.83 23 13 0.015 0.0027 6.2 2. Olkiluoto, Puskakari 12.08.82 24 14 6.0 - 3. Houtskari, Fiskö 29.07.828 3. 24 6 6. 17 0.002 - 6 1.9

4. Tvärminne, Langskär 23.08.82 25 14 2 0.0034. 9 0.0013 6. 2 1.1 09.06.83 19 13 - - 6.0 -

a fresh weight/ dry weight 3.7 - 4.1, mean 3.9 t analyseno b d cone n wate.i q draB r ~ basis.

Fucus vesiculosus Concentration factor, P fres C dryF (C h ) Location 90 239,240 241 Sr "7Cs pu Am

1 . Ulkotammio 160 (960) 110 (660) 6100 (34000) _a _ . 2 Haapasaari 150 (870) 120 (730) - - 3. Kaunissaari 140 (830) 100 (610) - - . 4 Loviisa area 180 (1100) 180 (1100) 3900 (23000) 3600 (20000) 5. Pellinki 160 (960) 130 (730) - - 6. Tvarminne 160 (920) 87 (510) 3500 (19000) 1700 (9200) . Jurm7 o 120 (720) 92 (540) - - 8. Seili 130 (740) 160 (920) - - 9. Houtskari 110 (670) 110 (650) 18000 (100000) - . Olkiluot10 o area 140 (790) 85 (500) 3600 (20000) 7400 (44000) 11. Norrskär 110 (650) 68 (400) - -

Mea 1 S.Dn+ . 140 + 23 3 3 + 0 11 700 0+ 620 0 420 0+ 290 0 (840 +140) (670 + 200) (39000 + 35000) (19000 + 14000)

Macoma baltica

Concentration factor , CF fresh (CF dry) Location 90Sr 137Cs 239,240pu 241An,

1. Tamraio 670 (1600) <24 (<60) 3200 (8100) _ _ a 2. Loviisa 790 (2200) 48 (110) 0 (250094 ) 1100 (2900) , (filtered - -" ) 790 (2200) 34 (80) 5300 (14000) 27000 (73000) 3. Helsinki 600 (1400) 29 (79) 3500 (8500) 7500 (18000) 4. Hanko 380 (800) 170 (360) 18000 (38000) 7400 (16000) 12000 (25000) 19000 (41000) 5. Seili 440 (1300) 39 (110) 1600 (4800) 1000 (3300) 6. Eros-1 - - 4900 (9500) 2700 (5100) 7. Olkiluoto 0 (130048 ) 37 (100) 2000 (5400) 1200 (3200) - (filtered-" ) 730 (1900) 40 (110) 6700 (18000) 1200 (3200) . 8 Vaasa, Bergöfjärden 790 (1900) 31 (77) 5700 (15000) 6300 (16000) -"- (filtered) 830 (2100) 24 (59) 6100 (16000) 3200 (7800)

Mean + S.D. 0 17 + 0 65 5 4 48+ 580 0+ 490 0 7600 + 8700 (170 4700+ ) (110 + 89) (1400 100000+ ) (11000 + 21700)

Mytilus edulis Concentration facto rF fres C ,F dry (C h ) Location 90Sr 137Cs 239,240pu 241Am

1. Olkiluoto A 210 (833) <8.1 (<21) 1000 (4000) 6400 (25000) 2. Olkiluoto B 220 (870) <8.1 (<21) 0 46 (1800) 3300 (13000) 3. Olkiluoto, Puskakari <9.3 (<36) 670 (2600) 7000 (28000) 0 (120096 ) shell <9.3 (<11) flesh 5.4 (150) . 4 Houtskari, Fiskö 220 (880) 10.6 (43) 1300 (5400) shell 0 (100088 ) <7.6 (<9.4) 13000 (15000) flesh 8 (2508. ) 4.2 (115) 960 (27000) : : 5. Tvärminne, Langskär 300 (1100) <9.6 (<37) 3100 (11000) 2200 (ÙÛOO)

Mean + 1 S.D. whole 240 + 41 <9.1 + 1.1 1300 + 1000 470 2300+ 0 (920 + 120) (<32 + 10) (5000 + 3700) (19000 + 9500) shell9 5 b+ 0 88 2 1. <8. + 4 13000 (1100 + 88) (<7.6 + 4.1) (15000) flesh 8.8 (250) 4.8 + 0.8 960 (130 + 25) (27000)

a not analysed b the mean ratio of shell/fresh (dry weight) was 8,7+0.4 (1 S.D.) 76 :onc.in organism, Bq kg •* fresh wt two Finnish nuclear power station area d betweean s n Tabl . ConcentratioV e n ratios (CR=- :onc.in sédiment, Bq kg •*• fresh wt the south and west coast /I,5,67. The concentration between Macoma baltica and surface sedimeat. factors of 9°Sr and 137Cs calculated from the 1975-80 sample / wer /H sn gooi e d agreement wit e presenth h t Concentration ratio R fresC , h 239 2 results. The present CF values of > ^°pu were, Location 9 137Cs 239,240pu 241Am °Sr however o thret o etw , times higher thae earlieth n r 1. Tammio 72 <0.038 0.079 0.083 results. o lowet Thie du rs contente seemb o t s s 2. Loviisa 44 0.028 0.020 0.058 3. Helsinki 180 0.12 0.52 0.38 of plutoniu a watese n 1982-83i n mi r . 4. Hanko 43 0.11 0.11 - The concentration factors given for Fucus vesicu- 5. Seili 47 0.030 0.029 0.067 6. Eros-1 - - 0.21 0.31 y Aarkro e Balti. b losu_sth /1Öal a n t i Se _ce g / were 7. Olkiluoto 20 0.026 0.020 0.024 r 69137fo 0d 700 Cr 239an sfo value0 F 'C 240 e PusTh . 8. Vaasa 0.051 26 0.020 0.015 of 137Cs are in good agreement with our value 670, r valubu 239>240ou r t fo e Pu, 3900 clearls i 0 y higher thae Danisth n h value.

The concentration factors of 7Q QSr for the intact DISCUSSION Hacoma baltiea mussel increased when moving towards the inner parts of the gulfs showing the influence According to the results of this study the of rive re accumulation wateth n o rF valueC e Th s. 9 137239 240 1 a ? n ?u Q ?3 1-37 accumulatiof o °Srn , d Can 's pn Fucu± u s of l;MCs, "^'""Pu and ^ 'Am were contradictory, vesieulosu se differenb see o mt n differeni t a se t however. areas (Table IV). The areal differences in concentration When using the lower 9°Sr and 239,240 Q 0 137 pu contents factors of Sr and Cs were obviously due to of the filtered sea water in the CF calculations, the influence of fresh river water in the area. the CF values were naturally slightly higher. This QQ The highest CF values for * Sr were found in inner mus e takeb t n into account when usin e concentratioth g n parts of the Gulf of Finland and Gulf of Bothnia, factors for model or burden calculations. except at Norrskär, where the growth rate of Fucus The qualit f bottoo y m sediment, e whicth s i h is very slow /6/. For 137Cs, 239,240 241 pu gnd Am habitat of Hacoma, seemed to have no clear influence e concentratioth n factors were more contradictory. e accumulatiooth n e radionuclidesth f o n concentrae Th . - ThF valueC e f o Fucus d soman s e hydrographical tions in mussels living on hard or soft bottoms factors were examined for possible correlations, were approximately the same (Table II). However, but becaus e limiteth f o ed materia cleao n l r correlations e informatioth n characterizin e bottoth g s insuffimwa - were observed. correlatioy an cien r fo t n examination. The previous studies by the Institute of Radiation e wholeOth ne radionuclidth , e levels were Protection showed areal difference e concentrationth n i s s so low that no areal differences in CF values could 9 13T e th of °Sr, CS and between e foundb . The CF values obtained in this study for QO Sr The organisms examine n thii d s study livt a e s wer C n gooi ane dd agreement wit e 1977-8th h 0 low trophic levels. They may have an impact on values /4/presene Th . t concentration factorr fo s e radiatioth n e burdepopulatioth f o n n onl s linka y s ^' ' Pu were, however, some five times higher of food chains: water (sediment - organis) m- fis h e loweth duo rt e plutonium content a waterse f o s. - man. The concentrations, however, are too low When calculatin e concentratioth g n factors to be of any practical significance. for the Hvtilus edulis mussel only concentrations of unfiltered sea water were used. No local differences ACKNOWLEDGEMENT ' in the CF values could be established, which may be due to the low activity concentrations and the The authors wish to express their thanks to small size of the material. Kari Sinkk d Jaakkan o o Ojal r carryine fo ath t ou g The intact Mytilus was analysed and the shells gammaspectrometric analyses and. Kirsti-Liisa Sjoblom and flesh were analysed separately to compare the for her valuable comments on the manuscript. concentrations with the results of the other parts e Baltioth f c Sea e resultTh . s showed thae th t 2399 240 mai e nactivit th par f o tf d o °Sy an 'r pu REFERENCES apparently accumulated into shells, as is commonly known. Only at Houtskari where the mussels were . 1 Koivulehto d , TuomainenSaxénan M. ,. R , , K. , clearly larger than elsewher s possiblwa t i eo t e 1980. Radionuclides in aquatic environments. detecs bot C n intaci h t t musseln fleshi d an s. Studie n environmentao s l radioactivit n Finlani y d The mean ratio of shells/flesh (dry weight) 1978. Annual Report, STL-A32, Institutf o e r materiaou wan i s l 8.7±0.n Denmari d an 4 k 0.31±0.07 Radiation Protection, Helsinki. /9/, indicating a difference in mussel size. 2. Koivulehto, M., Saxén, R. and Tuomainen, K., In the 1977-80 Mytilus samples of the Olkiluoto 1980. Radionuclide n aquatii s c environments. 9 137 2 area the CF values of °Sr and Cs and 39,240pu Studies on environmental radioactivity in Finland were e valueflessimilarF th C f r Mytiluo n hi s Ou . s 1979. Annual Report, STL-A31, Institute of are in good agreement with the Danish results /10/. Radiation Protection, Helsinki. Of the different species in this study " Sr 3. Studies on environmental radioactivity in Finland seems to be accumulated best by Macoma ba11 ica . 1980. Sediments and aquatic indicators. Annual Probably, the activity is mainly enriched into the Report, STL-A38, 1982. Institute of Radiation shells from sediment, the habitat of this mussel. Protection, Helsinki. In contrast, Fucus vesieulo su s accumulates best t. Ilus, E., Koivulehto, M. and Tuomainen, K. 137Cs, Hvtilus edulis the Accumulatio f 9o °Srn , 137 239d Can 's240 pn i 90 241 u concentration factors for Sr and for Ara are bottom animal d littoraan s le coasalgath n o te rather high. f Finlando . STL-B-TUT . Institut15 O f Radiatioo e n 11 Protection, Helsinki e publishedb o T . . 78 5. Ilus, E., Ojala, J, Sjoblom, K-L. and Tuomainen, K , . 1981. Fucus vesiculosu s bioindicatoa s r f radioactivito n Finnisi y h coastal waters . Gul1 . f f Finlando . STL-B-TUT . Institut14 O f Radiatioo e n Protection, Helsinki. . 6 Ilus , OjalaE. , , SjoblomJ. , , K-L d Tuomainenan . , K., 1983. Fucus vesiculosu s bioindicatoa s r of radioactivity in Finnish coastal waters. 2. Archipelago Sea and Gulf of Bothnia. STL- B-TUTO 18. Institute of Radiation Protection, Helsinki. 7. Ilus, E., Ojala, J. , Sjoblom, K-L. and Tuomainen, K., 1983. Fucus vesiculosus as bioindicator of radioactivity in Finnish coastal waters. . 3 Completed studies. Institut f Radiatioo e n Protection, Helsinki e publishedb o T . . 8. Taipale, T.K. and Tuomainen, K. Radiochemical detemination of plutonium and amencium from seawater, sediment and biota samples. STL-B- TUTO 26. Institute of Radiation Protection, Helsinki. To be published. . 9 d FolgerToneran . L ,, D.W., 1974 n inexpensivA . e titration e determinatiomethoth r fo d f organio n c carbo n receni n t sediments. Journa f Sedimentaro l y Petrology . 249-253pp , 1 . , volNo . , 44 . 10. Aarkrog, A., Better-Jensen, L., Dahlgaard, K. , Hansen, Heinz, Lippert, J., Nielsen, S.P. and Nilsson, Karen, 1981. Environmental Radioacti- vity in Denmark in 1980. Ris«S-R-447. Risrf National Laboratory, Denmark. PAR1 T4.

LOCAL PATTERNS OF THE DISTRIBUTION OF RADIONUCLIDE RELEASES FROM THE LOVIISA NUCLEAR POWER STATION

. OJALAJ . ILUSE , , K.-L. SJÖBLOM Finnish Centre for Radiation and Nuclear Safety, Helsinki, Finland

The brown seaweed Fucus vesiculosus has generally been a bioindicatouse s a d f radionuco r 1 iden i s the aquatic environment. In Finland it was chosen for the environmental programmes carried out around e nucleath r power stations alreade 1960sth n i y, whee biologicath n d radiologicaan l l background studies were started. Since the nuclear power plant at Loviisa was o samplintw e e Th th g n i . location 1 B Fig .d an A s put into operation in 1977, small amounts of activation discharge area of the Loviisa nuclear power station, products have been detecte s wateit n i dr recipient. Consequently, it was decided in 1980 to study the spreading of gamma nuclides in the different parts of the discharge area by means of Fucus samples from e a distanccoolin th m Locatio0 t a 20 s f i g o e A n n parallei /1,2/ l wite regulath h r monitoring programme. water e locatiooutle th a distanc d t a an tB nf o e Durin e yearth g s - 1981982 3 Fucus samples were 2 km. taken monthly at two locations in the Hastholmsfja'rden The samples were taken usin e SCUBth g A diving bay and measured gammaspectrometrically. One purpose technique.The diver collected the algae one by one of these studies was to clarify the activity distribution in a net bag. Only well-developed and attached indivi- and thue exchangth s f releaseo e adionucr d 1 ides duals were chosen. between the Hastholmsfjärden bay and the outer open The fresh weigh f eaco t h sampl s determinewa e d sea area. after shaking the algae thoroughly on porous paper. Then they were preliminarily drie t a rood m temperature MATERIAL AND METHODS in the field laboratory (1-2 days). The final The location of the two sampling points A and dryin s performewa g t a 105°Cd . After weighind an g B in Hastholmsfjärden are presented in Fig. 1. Fucus grinding the samples were measured gammaspectrometri- 79 samples were taken monthly in the years 1982 - 1983. cally. The dried samples were measured with a Ge(Li)- e liquiTh TABLd . I dischargeE f 58o s CO) 60d Can o spectrometer (eff. 21 %, res. 2.05 keV) in Marinelli 110m^g froe Lovusth m a nuclear power station geometry. The volume of the Marinelli beakers was in the years 1981-1983. 0.5 1. Counting times were 1000 - 2000 minutes. The Nuclide Liquid discharges Bqa"1 results were calculated by means of a computer programme 1981 1982 developed at the Finnish Centre for Radiation and 1983

Nuclear Safety. The minimum detectable activity 8 58Co 4.6-108 8.2-10 1.6-109 58 6 110m (MDA f radionuclideo ) s Co, d °Can o Ag achieved 8 8 60Co 3.9-10 5.2-10 4.0-109 1 by these methods is about 0.5 Bq kg" for 0.2 kg 1 1 Omjig 4.5-108 6.0-108 6.2-109 y Fucudr f so sample e MDTh .A correspond1 0. o t s Bq kg~1 fresh wt. The statistical counting errors (±1 S.D.) vary betwee - 10%. 3 n ACTIVITY CONCENTRATION RESULTS a _ a H mtASURED o. • — • B MEASURED The liquid discharges of radionuclides 58,Co, >*x CALCULATED g froe A Lovusth m d a Can poweo r station i n ^ / ' ^ ,1 v ° , ' v r ~~v 1981 - 1983 are presented in Table I and in detail J/ — —/ " ^ \ V / - - Y j N in Figures 2, 3 and 4. These three nuclides were chose r closefo n r consideration ,because thee ar y V i' V > the main components of the released activity. * 1 Most releases of radionuclides take place in connection wite partiath h l refuellin d servican g e times n additionI . , some waste tanks were emptied ACTIVITY DISCHARGES at the ends of the years 1981 - 1983. The annual discharges of the three nuclides were about 10$ Bqa~1 t sombu , e temporal differences were found betwee e nuclidesth n e monthlTh . y concentrations f o activation products 58Co, 60d 110mCan o An i g Fucus durin e yearth g s 198 d 1982an e presente3ar d ) o locationB tw d t an a A 4 ( s d n i Figurean 3 , 2 s n Hastholmsfjardeni . Fig. 2. Time variation of measured and calculated c 0 The concentrations varied between 0.5-120 Bq o activitC y concentration n Fucui s s vesiculosus kg-1 for 58co, 0.5-170 Bq kg-1 for 60Co and 0.5-130 e dischargth n i o location atw B t ed arean t A sa a R o 1 Bq kg- for HOmAg all on dry weight basis. Lovusa and the weekly Co activity discharges from the Lovusa power station in years 1982-1983. ACTIVITY CONCENTRATION ACTIVITY CONCENTRATION

^_^A MEASURED A MEASURED ———————————————————————————————————————————————————————————————————————————————— * • — -B MEASURED B MEASURED / /; """ CALCULATED CALCULATED

———j-^. . ——- —————————————————————,T-» V^———————————— 7 - •-"•.-- •//•

/ "~ ' ' <3::f>~^~-Q ——"-**>. ——————° —— ——J./ '^iv*-. u_ ~°ct^>^- 'RV/^ "'^<^^-.^ v ——————— '\2J ————————

1-

ACTIVITY DISCHARGES ACTIVITY DISCHARGES

. 3 FigTim. e variatio f measureo n d calculatean d d Fig. 4. Time variation of measured and calculated Co activity concentrations in Fucus vesiculosus Ag activity concentrations in Fucus e dischargth n i o location B tw d t ea an A s vesiculosu n i o location tw B t d a san A s are t a Loviise aweekl activito th C d yan a y the discharge area at Loviisa and the weekly discharges froe Loviisth m a power station raAg activity discharges from the Loviisa n yeari s 1982-1983. power station in years 1982-1983.

81 82 The theoretical value f 58o sCo , 60d 110mCan oA g constante Th TABL . e II Etheoreticas th use n i d l calcu- 110m in Fucus were also calculated (Figs. 2, 3 and 4). These lations of 58Co, 60co and Ag calculations are based on the model used by many authors /3,4,5,6/. Accordin o thit g s mode e timeth l - radionuclide a T1/2biol. T1/2phys. T1/2eff . dependent concentration C(t) in Fucus can be expressed ke drv wt d d d kg water

58Co 10000 75 70 36 d C(t) 60Co 10000 75 1919 72 A(t)-(k )C(t) 110m dt Ag 1000 120 251 81 where a n accumulatioa s i n facto a nuclide f o r , describin e increasth g f activito e y 110m concentratio n Fucui n s compared with 60c0 and 120 d for Ag.The accumulation factors a waterse , are taken from several references as a typical mean A(t) is the concentration of a nuclide value applie o brackist d h water. a watese n i r surroundin e Fucuth g s A(t), the concentration of a nuclide in sea plant, water was calculated separately for every release k is the elimination rate of activity befor e samplinth e g tim f Fucuso e , assuming that of a nuclide, each of the releases is mixing very fast in the s i disintegratioA n constan a nuclide f o t . volume of Hästholmsfjärden (0.068 km ) . The results calculated by the mathematical equation (1) are Principally e mathematicath , l equatio) (1 n presente. 4 d n Figurei dan 3 2, s describes how the instrument of the 1st order reflects The most important observatio s i thae n th t a transient change in its environmental conditions. Some shape of the theoretical and experimental curves differences are found to determine the constants are in reasonable agreement with the time variation e dischargth d an k e , a rate compared with A(t). of releases. Although a and A(t) are describing r calculationIou n e releaseth s d activit s mixini y g e situatioth n e roughlconnectear d an y d with each o fass y t ba tha e tth A(tn i s i assume) o decreast d e other e differenceth , s between experimentad an l immediately. Thus, constan s i handle a t d without theoretical calculation t verno y e largear s . time-dependence. Tabl I I showe e e constantvalueth th s f o s a s DISCUSSION and T-]/2biol.> T1/2phys-> which were e th use n i d

theoretical calculation r nuclidefo s s 58cOj 60co There are too few results of radionuclide concentra- and 110mAg. The biological half-lives were calculated tions in Fucus in different seasons to enable calculation froe resultth m f o January-Mas y 1983w , ne whe o n n of the seasonal variation of the biological half- releases occurred. The values were 75 d for 58co, life, because the releases are so occasional at Loviisa. The currents and the mixing of water masses propert s beeha y n appeared clearle currenth n i y t n i Hastholmsfjarden hav e n seasonaeffeca th e n o t l pattern se hydrodynamigiveth y b n c model (4.2), variations of A(t) . Thus, the seasonal variations as well. t dominantno e "constantse th ar f k o . d Hencean a " , There are many factors which may influence e differenceth s between experimenta d theoreticaan l l e uptakth f radionuclideo e n Fucusi s , e.g. physicochemi- resulte explaineb y ma s d primaril e timth ey b yvariatio n cal state of the nuclides, temperature, light conditions, of A(t) caused by the hydrodynamics in Hastholmsfjarden, chemica biologicad an l l characteristica se e th f o s where the cooling water discharge has a significant water, seasonal variations in the growth of Fucus. e impacbehaviouth e n bayo th t f . o r However e maith , n factor t e Loviisa discontinues th e ar a d Experimenta d theoreticaan l l result e mainlar s y discharges and the time variation of hydrological n reasonabli e agreement with each othe o explait r n conditions in the discharge area. The mixing of the distribution of released activity in Hastholmsfjar- released activity with sea water depends markedly s evideni den t I . t thae activitth t y concentrations on seasonal time variation e hydrodynamicth n i s s in Fucus reflec e releaseth t thad e releaseth an st s of the Hastholmsf jarden bay. We need more frequent wil e mixeb l d relatively fast (1- ) 3almosd n i t data to be in control of all the factors. the whole volume of Hastholmsfjarden. This was also shown by our earlier results of sea water and REFERENCES Fucus samples. Activity concentrations in Fucus are relatively . 1 Ilus , OjalaE. , , SjoblomJ. , , K-L Tuomained an . n thed lowe decreasinan ar y, o fass g t that there K. 1983. Fucus vesiculosus as bioindicator s i onl a slighy t effec f activito t y accumulation f radioactivito n Finnisi y h coastal waters. r longefo r periods slighA . t saturation effect 1 .Gulf of Finland. Report STL-B-TUTO 14, Institute was also observable during the autumn of 1983, when f Radiatioo n Protection ,Helsinki. there were several consecutive discharges. More variables are needed in the model to describe more Ilus , OjalaE. , , SjoblomJ. , , K-Ld Tuomainenan . , accurately the concentrations in Fucus in different K. 1983. Fucus vesiculosus as bioindicator types of releases. Obviously, the model gives good f radioactivito n Finnisi y h coastal waters. result f theri s e severaar e l point-discharges /6/. . 2 Archipelag d Gul f an Bothniao f a Se o . Report The nuclear power plan t a Loviist s dischargeha a s STL-B-TUT , Institut18 O f Radiatioo e n Protection, of this type. Helsinki. The differences betwee e activitth n y concentrations in Fucus at location A and B may depend on the intensity Young, M.L. 1975. The transfer of °5zn and of sea level variations. Sea level variations cause 59pe alon a Fucug s serr s (L.atu ) Littorina water exchange between the bay and open sea and obtusata (L.) food chain. Journae Marinth f o le this increase e effectivth s e mixin dilutiod an g n Biological Association of the United Kingdom, 83 especially in the region of point B. This same 55, 583-610. 84 4. Pentreath, J. 1976. Monitoring of Radionuclides. The Food Agriculturan d e Organisation Fisheries Technical Paper . 150No , .

. 5 Nilsson , DahlgaardM. , , EdgrenH. , , HolmM. , , E., Mattsson, S., Hotter, M. 1981. Radionuclides in Fucus from Inter-Scandinavian Waters. IAEA-SM- 248/107.

. 6 Edgren , HotterM. , . 1981M , . Radionuklider i biota frân vattenomrâdet utanför Ringhals kärnkraftverk. Nordiska Sa'llskapet för Strâlskydd, 6. ordinarie mötet, Reykjavik 18.-20. juni 1981.

7. Launiainen, J., University of Helsinki, Dept.of Geophysics, personal communication. PART 4.2 the cooling water is discharged and a region of open sea off the bay, in the northern coast of the Gulf of Finland. The total number of grid points is 455. SITE-SPECIFIA C HYDRODYNAMIC MODEL The input variables for the model are: local wind con- LOVIISE TH R A FO NUCLEAR POWER PLANT AREA ditions, sea level changes in the open sea outside Hästholmsfjärde e coolinth d an gn water discharge. . JOKINEO N f dischargeo y wa w velocit e lo Th a , y spreading into Institut Marinf eo e Research e surfaceth , make a sspecia l near field modellin- ir g relevant. The dispersion part of the model is calcula- J. LAUNIAINEN ted usin e so-calleth g d Monte Carlo method n whici , h Department of Geophysics, parcels (concentration) from a source are studied, University of Helsinki when they make random steps (diffuse e advecth n i )- Helsinki, Finland tional current field. The model is numerically operational and several simulations have been made s examplesA . , Figure2 s In addition to the considerations of modelling and 3 give the current fields for two different input described in part 4.1 concerning the statistical beha- condition d Figan s 4 .show e spreadin th spare th -f o g viour of radionuclides, a numerical hydrodynamic model ticles in the latter case. s beeha n constructe e Lovilsth r fo ad nuclear power Figures 2 to 4 show a rather high sensitivity plant are o estimatt a e aquatith e c current field an d of the results to the environmental conditions, and pathways of cooling water and, to simulate transfer the results and experience gained from the simulations and dispersio f radioactivityo n y combininB . g this mae summarizeb y s followsa d : kind of information with such as considerations of Vertically integrated velocitie e semiencth n i s - sedimentation, radioactive decay, bioaccumulation, losed bay area are quite low. it should be possible to get further insight into the A rather complicated topography makes the current overall behaviou d accumulatioan r f radioactivityo n . field very sensitive to wind, which controls the This way of modelling approach, however, seems to be current e centrath y n areai sba l . the most proper for case and short term studies to Currents, especially in the sounds (c.f. exchan- find predican d e criticat th suc s a h l pathway- re f o s ge of contaminants with the open sea), are prima- leases in accidental situations. rily controlled by sea level changes outside. The hydrodynamic model for calculation of current This create a difficults f opeo y n boundarien i s fields is a one-layer (vertically integrated equations e modellinth e calibratedb o t g . of motion) time-dependent model with a grid size of Especially during calm periods witwinw lo hd velo- a calculatio d an m e mode0 Th n20 ltim. s e0 1 ste f o p 2 cities and slow sea level changes, the cooling area of 21 km (Fig. 1) covers the semienclosed bay o water brings a significant contribution to the 85 (area of 15 km with a mean depth of 7 m) into which local current pattern, too. r

3?

55

k-?^ V X /' i »- «C-49 \ „'TÄ-?-'" \ ) J-ï*ï~—*~(t2ß^ . r r~J/i«i„/i 2 ' 0'i™

'^^^4

Fig. 1. Sea area near the Lovusa Nuclear Power Plant. The broken line denote modee th s l areaI . = cooling water inlet coolin= 0 , g water out- let. Thoug a majoh e rare th s pari shallowaf o t a , * » * - . • one-layer model, however t abl no o describt e s i , e » v , , e verticath l velocity profile. This means that, I < • especiall e caseth f higo n si y h stratification . » _ ^ ~ t during summer and/or whenever the cooling water ,-.*»,.» v ,.,.*,f . totalle x verticath mi doet n i y no s l wate- co r xâ t t - - * X -, -.f ,,-,.,,,. lumn, additional considerations are necessary. . * \ Dispersio f radioactivito n y depend a loca n o s l \ X. X . » . , , turbulent diffusion coefficient (i.ee randoth . m . / » \ step velocit n thii y s model) diffusioe Th . n coef- : , /- • " ficient involves considerable inaccuracy and may be best calibrated by local case studies or tracer studies. Because of a rather short (2 h) stabilisation time of the model (local scale) it is irrelevant e modeth n l ru continuousl o t r longefo y r periods; o fint s ond ha erepresentativ e hydrometeorologi- cal conditions and try to combine them to descri- be average and long period results. It seems that this kind of investigation is most proper for short-term studies. Onl n speciai y l cases, suc s casea h f accidento s r caso s e studiess i , a continuous real data running or predicting fi- nancially relevant. These standpoint e ratheth d r an sspars e experimen- tal data existing for verification make to further studies necessary in the project.

10 cm/s

Fig. 2. Vertically integrated stationary current field generated by a southwest wind of 8 m/s and a cooling water discharg 0 m3/s5 d : an ) (0 e a sea level increase of 2 cm per hour, at the 87 open boundary below. / i •• • » f (...* . •. * l l ' • / -A. . *. . "f-lf V t i A 'i'-N'?!^; "/*"•> '••/.:•".

Fig. 3. Current field without wind action. The local current fiel s generatei de coolinth y b d g water . 4 DistributioFig. f particleo n s (concentrationn i ) discharge and a decrease of 2 cm/h in the sea the current fiel 3 within Figi d. , 12,...46 n 8 e opeleveth n t a boundarl y below. hours of an instantaneous release. RESULT RADIOLOGICAE TH F SO L BALTIC-MONITORING PROGRAMME DURINR GD E G 1975-198TH F O 3

D. WEISS . MOLDENHAWEF , R National Board for Nuclear Safety and Radiation Protection, Berlin, German Democratic Republic

Abstract

During 197 5198- 3 complex field studie contene th d n so an t ANNEX4 distributio artifice.e th f no I radionuclides H-3, Sr-9d 0an Cs-137 of the open Baltic Sea and of some GDR coastal waters GERMAN DEMOCRATIC REPUBLIC were carried out. Sample differenf so t compartmente th f so marine environment were taken. To estimate the radionuclide balancBaltie th measurementa n cSe ei riven o s rn wateo d ren transition areas between the Baltic Sea and the North Sea •were included. The distribution pattern of Sr-90 and H-3 in Balti watea cSe r reflec falloue th t t burden distribution ni the component vvatee th f r so balance n contrast.I Cs-13e ,th 7 distribution pattern are highly influenced by liquid effluen- ces fron nuclear reprocessing plant westerf so n Europe. The mean values and concentration ranges for Sr-90 and Cs-137 in biota and sediments confirm other published results. The dose calculations via ingestion of Baltic fish demonstrate that no radiological concequences recently occur.

1. Introduction

The main part of the reported investigation results during 1975 - 1983 has been obtaint during the yearly cruises with the research vessels "Alexander von Humboldt" or "Professor Albrecht Penck". Y/ith exceptio e Gul th Bothnif o ff no d an a the Gul Rig f wholfo e ath e Balti a includinSe c Kattegae gth t as well as the Skagerrak and the North Sea were covered in these cruises. The samples from coastal waters and rivers were taken within the scope of the NPP survillance programme. falloue Th t front nuclear weapons testin alss gi o recentle yth main source of H-3, Sr-90 and Cs-137 in the compartments of the Balti environmenta cSe present .A Cs-13e th t 7 contenn ti 89 the increasins Baltii a cSe g influence liquiy db d effluents 3. Results and discussion gQ from nuclear reprocessing plants of western Europe. The radio- active discharges from nuclear power plants along the Baltic 3.1. e Strontium-9th d Balti e an watee th a th f cSe rn o 0 i Sea coast are unimportant in comparison with the tv/o above Kattegat mentioned source artificaf so l radioactivit Baltie th n cyi The Sr-90 concentrations in Baltic Sea water were fitted to Sea. a Gausian distribution during the whole investigation period using the J^ Ç, -test. 2. Material and Methods The annual mean values during 1975 - 1983 did not differ Sample waterf so , sediments, commercial fish, benthic organisms significantly (Table 1). and aquatic plants have been collected in the open Baltic Sea,

in coastal rivers n areai d san . Table 1 The Sr-90 concentrations in the Doltlc Coo during 107S to 19C3 The water samples with a volume of 25 to 100 1 were passed through a filter of 0.45 /urn pore sire and acidified with HKO-, > - / 1 Year Number of Stront ium-90-conccntrat ion in Dq . m Cs-13e Th separates . 7 ) wa exchang n io 1 y • db n l (o e2m values Mean*' Extreme valuce Range triammonium-dodekamolybdato-phosphate (AMP) and either deter- n w t - x ' sx Min. Max. mined directly by

Baltic Sea Since 1979 water samples were taken also below the halocline whole 56 0 0. 19.- 9 10.5 26.7 16.2 d increasean d Cs-137 concentrations allways connected with high salinity values could be observed. In contrast to the Baltic Sea above hnlocline 29 20.2 - 1.2 10.5 26.7 16.2 Sr-90 values the Cs-137 concentrations are non-normaly distri- buted. According to the salinity the ranked Cs-137 concentra- Baltic Gea below halocline 27 3 1. 19.- 6 35.6 26.4 1O.O tion values were divided into classes and their arithmetic means were calculated (s. Table 3 for 1983). A correlation western Baltia Ge c above halocline 8 5 3. 19.- 1 10.5 2/1.5 14.0

western Baltic Sea Table 3 The Cs-137 concentrations in depor.dsr.ee on thc- belo-.v halocJine 11 3 2. 20.- 3 16.0 26.4 10.4 salir.ity in 1333

Kattegat classes of Numbe f o r Cs-137 concentration i n whole 17 5 1. 19.i 7 15.6 24.6 20. Salinity values Bq . m Kattegat Ko. K. n Mean ** Extreme Range above haloclino 10 7 1. 19.Î 4 15.6 24.6 2C. x - V s- values Kin. Max. Kattegat below halocline 7 1 3. 20.~ 1 14.3 23.3 6S. I s.01- 7.00 6 11 .1 7 ± .8 9.5 14.4 4. S II 7.01- S.00 13 15 .5 t 1.3 11.2 18.7 7.5 III 6.01-10.03 14 17.1 8 Î .1 15.3 21. S 6.5 * 3 <•) see footnote *, Table IV 10.01-12.03 9 23 .S .3 18. 1 31.4 13.3 V 12.01-15.00 5 24.5 i 9.0 16.0 33.8 17. S VI 15.01-20.00 10 35.6 Ï 4.0 28.5 44.8 16.3 VII 20.01-25.00 6 44.0 in.1 29.1 55.9 2S.8 VIII 25.01-30.00 3 59 .7 Î13 .9 55.5 66.1 10.6 IX 30.01-35.00 6 67.8 i s.1 58.1 75. 3 18.2 Owing to the Gausian distribution of the t>r-90 concentrations Balti e a loca th a n cSe li Sr-90 excludede b inpu n ca t o .ÎT significant difference Sr-9e th 0f so concentratione th n i s e .*footnotse } Tabl) t e l e e Baltiwateth f rco SeaKattegae mose th ,th t n i wels a ts a l important rivers from frod SovieFinlane an mth ) t(3 d Unio n 91 (40» mostly connected with larger lakes, can be observed. 92 analysis confirms the relationship between the Cs-137 concen- Stora Kjets OM tratiosalinite regressioe th th d d nan yan n analysis showed 6 Widdelgrun6F d Nor 010 030 113109 259 2« 271 m 281 305 301 »(till « i ( til significant regression:

0.750= r ( 1.0= 9.73)+ y 3x 1979 ': ^30- x Cs-137— , surface water —+ Cs-137, near bottom water 1980: y = 2.77 x - 5.00 (r = 0.946) —•-° salinity, surface water 1981: y = 2.09 x + 1.22 (r = 0.913) —* salinity, near bottom water 1982: y = 2.09 x - 0.01 (r = 0.915) 1983: y = 2.05 x - 0.25 (r = 0.962) 10- where x = salinity (S) in °/Oo y = Cs-137 concentration in Bq • m~^ 0J She regression functions are valid for the salinity ran^e from -100 500 300 0 70 400 0 60 500 800 •- distance in n.m. 5 °/oo . 35%o The correlation between Cs-137 concentration and the salinity Fig.-l. Cs-137-concentration and salinity from Kattegat to Gulf of Finland 1980 n als illustrateca e ob arranginy db valuee gth s accordir.o 3t Cutting lines . fro1 =m 58°N/tf° 55°N/1-1Eo t 0£ different regions of the Baltic Sea as well as by dividing the 2. from 55°N/11°E to SS'N/IS'E 3. from 55°N/18° EGO°N/25°o t E v/aterbody in water above and below the halocline (Table 4 and (the coordinates fro monitorine mth g station projectee scuttinar e th o gt lines) ?igurea 1 to 5). Figures 5 to S demonstrate this relationship by verticae meanth f so l profile differenf so areasa se t .

Table 4 The Cs-137 concentrations in ourface - and near bottom water from different parts of the Baltic Sea in 1983

'area 3c a Cs-137 concentration in 8q . m Numbef o r Surface water Numbef o r near bottom water valu'os Mean ' Gxtremc values values Mean ' Extreme values n + 1 - x t«f sx Min Max n x . s- Min Max

Kattegat 5 36.7 i 5.7 30.5 41.9 5 69 .8 - 0.4 59.7 76.3 v;OGtcrn Oaltlc Ooro 4 t ßp u a Se 23.4 Î 9.2 20.5 33.0 4 52 .6 i 24.2 30.7 65. 1 Sill

Arkona Soa 4 18.0 - 4.3 15.3 ?.1.S 4 23 .4 i 10.0 17.0 ?9.0 nornholm Oca n4 nd c ou n tr Î io 17,6 - 1.6 16.4 10.7 4 22 .2 - 10,5 16 .4 31. .4 Sea northern Gotland Goo 3 13.5 i 3.7 11.0 14.4 3 21 .7 - 8.2 18 .1 24.6 Gulf of Finland 2 9.8 - 4.4 9.5 10.2 2 18 .3 - 11.4 15 .4 17.2

soo footnote *) Tablo 1 Cutting line fro1 sm 58°OOlJ/-M°OOE to55°OOW/-l1''OOE Cutting lines 1 from 58°N/11°E to 55°N/11 °E 2 from 55° OON/118OOE to 55°OON/18°OOE 2 from55°N/11°F.to550N/18°E 3 from 55° DON/IB" OOE to 60° 18'N/25°30'E 3 from 55°N/18° 60°N/25°o Et E

e t « S J £ « 4î u t 55 KÎPR s R a •Jj S^ J5 c ^£S § ï?&$ >~ e f x ~ i * 3K^' e f S"' Stora Kjels 0(8 M 3t 3 30 5 2* 1 28 BV-1 9 25 * 528 3 21 9 10 0 6 03 6F Middelgrun 0 01 r Ho d i ï ïï i t „.u ï tï Ti T i i T i i it I » ^ 1 H 1 1 \ 1 1 \ 1 1 1 . 40- 100- w ^100- 1 £ l c X * ——" Cs - 137, surface water *"^V - i o ^ N " . \ ^ x K —+ — + C s- 137 , nearbottom water 830- er s ''4. *— — Cs- 137, surface water- c o ^** CO u o— — o Salinity, surface water X f\ -i —— h Cs- 137, near bottom water ^,^~1 T>j e. —— * Salinity, nearbottom water * 20- n \~ -A i^ 1 u a . /. _ t . \ 1 v V^ CO ^" "i\ \tf~' "** ^ "* ~" '*•_ -^---"'^" ""^-* — •— —\ ^ 40- 10- C_J 4 -s A . \ ä:£^-s-:_r^a)=^=J\ä=T;=^är^-,.ra _ _ _ » \x^ ^^H V £ •' + ''• .--A--^. ...t. - ~ 10 -^N~ " , | iXl^l--'''^""^Ot" ...^-••>~~+~.^ ""•-...... •» r 20- 0- 0- i ( 100 200 300 400 500 600 TOO 600 900 i K .———————— » — rii<;f^nrf» in n m i 0 100200300MB500600TO)Ca) Fig 2 Cs-137-concentration and salinity from Kattegatt to Gulf of Finland 1981 ——— ——«-Distancm n em Fig Cs-137-Concentratio salinitd nan y fro Kattegae m th Gule f Finlanth o f o t 198n di 3

Cutting line fro1 sm 55 N/11° 55°N/18°o Et E 0 fro2 m S50W/18° o 60°N/25°Et E (The coordinate f samplso e stations were projecte cuttine th o dt g lines) 92,5-1 25-1 e w KjclsOl Noa v r O Kattegatt l «i H i I 4 o near bottom waten S x surface water E 20- 50- Ä 74- xCs-137x— , surface water i\ + —— \ Cs -137, near bottom water o —— o Salinity, surface water a— ^Salinity, near bottom water 15- cr AL. i A ...--*-V . 555- a jf\ E30- ...••*-... "•^ - ' a AA\1 — t x 3 x x 37- 10- lk V ^- *^**. \t B_._.- >-._.__ Bornhotm-sea and 520-

o-J 0- 0 70 0 60 c0 20 0 •1050 0 O W 0 30 —————— relative distance -Dislancm s em 93 Fig 5 The Cs-137 concentration in surface- and near bottom waters of different Fi g3 Cs-137-Concentratio salinitd an n y fro Danise mth h StraitGule f hnldiith o f o st 190dn i 2 Baltic sea areas (1980 and 1981 ) Fig 63 6DR-t13(ßy5) E 0- w 94 115 Fig 8? 3 8 •Jh°g Fi - t jf -0.10- -010 -10- eDR-O'iS o. GDR-113 1-15 ä a- 125 •^uL i1 w* - iV W mBq r1 ?0 lOmBq I 20 ' 10 mBq l"1 JO 15 20 %> ) -K 20% ) > OT o- o- 10 20 10- / FigS6 E 20- TO- / 6DR-303 Figfi'f Fig85 E20- l 30 SDR-213(BY5) E 60- î ' 5 30- * -155 80 f-Ismeast) CL (t î :. 36 Salinit» y l J(%o\ . ) 50- S -IM• V x Cs-137(mBq t") x- *. + Sr-90(m8q l~i) 60- 200- I 60- 70- 300- «00 M) mBq l"1 10 20 %o WmB 10 10 20 %o

Fig 61 to66 Vertical distributio f Sr-90no Cs7 concentrationd -13 -an watee th n i sr f differeno t Balti areaa cSe s -1980 Fig 8 Vertical profiles of Sr-90 and Cs-137 -concentrations in water of different parts of the Baltic Sea in 1982

60 mBq l "i y«

%o 10

» sa[inity(%o BCS-K-15 x Cs-137(mBq 266 + Sr-90 (mBq 0 •> SalinitM y(° x Cs-137(m8q L"1! * Sr-30(mDo T1) i H 3 { Bq l1)

"?0 mB1 ql"

|______^ Bq 6 -ib 20 %o o 10 Fig 71 to? 6 Vertical distribution of Sr-90 and Cs-137-concentrations in the water of different Balti areaa cSe s 1981 Fig9 Vertical profi [es of Sr-90, Cs-137 and H-3 concentrations in water of different parts of the Baltic Ssa in 1993 n 196I meae 3th n Cs-137 concentration Skagerraî;e th n si d :an - The determination of Cs-134 (absent in global fallout) is the south-easter 66.t m"- • a d 130. nq 3e an 2B Nort li 6 a hSe mormord an ee difficult with increasing distanc d timean e accordancn i e reap^ ar m~ d £• qe,an 1581f wito h) . (5 dat y ab from the point and date of release. The sampling points in these areas are located within the nain transport path originating from Sella Field (6). Howevere ,th Nevertheless, the immigration of Cs-137 from the North Sea Cs-137 concentrations in the south-western North Sea and the t leasa intBaltis e ti th oqualitativela cSe y derivable taking English Channel are evidently lov/er. The data on the sampling into consideration that the time and the amount of salt-water stations "NS IV", "K I" and "Seine Bight" lie at 23.0 Bq • m*3, inflow int Baltie oth bassina provee cSe b n meany sdca b f o s 13.4 Bq « m~*^ and 26.9 Bq • m~"^ resp.. These stations are hydrophysical and hydrochenical parameters (salinity, water locatenorthware th n i d d passing transport path originating temperature, oxygen and hydrogensulfide content etc.). from La Hague (6). The station "NS IV" will be influenced On the other hand a relationship between the salinity and alreadfirst-mentionee th y yb d path evidentle n spit.th I f o e y the Cs-137 concentration was established. With respect to lower discharge radioactivitf so y fro Hagua mL comparison ei n this, looking at the horizontal and the vertical distribution with those from Sella Field (7) the Cs-137 concentrations in patter salinite Cs-13f th no d 7an y during 1980 1933- , higher the English Channe influencee lar d probabl liquiy yb d effluents Cs-137 concentration d salinitan s y neae valueth r n boticsi m frofuee mth l reprocessing plan Haguea L t , becaus e conpath e - westere wateth f o rn Balti wera Se ce measured durine gth rable fallout burden Cs-137 concentrations are significantly cruises in 1980 and 1983 comparing to the data in 1981 and lower in the adjacent regions North Sea with 3.7 to 7.4 Bq • 1982 highese Th . t salinity BornhoLnvaluee th n si i depth were m (6) and Biscay with 4.4 to 6.4 Bq « m~ . also measure 198n i dd 1983 0an courcef .O correspondine ,th g Y/hile the transport pathways and the velocity of transporta- Cs-137 data deviate from the salinity values at this station tio cesiuf no m isotopes originating from fuel reprocessing but the distribution pattern are similar in relation to the plant e goosar d ascertainable withi Norte regioa nth Se h p nu neighbouring stations. No appreciable changes of the salini- to the Danish Straits (6, 8) the feasibility of the determi- Cs-13e th d 7t an yconcentration s were detecte Gote th -n i d nation of the cesium movement trough the Baltic Proper is land depth during these years. Nevertheless ,clearla y con- very limited. The reasons are: formity of the vertical distribution of Cs-137 and the sali- nity was only visible in 1982 and 1983. instreae Th - salt-watef no r (containing Cs-13 Cs-134d 7an ) into the bassins of the Baltic Sea depends on the hydrophysicae Th d hydrochemicaan l l, parameter11 , 10 , (9 s meteorological conditions only because permanent currents demonstrat) 12 e that small instreaa salt-watef so r took do not exist. plac n sprinei 198f go 1983d 0an , wherea perioa s f o d Consequently, the cesium input arrives in varying time stagnation was observed from the autumn 1980 to the autumn intervalle in connection with the meteorological conditions. 1982 reaso.e th Tha comparably s nwh ti y high Cs-137 concen- tration e occurin near-bottoe sar th n i g m westere wateth f o rn - The Cs-137 background resulting from the cumulative fallout _o "> Baltic Sea in 1980 and 1983. The results of the hydrophysical- ranges from 15 Bq • m to 17 Bq • m . This range of the J chemical investigation n conformiti e sar y also wit trene hth d background concentration is evidently higher comparing to of the Cs-137 concentrations within the Bornholm bassin during 95 the North Sea. 198 1983- 0 . This connection point Cs-13a o st 7 input wite hth 95 salt-ric hBornhole Wortth watea o t hSe m p r u bassi a s na into salinity classes it can be pointed out, that the lowest weakle resulth f yo t instrea salt-watef mo d 1SS3 198n an ri .0 concentration3 H- mainle sar y combined wit relativelha y high An indication that Cs-137 was invaded with the North Sea water salinit . Tabl (s . Thiy e5) s relatio clearlt no s ni y visible up to the Gotland depth is given by the formation of the ver- at the low salinity classes. However, the correlation ana- tical distributio Cs-13f no 7 analogousl e salinitth o yt y during lysis confirms the relationship between the H-3 concentra- the lasyearso tw t . tion and the salinity and the regression analysis supplies Nevertheless, a confirmation of this hypothesis or a definite the following equation: identificatio source th near-bottoCs-13e f f o neo th n 7i m water of the Bornholm bassin and the Gotland depth is only y = -0.2285 x 4-8.6466 r = -0.51 provable by the determination of Ce-134 in these areas. In wnere contrast, the main source of Cs-137 in the western Baltic Sea 2: = salinity (S) in °/oo Arkone th (uo apt bassin unequivocals )i present a . e t. ,i y = Tritiumconcentration in the Cs-137 concentrations in this area are mainly influenced by the instream of salt-water. The freshwater run-off did not influence the Cs-137 concen- Table 5 ïbe H-3 concentrations in dependence on the tration westere th n si n Balti besida Se ce snai eth l concen- salinit 198d 3an n 198yi 2 trations (weighted mean: 4.5 Bq • m ) in rivers flowing classef so Hunber of H-3 concentration in into this area. The Cs-137 feeding by freshwater run-off from salinity values kBq • a \ ^ the GDR-territor d 198 198n an 3i 2 q resp.abous GB yi 7 7 t. Ko. °/oo n Bean'1"'' Extreme values Range *«

In contrast to the precipitation and the fresh-water the North Greifawald 1975 12 26.7 - 2.0 20.7 ... 32.9 Sea water contains smaller H-3 concentrations with a rela- Bodden 1976 10 3 22.3. 9- 17.0 ... 28.5 tivel ^ (14)m~ y• . constan Thiq B s3 valuE0 t 0 value1. t ea 1977 10 17.8 - 1.7 12.6 ... 20.0 increases up to 2.2 - 2.4 E03 Bq • m"-3 in the surface layer 1978 7 9 19.1. 7- 15. 2** 9 8 * î » • 1979 6 9 18.2. 8± 15.9 ... 22.2 of the Kattegat entrance (13, 14). The salt-water, poor in 1980 10 3 17.2. 2i 11.9 ... 23.1 H-3, invades over the Kattegat and the Danish Straits ir.to 1931 11 8 21.3. 0i 13.0 ... 34.1 th ewild Baltian e mixe lb a Se cd increasingly with surface 1982 18 1 20.1. 0i 16.3 ... 25.6 water containing highe concentrations3 rH- . Hence follows IIP? outlet 1975 12 24.9 - 1.8 20.7 ... 30.0 3 concentrationH- thae th t increasine sar g with decreasing channel 1976 9 7 23.2. 3- 20.0 ... 23.5 salinity. 1977 10 6 17.2. 4- 9. 221.. .. 5 1978 7 2 20.1. 5- 18.9 ... 22.6 1979 6 4 3. 19. - 1 14.4 ... 22.2 1980 7 19.8 - 3.8 15.2 ... 24.9 3.4 Strontium-90 and Cesiun-137 in coastal waters and rivers 1931 9 18.2 - 1.5 15.9 ... 22.0 1982 10 9 19.1. 8- 16.1 ... 24.2 3.4.1 Greifswald Bodden and outlet channel of the Greifsv;ald HP? *5See footnote ^Table 1. It was proved by Ar O-test that the values of Sr-90 concentra- tion in the Greifswald Bodden and the ÏJPP outlet channel n contrasI opee th n Cs-13e o Baltit th a 7c Se concentration s were normally distributed during the years 1975 - 1982. The are vitted to a Gausian distribution in the Greifs-.vald Bodden annual mean valueSr-9e th 0f so concentration Greifse th n si - outlee anth d t channel ?-tese .Th t (relatively insensitive waloutlee dth n Boddeti channe d diffet nan no o lrd signi- to minimal deviations from normal distribution) shows tl-at ficantly exceptin date gth 1975f a o differenceo .N s could the means of Cs-137 concentration of the Greifsv/ald Bodden als foune ob d betwee yearle nth y mean Greifse valueth f so - and the outlet channel do not differ significantly (Table 7) wald Bodden and the outlet channel. The results have been but they are lower in comparison to the Cs-137 concentrations listed in Table 6. As compared with the open Baltic Sea, in the adjacent region of the open Baltic Sea. Uore mean Sr~90 concentrations in the Greifswald Bodden and outlet conspicuou concentration7 13 s - thaSr-9r Cs nfo e 0th e sar channe onle lar y slightly lower. This result agrees wite hth higher concentrationw influencelo e th y db fresh-watern si . data discusse nexe th t Sr-9 e n chapteri dth 0. e concen . ,i - This can be clearly seen especially in the outlet channel trations reach values typically for the open Baltic Sea characterize higy db h change salinitn si dependencn yi n o e 97 alread innen yi r coastal waters. the meteorological conditions. Tabl 7 e Mean Cs-137 concentration e Greifsvîalcth n i s l Toblu 8 Sr-9 d Cs-130on 7 concentration n riveri s o flowing intBaltie th oa Se c 98 Bodden and in the outlet channel of the C-reifs- en n coastan i 198di d 198 R 2on GO l3 e voter(filtrateth f o s d water) H«IJ.U 41XLJ UU_i L-L J& • S 1 S » -"-».>

Waters Sr-90 concentration in Cs-137 concentration in Area Year Number Ce-'i37 concentration^ inSn~ « q Bq . m~3 Bq . m"3 Mean Extreme values Mean Extreme values - s * i « t ± x x Min. Max.x Min. Max.

r. Oder 5.0 4.5 5.4 4.6 1.1 6.1 Greif swald 1975 ) 5 20.3 t 6.1 13.7 ... 25.9 r. Ocker 6.8 6.6 7.0 1.7 1.4 2.2 Bodden 1976 ) Pcrn. r c 5.7 5.3 7.1 1.4 O.S i.n 1977 } 6 22.5 i 7.0 14.1 32.. .. 6 r. Rocknitz 3.7 3.3 4.1 1.5 0.9 2.1 1978 ) . Borthr c 10.4 5.8 15.0 2.5 1.3 4.2 1979 5 20.1 i 8.6 14.1 ... 28.9 Warno. r w n.a.0) n. a. n, .a (1.7) _ _ 1980 11 17.4 - 3.1 9.8 ... 24.5 rivers, weightcd 5.0 - - 4.5 - - 1981 13 4 16.1. i 6 14.2 ... 22.9 overall mean ' 1982 17 14.6 ± 1.0 10.6 ... 18.3 1983 15 16.3 i 0.7 13.9 ... 18.4 Pccne-streem 13.2 13.1 13.4 4.8 1.3 5.5 f Odeo ry Da 15.9 14.8 17. 0 4.7 3.8 6.0 Saal Bodden (10.4)b> outleP NP t 1975 ) 5 1 21.8. i 0 12. 628.. .. 1 - - (6.5) - - channel 1976 ) Zodstedt Bodden 17.3 IG. 7 17.9 9.8 9.4 10.6 3srth Bodden (10.5) (14.5) 1977 ) 6 4 17.1. 3t 15. 513.. .. 9 - - - - 1978 ) Crobow Bodden 15.3 14.0 IS. 5 13.7 12.6 14.8 1979 6 3 17.5. i 3 8.1 ... 21.8 coastal water? 1980 8 2 14.3. - 6 10.7 ... 22.7 overall mean lfi.0 13.1 17.9 7.8 1.3 14.8 1981 9 16.3 * 1.2 14-.1 ... 23.7 1982 10 6 15.1. ~ 2 11.0 ... 13.7 s) n. a, = not analyze) b d (...) = c-ingle value c) weighted wit he annuath l amoun{ o t 1983 12 14.8 ± 2.2 8. 018.. .. 6

ficantly lower in comparison with the data of the open footnote 1. Baltic Sea. The Sr-90 concentrations in the mouth region of the rivers as well as in the inner coastal waters reach the data typically in the Baltic Proper. In contrast, the Cs-137 concentrations were rauch smalle thesn ri e regions 3.4.2 Darß-Bodden chai riverd nan s comparin concentratione th o gt adjacene th n si t regionf so ïhe results of the Sr-90 and Cs-137 measurements fron the Baltic Sea (s. Pig. 10). In the Dar£-r.oaden-chain the coastal waters and rivers obtained in 1982 and 1983 were Cs-137 concentrations increase froSaae mth l Bodden (the listed in Table 8. These data are referring to filtrated innermost Bodden) to the Barth Bodden. The Cs-137 concentra- water (0.45 /urn pore-size). It can be illustrated, that the Bare tionth t Graboe n sBoddei th d w an nBodde n reach values Sr-9 Cs-13d 0an 7 concentration riven si r wate signie rar - characteristicall °/o6 °/c7 e o oot th salinitr fo y y level Darß- Bodden chain river 3.5 Radionuclide and stable element concentrations in ^ 20-1 7777\ Sr-90 commercial fiswater/fisd han h concentration factors v 1 1 Cs-137 r 7- T Measurements on radionuclides and some stable elements in CO ;/ ^ / / e / /, /, / commerciacoastaR GD f o l d waterBaltile an fisth a f sSe cho .£ -15- X /, / 7 y c o ^ / y ', have been performe obtaio t d n site-specific water/fish con- o y y / y v\ y •£> y / / y y centration factors and to estimate the radiation exposure w y / / y y along the water-fish-man pathway. |10- ^ / ^ ^ ^ c y / / y y y / / y y The results of radionuclide and stable element analyses on y y y y 7 \ 5- /. ^ ^ ^ 7 - fish flesh from different fish specie e listesar Tabln i d 9 e i__ y / y y / y 1 1 $ and 10. The concentrations of calcium in fish flesh varied f/j / / y y / j 0 M 1 /, ^ / /; / ~| /, from 260 to 1500 mg • kg" fresh weight and of strontium \1 _/_ 1 r.Recknilz Ssal- Bodstedt Earth Grabow r.Peene r.Pcene fccnc-slream 6rafsivr!d Bodden Bodden Bodden Bodden at Stotpe 31 AnkUim at Bodden rvar from 0.34 to 5.5 mg • kg fresh weight. These wide concen- tlie mOiithof ftcne -sliv.nn tration ranges shoulo be caused by the use of household cleaning methods unsuited for an exact fractionating. The Fig.-70 Sr-90 and Cs-137 concentrations in the Darß-Bodden chain and the river Peene in -ISS?and 1933 (filtrated water ' highest calcium concentrations are always combined with the

Baltie ofth c Sea e Sr-9.Th 0 concentration rangee sar d from 3 Table 9 Radionuclid d stablan e e element concentration n fisi s h flesf o h whole 18.m"-th o • t Darße n q i 2 5 B th are m" - f ao • 14. q B 0 fresh-water fish Bodden-chain. Species element or radionuclide . kg"1 f.w.) (B kg"• q 1 f.«.) determinatioe th r Po Sr-9e th Cs-13d 0an f no 7 concentrations K Ça Sr Fe Mn Zn Cu Cp Sr-904'' Cs-137 fixed at particles the filter sludges of all samples were- Roach 320ot 4.lt 7.0t 0.28t 4.9t 0.35t 0.023t <0.015- 1.73t (Rutilus 47O 220 1.2 1.4 0.04 0.4 0.09 0.000 0.40 0.32 analyze mixea s a dd sample resultine .Th g Sr-90 concentration rutilus) is 1.0 3-03 Bq « g~' particulate matter or 0.05 Bq • m~3 and Breom 3140Î 3.lt 6.7Î 3.9Î 0.3lt 0.014t

herring 3690 i 600 - O,75± 11. G- 0.45Î 6 .6Î O.G5Î 0 .020- <0 .015- 3.74Î occuring in such cases, when the concentrations of calcium (Clupea 330 32O 0.19 2.5 0.09 2 .4 0.14 0.011 0 ,OGli 0.97 harengus) and stable strontium are also high. The Cs-137 concentrations show a clear relationship to the trophic level of the fish Cod 3GGot 570Î 0.79Ï 2.9Î O.34Î 5 .2Î 0.17- O.043Î <0 .015- 3.02Î (Gadus morrhua) 430 460 O.41 0.7 0 .05 1.3 0.03 0 .021 O .020 0.70 species, i. e. the highest concentrations are occuring in *+) Sprat (3470) (1240) (0.86)(11.2) (1.3) 0.2) (0.47) (0 .028) n.d. 2.89Î piscivorous fish Sr-9e .Th Cs-13d 0an 7 concentrationn si (Sprattus O.44 spra ustt ) fieh flesh varied from < 0.015 Bq • kg"1 to 0.4 Bq • kg"1 ,-1 Flatfish 3480Î sooi l.lî 6.4Î0 .32Î 7 .li (0.32) 0,O44i 40 .015- 1.90Î fresh weight and from 0.6 to 7.7 Bq • kg' fresh 7/eight (Pleur once t es 140 4O O.O4 2.1 O.007 0 .2 0 .01O O.OG7 0.35 platessa; respectively. Pleuronectes flesus) Likdifferencee th e n elemensi d radionuclidan t e concen- . foot-nots ? + e ^Tablo9 trations in fish the water/fish concentration factors (C?), foot-note^Tafal. **s J e9 defined as the quotient of the equilibrium concentrations in fish and water, are wide spreaded both in fresh-water highest strontium concentration theio t e r sdu chemica l simi- and marine environments. Due to this high variability of up- larity. Both elements are so called osteotrophic elements and values site-specific factor necessare sar predictinr yfo e gth therefore the highest concentrations appear mainly in fish radiation exposure resulting from liquid discharges of NPP's species containing loose fish-bones in flesh. alon water-fish-mae gth n pathway result e watere .Th th f /so e concentrationTh e otheth rf so investigated elements differ fish concentration factors for Mn, Fe, Co, Zn, Sr and Cs from only slightly within the same species, excepting cobalt. commercial fish Greifswale livinth n i g d Bodden have been These elements having special physiological importance ear compiled in Table 11. Due to the peculiarities (especielly in homoeostatically regulated. Greater interspecific concentra- ionic concentrations thif )o s brackish v/ate determinee th r d tion differences could be observed for iron and manganese. CF-values deviate in many cases from literature data /~15, The highest iron concentrations were foun non-piscivoroun di s 16, 17, 18, 19_7 both for fresh-water fish and marine fish. highese th fis d than manganese concentration marinn si e fish. The resulting CP-values for Pe, Co, Sr, Sr-90 and Cs-137 lie The iro manganesd nan e concentrations varieo dt fro0 m2. between literature data from fresh-water and marine water en- g k • g k g fresm • 3 g 15.hm 1. 8weigh o t frod 1 an tm0. vironments CPy^-valuee .Th fresh-watef so rGreifse fisth n hi - fresh weight respectively. The zinc and copper concentrations wald Bodden are in accordance with results of typical fresh- were approximately constan ranged an t 10.o d• t frog 44 m m2. CFj^-valuee waterth t sbu marinf so e fise lowehar r than 1 kg" fresh weight and from 0.14 to 0.85 mg • kg" fresh weight thos sea-waterf o e Z -valueCP e lov/ee .Th sar r than literature respectively e cobal.Th t concentrations varie4 7 d o fro"t m3 data bot fresh-waten hi marind ran e water environments g k /u fres• g h weight having greater intraspecific diffe- 18, 19_7. n comparisoI n wit CP-valuee hth s obtained froGrabov:e mth - e water/fisTh TaJl 1 h1 e concentration factors (fish flesh end «hole fish) of comnercial fish from the Bodden/Barth Bodden with similar trace-metal concentrations Greifswald Sodden watern i onlr o yo ,n sligh t differences coul observede b d . Element Comparing-the CF-values of marine fish living in the Greifs- Species Part Mn Fe Co Zn Sra Csb v/ald Bodden 7,'i'c e valueth h s fro westere th m n Baltic Sea, -ehe Perch , flesh 25 185 75 95 l.B 230 water/fish concentration factors for lin, Fe and Zn are lower whole 360 495 90 325 50 170 in the Greifswald Bodden and higher for Co and Cs-137. 'The Pike- flesh 15 160 60 105 0.7 C.SO diffet Sr-9d CP-valueno an n thes o r i r 0d bio-copes o S tw er sfo . perch , whole 215 425 S5 365 10 270 e CP-valueTh analyzee th f so d isotopes excepting Cs-13e 7ar Pike, flesh 20 140 45 150 1.0 210 whole 255 420 60 645 25 170 lowe fisn ri h flesh tha wholn ni eTabl. e ) fis se 1 1 eh( Roach, flesi 25 270 90 125 4.4 90 Including results of water/fish concentration factors from whole 165 610 110 655 60 S5 fresh-water fie somf ho e-cerriR riverGO e -d laketh san f so Brean , flesi 25 240 50 SO 2.5 70 tory published earlier /~20_7 inversn ,a e correlation betv/een whole 275 600 60 350 60 55 Eel, flesh BO 155 65 110 0.9 130 potassium concentratio waten ni d CFcg^n clearle ran b n ca yy whole 200 1000 95 530 30 100

seen. Flounder, f lesn 25 190 140 ISO 1.0 95

resulte Th s also demonstratce_i3 thae 7 tth value freshf o s - whole 320 650 150 510 35 85 s

water fish differ, dependinCp g on their trophic level. The Herring , flesT 35 430 60 160 O.S 250 whole 530 740 65 340 4.5 190 CP,., .„ value,e expresse, b n sca n dependenci d e potassiuth n o e m c OS—1jI Cod, flesh 110 660 40 850 1.0 170 concentration in water and the trophic level of fish as r see whole 720 1460 55 1370 6.0 150 Pig. 11_7: Sprac , tt flesh 350 2550 25 1600 0.9 140 whole 710 5500 30 3350 2.5 105 a) piscivorous fish: Mean CF-values v-0.62 fresh-water C? 407 =-0.99r 5 fish flesh 20 200 60 110 1.9 130 Cs-13= 7° whole 260 510 BO 470 30 145 •where Marine fish. flesh 230 1600 30 1250 0.9 1C5 whole 720 3500 40 2350 5.0 130 CP water/fise th - h concentration Cs-137 a - Strontium-90 and stable strontium; factor b - Cesium-137 - CF-value c s frowestere th m n Baltia Se c (K) potassiue th - m concentration in wate) ~ 1 r • (ing

- correlation coefficient The CP-values for some fish species, for example eel, lie between the values of piscivorous and non-piscivorous fish b) non-piscivorous fish: overale th d lan P meaC f no Cs- values will be used: CP 2135 r = -0.994 0 64 101 Cs-137 CP,Cs-137 3070 (K)" ' r = -0.996 « non-piscivorous freshwater fish 102 - sessil elife stagth e n cycli e e A piscivorous freshwater fish - special nutrition x mean of fresh water fish The disadvantage is the fact that the shell comoosition depends on the salinity and that the body size and the vitality of any marine mussels are reduced with decreasing salinity. For regions of similar salinity, however, thee welar y l suite s bioindicaa d - P--0995 tors. The results listed in Table 12 confirm this statement at T--0996 102: least for Sr-90 which, due to its chemical similarity to cal- cium, is mainly tne more accumulated in Tiussel shells, tne less the Ca-content of water. In tnis case Sr is incorporated

Taole 12 water/nussel concentration factors (CF )

III-101. I I L l t l t 10I I 2„ I | I -Potassium concentration[mg-f1] Location CF„ n FI 1 Cs-13G1 7 concentration facto dependencn ri potassiun eo m concentration in water and trophic level of fish Sr-90 Cs-137 Numoer Mean Range Nunber Mean Range

mussel Greifswald flesh Bodden 3; 5 17 5...37 4 54 14. ..90 valuef so 16 The higher ^Qs_-t^7 "t* herring Greifse livintn n gi - sout n-wes tern walder Bodden in comparison to those of the western Baltic Sea Baltia Se c coast c) 12 18 6...39 14 21 7. ..53 is also caused by differences in the potassium concentration of water. Due to the shorttera immigration of some marine mussel Greifswald species (cod, sprat; into the Greifswald Bodden, the CF-vaiues shell Booden 9 990 640..1310 89..2517 06 0 from the western Baltic Sea were taken in account /"see Table 11 south-western Baltic Sea 0 120...9044 9 1 01 1 coast 94 47..220

6 Sr-9 3. a Cs-13an 0 7 concentration d concentratioan s n factors n benthio c organisms (mussels) ) a concentration factor (CF„) e samplinTh f oenthio g c organisms orimarily serve o fint t s ou d suitaole bioindicator r radionuclidefo s s occurin n liquii g d J nea£& r bottom water in Bq • kg effluents on nuclear oower plants. It therefore comprises al- most exclusively common mussel species which s possibla , - in e *>) including the mussel species Mytilus edulis, Cardium dicator organisms, meet the following conditions: edulo; Mya arenaria; Macoma baltica, - high copulation density

' Including 'and cyprina islsndica - widerspread occurrence c Tabl3 1 e Sr-90 and Cs-137 concentrations in seaweed and aquatic plants inte shellth o r instancsFo instea . e concent-atioCa th e f o d n (Greifswald Bodden, Grobow Bodden, offshore region) factors for Sr-90 in shells of marine mussels in tre Grens-

wald Bodden lie about twice as high as in the same soecies Species/ fresh weight/ Radionuclide concentration inBq • kg"1 f.w. group dry weight Sr-9O fro~i the offshore region of the Baltic Sea. However, no di-fe- ratio Cs-137 Number Mean Range Nurtiber Mean Range e Sr-9rerceth 0f o saccumulatio e detecteb n ca nn flesi d f o h russels originated from both biotooes. For Cs-137, accumulation both in flesh and shells of nussels Zostera marina 9.9 4 0,4110,19 O. 18. ..0.64 2 O.44...1.24 Myriophyllum, 6.4 11 0.39ÏQ.24 0.1O...0.75 13 0 r .09 ir the GreiTS^ald Bodden is aoout twice as high as in tnose Potanogcton 7.1 .84io,48 O.? i..,l

from the offshore region. Here, similar relationshio occu- Chloroohy^a

oetween the potassium content of surrounding water and the Chara , 6.6 Cs-137 content in the nussels as exhibited between Ca- ard Chactomorphy 8.3 9 0.82Î0.79 0,15. ..2. 35 8 0.56Î0.1G 0.28...0 ,78 Enterono rpha, 10.2 Sr-90 content. 10 0.16ÎO.OG 0.1?0 . ..0.3 2 1 2 .51Î0.18 O.??..,0 ,U2 Cladoohora 9.5 e meaTh n value f Sr-9o so Cs-13 an 0 7 concentration n shelli s s " freskg - f Mytiluh o q S weigh 5 d 1 s an t eduli a e li s OelesGeria , 6.7 Polys i_phonxa 5 0.?*-0.07 0.170 . ..0.3 6 3 .96^0,13 0.70...1,08 3.2 3q • kg fresh weight resoectively. Tne corresoondzng 7.5 Phocoohyta concentrations in flesh lie at 0.3 3q • I5 1,41,..2.17 tions in other mussel soecies are s^irilar to these in Mytilus. Ljniriiria sarchanna /.4 The relatively high Cs-137 concentrations in shells are pro- bably caused by fixation on the shell surface because the mussels were not cleaned before fractionating. corditiors. Especially the inner coastal waters show great fluctuatiors or the salinity and also of the Sr-90 ano Cs-lC7 7 Sr-9 3. Cs-13d 0an 7 concentration concentratiod an s n tactors concentration n deoendenci s e reteorologicatn n o e l concilions. n seaweeo d aquatian d c slants Sr-9e d th Cs-13 0an s a same 7y I th nconcentrationwa e s differ The aquatic plants and seaweed included in the investigation the concert ration factors are also wide soreaded. The rean orogramn can be taxononcally classified as spermatoohytes concentration factor f water/aquatio s c olant r seaweeo s d an d (flowering olants), chloroonytes (green algae), rhodophytes their range e listear s Taoln i d. 14 e (red algae d ohaeophytean ) s (brown algae). Wherea e concentratioth s n factor r aquatifo s c olantc a^ s s resultA s show, ther e relativelar e y large both intraspe- sea.vee f marino d e origin agree well with literature data (19) cifi d intersoecifian c c concentration ranges esoeciallr fo y the CF -values for plants and algae of limnic origir lie olants and algae of linnic origin (see Table 13). obviously belo.J the values given in (19). This shoulo be cau- d probabl se e adaotioth y b yo brackis t n h water conditions. In this resoect have to oe considered the particular physio- logical differences or the species or grouos studied and the In the same way the results demonstrate that, oue to relati- 103 circumstance that the plants growing under brackish water vely snail accumulation, only few of the soecies studied are 104 Table 14 Wgter/aquatic plant r seaweeo s d concentratio actors'*f n ' (CF) - Balti a werSe c e sample y meana b "Nimisto"-corerd f o s . There- fore the vertical distribution of radionuclides could oe Species/ Concent ration factor establisheo only on tne open Sea samples. However, the measu- group Sr-30 Cs-137 rements of Sr-90 and Cs-137 in samoles from coastal waters Number Mean Range Number Mean Range allo.v preliminary assessment e concentratioth f o s n rangen i s Sge rma t ojj>hy_£a tne upper sediment layer (about 0 to 10 cm) and exhibits diffe- Zostera marina 23 10. ..35 2 52 27. ..77 rent accumulation properties of different sediment tyoes (Table 15). 13 54 17. . .126

Chloroghy_ta *-1 9 S1

Classification , 9 6.. .16 12 29 11. Nunber Mean Range Number Mean Range Rhodoghyto Silt 6 95 43. ..127 7 2340 1330. .,3160 Sandy silt 4 364 8.. 7 .5 580 350... 710 12 9...17 3B...64 Sllty sand 4 7.5 3... 10 5 300 120... 490 Phaeop_hy_ta 7 sediment inBq * kg dry weicht *>*„. L~C- Fucus vcûiculosus F. serratus near botton water in Bq * kg" Laminaria 9 70 41. ..97 82. ..132 sacchonna Concentration factor (CI- ) = CCJ aquatic plant or seaweed in Uq • kg" frch WC i qh t

£~C_7 water jnlq . kg~ Tne comoarable l

5 for the critical grouo (fisherman and their families) have

6 oeen listet in Table 16. To oredict ingestion doses via fish consumption caused by routine releases of the Greifswaid NPP, 7

8 • Taol6 1 e Elective ingestion equivalent dose rates resulting from fallout Cs-137 in fisn of the Greifsvald Bodden

Year Individual effective Collective dose equivalent dose rate (Sv . a'1) (man Sv * a~ )

2 1 Vertical disinbjio f rcdionuclideno sedimeno n o s f core Arkone oih f a bassi n -138i n 5 1S79 2.06 5E- 1.63 4£-

tion on tne type of sediment and on the samoling area can also 1930 S 2.3E- 9 1.91 E-3 be clearly seen. Soft sediments representin a long-terg m reservoir of various radionuclides due to their hihg content 1931 2.21 E-S 1.77 E-3 of organic matter or clay minerals respectively. With in- creasing conten n matrii t x materials (sand, gravel- uo e th ) take capacity of the sediment decreases consideraoly. 1932 2.02 E-5 1.62 E-3

1933 1.37 E-S 1.50 E-3 3.9 Ingestion equivalent doses resulting from consumption of fish from the Greifswaid Bodden * ^- critica parsonl0 grou80 f o ps The Greifswaid Bodden is the cooling water reservoir of the Greifs'.-.'ald NPP. The investigations of fish and water in the a simple determinatio th modex r bo e fo l f radior.uclido n e Greifswaid Bodden indicate no differences in radionuclide concentration in the Greifswaid Bodden will be used. This concentrations in comparison with the other biotops. Never- model was describe n i d~16 . theless due to the high fishing yield in this coastal water, the water-fish-man path/va e criticar liquith fo s y i yd wa l w ,1 (3.1) 10d model5an P effluentsKP describine th f o s g this pathwae ar y V ( + F) where 106 Taol 7 1 eCalculate d radionuclide concentrationr ; n i s 1 the input of radioactivity (3q a' ) Greifswald Bodden annuafollowinq G3 0 l 1 ga V = the volume of the Greifswald Sodden (m ) K?P discharge ^ = the radioactive oecay constant (c'~ ) for a YEAR given radionuclid. i e 1979 1980 1981 19C2 r^clide Cw.l Cw,i The value F (d" ) describes the loss of activity by water (Sq . I'1) (3q . I"1} (Bq . I'1} 1 ~- ' exchange between the Greifswald Boaden and the adjacent re- gion of the Baltic Sea and is defined as: C.-- 51 6.7 E-OE 4.2 E-06 S.2 E-OS ;:.-.- 54 5.6 E-05 7.8 E-05 3.5 E-05 4.5 E-33 (3.2) Fc- 59 8 E-O2. S 2.0 E-OS - _ Co- 53 E-03 3. 5 E-07 2. £-07 54. 5 4.5 =-05 where Co- 6O 4.3 £-05 £-02 2. £-03 53. 5 3.C S-05 So- 75 - - 2.3 ;-cs rat f outpuo e t from Greifswald Bodde~ (m n -1 2r- 95 2.9 E-OS - 8.9 E-07 The computed value of F is 0.032 d Us- 25 1.7 E-05 7.0 E-OS 1.0 E-05 .-,„-103 2.5 E-05 - - The interactions with sediments will not be considered because A;-llO.-3 E-01 3. 5 4.9 E-05 1.3 £-04 5.1 E-05 the redistribution e processeGreifsival th t know no r fo e n ar s d e^-124 - - 3.5 E-05 Sodden e dat Th .f comoute o a d radionuclide concentratioe th n i n Cs-134 3.0 E-05 1.4 E-05 2.0 E-05 3.1 E-05 3.7 E-05 Greifswaid Bodden resulting from an annual discharge of 10 G3q Cs-137 E-03 2. 5 2.6 E-05 3.6 E-05 Sa-140 - E-04 1. 6 - have been compile n Tabli d. 17 e Ce-141 5.4 E-07 2.1 E-06 - Co-144 S.3 E-OS 5.8 E-06 e.3 E-07 e calculatioTh e ingestioth f o n n equivalene tb dosn ca e expresse: as d q • U • F C • C = H ing,1 w,1 i ing, i (3.3)

where Due to the short effective half-life of the concerning radio- nuclides in man the resulting dose is almost fully efficient = effectiv H e ingestion equivalent oose ratf o s in the year of uptake and so the annual effective dose equi- the radionuclide i (Sv • a~ ) valent differs not or only slightly from the committed dose U = consumption rate per caoita (kg -a ) equivalent. The results of ingestion dose calculation follo-

= weighted ingestion dose constant of the win n annuaa g l q havdischargGB e 0 1 bee f o ne listen i d ing radionuclid i e(S B• v q) Table 18. e showb n nIca t that Cs-13 criticae d Cs-13th 7an e 4ar l radio- The g values from (22) were used. nuclides in the water-fish-man pathway. IS Ingestion equivalent dose-rates following s 1C 32ç "eferences annua dischargP MP l e ) (1 B30GMUS , Kiele,W. r Meeres forsch X (1952I . 5 )1

oc.- S '10 1979 1980 19S1 1SC2 ) (2 Gewässsrkundliches Oa'nrbuc DDRr de h, Abflußjahr 1965. r.u elide Hing,i Hing,i Hing,i 1 1 1 Inst Wasserwirtschaf. f . t (Ed.), Berlin (1969) (S a'• v) (Sv . a" } (Sv . a" ) (Sv •"a'1)

) (3 Studie n environmentao s l radioactivit n Finlani y d 1931. ., Cr- Si 2.4 E-12 1.5 E-12 .5 E-12 Ann. Rep. STL-A 40, Helsinki, Finland (1982) .v..-.- 54 7.0 E-ll 1 E-l4. 9l.5 E-ll 5»5 E-ll Fa- 59 7.5 E-ll S.4 E-ll - Co- 53 5.7 E-ll 8.1 E-ll 3.9 E-ll 7.7 £-11 (4) Radiological investigations in the Baltic Sea in 1982. Co- 60 2.0 E-10 1.6 E-10 8.8 E-ll 1.4 3-1D Radium Institute Leningrad, Se- 75 - - - 1.4 E-ll Leningrad, USSR (1963) (unpublished, in russ.) Zr- OS 5.8 E-12 - - 1.0 E-12 Kb- 95 1.5 E-10 6.3 E-ll 9.3 E-ll Ru-103 1.1 E-13 . - - ) (5 HUNT, G.O., Radioactivit Surfacn i y Coastad an e l Waters Ar;-110n 5.5 E-10 9 E-01. 98.8 E-1C 9.2 E-10 of the British Isles 1981. Sb-124 - - 1.1 E-10 Aquat. Env. Monit. Rep., MAFF Dir. Fish. Res,, Cs-134 6.9 E-09 3 E-04. 39.2 E-09 7.0 E-09 Lowes 9 (1982 t f to 6 )3 Cs-137 3.1 E-09 3.5 E-09 4.5 E-09 4.9 E-09 3Z-140 4.2 E-13 - Ce-141 7.2 E-14 - 3.1 E-14 - (6) KAUTSKY. H. et al., Dt. Hydrogr. Zschr. 33 4 (1980) Cs-144 7.7 E-12 5.8 E-13 7.7 E-13 ) (7 3ENKINS, W.O., LIVINGSTON, H.O., Radioactive Tracers in the Sea. Woods Hole Oceanogr. Inst., Woods Hole, K ! 1.1 E-OS E 09 1 1 E 08 1 .5 E-OS ing,i "ing,*8'0 - "ing.i ' - "ing.i Mass., DOE/EV/10694-3 (1980)

) (8 AARKROG , DAHLGAARD,A. Source, H. , Cs-13f o s Sr-9d 7an 0 The results indicate that the ingestion dose calculated from Danise ith n h Straits Annn .Da . Rep. 1981, e prepth o t , routine releases of the Greifswald NPP is more than two TC "Baltic Sea" of the IAEA (1982) order f magniduto s e lower compared wite dosth h e resulting from fallout Cs-137 in fish of the Greifswald Bodden. ) (9 NEHRING , FRANCKED. , , Fisch.-Forsch,E. .wiss, , Schrif- tenreihe 20_ 2 (1982) 69

(10) NEHRING, D., FRANCKE, E., Fisch.-Forsch., wiss. Schrif- . - tenreihe 21 4 (1983) 45

107 108 (11) NEHRING , FRANCKED. , , Fisch.-Forsch.E. , , wiss. List of GDR-Literature sources on the field of "Radioactivity Schriftenreihe 21 4 (1983) 56 in the Baltic Sea"

(12) NEHRING, D. et al., Die ozeanologischen Bedingungen zentraler ide n n Ostse m Dahri e e 1983 n press,(i ) BRUEGMANN, L. et al,: Preliminary results on the distribution (13) FROEHLICH al.t e ,. K , Beitr . Meeresk 9 (1983.4 7 )7 of same pollutant Baltie th n ci s 1980 and 1981. ICES, Marine Env. Quality (14) UEDEKIND, C., Dt. Hydrogr. Zschr. 3_5 4 (1982) 177 Committee, C.M. 1981/E: 51

(15) VANDERPLOEG, H.A. al.t ,e , Bioaccumulation Factors ETTENHUBER ROEHNSCHd fish/watee an Th . ,E : . ,W r accumulation for Radionuclides in Fresh-Water Biota, ORNL-5002 factor- an important oarameter for de- (1975) terming the environmental caoacity of surface waters", Impact f Nucleao s r (16) Generic Model d Parameteran s Assessinr fo s e th g Releases into the Aquativ Environment (Proc. Symp. Otaniemi 1975), IAEA, Environmental Transfer of Radionuclides from Rou- tine Releases, Safety Ser. No. 57, IAEA, Vienna Vienna (19753 )47 (1982) : FRÖHLICHal t e . K , Verteilung von Tritium in der Ostsee im (17) ETTENHU3ER Isotopenpraxi, ,E. (19713 7 s 5 )7 Oahre 1980. Beitr. Meeresk 9 (1983.4 7 )7

(18) EICHKOLZ, G.G., Environmental Asoects of Nuclear WEISS, 0., ETTENHUBER, E,: Die Verteilung des Strontium-90 und Power Arbon An , r Sei. Publ. Inc. Mien (1976) Cs-13 Wasserkorpem 7i Ostser de r e 1975- 1982. Symp. IsotooNaturr de n i ,e Leipzig (19) THOMPSON, S.E., et al,, Concentration Factors of 1983. ZFI-Mitteilunge (19844 8 n 2 )40 Chemical Element n Edibli s e Aquatic Organisms, UC"?L- 50564 Rev. 1 (1972) WEISS , KUNERT,D, , MOLDENHAWER,3. ; "Th,F. e distributiof o n Strontium-90 and Cesium-137 in tne 'Jäter (20) ETTENHUSER, E., ROEHNSCH, W., "The Fish/water accu- of the Baltic Sea including the Kattegat in 1980 and 1981". Proc. of the 13th Con- mulation factor - an important oarameter for deter- ference Baltith f co e Oceanograoners, ming the environmental caoacity of surface waters", Impacts of Nuclear Releases into the Aquatic Envi- held in Helsinki, August 1982, Vol.2, ronment (Proc. Symp. Otanieni 1975), IAEA, Vienna 2 oo;ed74 . Helsinki, Finland 1982 (1975) 473 WEISS, D., MOLDENHAWER, F.. Water/fish concentration factors of commercial fish in GDR-coastal waters and ingestion dose equivalents resulting from fish consumption". Seminan o r the Environmental Transfer to Man of Radionuclides Released from Nuclear Installations. Brussels, Belgium Oct. 1983, IAEA-SS-85/4S 110 RADIOLOGICAL INVESTIGATIONS IN THE BALTIC SEA, INCLUDIN DANISE GTH H KATTEGASTRAITE TH D SAN T DURIN 198D 3 GAN 1982

H. KAUTSKY, C. WEDEKIND, H.-F. EICKE Deutsches Hydrographisches Institut, Hamburg, Federal Republic of Germany

I. Abstract

ANNEX 5 In connection with earlier investigations during GERMANY, FEDERAL REPUBLIC OF , thdurine zj eth , year1 n gi /~ 198o 198s2t 1 1975 westere regioth f no n Balti a includinSe c Danise th g h Baltie whole th regioa th Straitf Se ceo n i d 198n3 san as well as in the Danish Straits and the Kattegat, water samples were taken from different depths for the investigatio f theio n r conten differenf o t t radio nuclides. In all the samples, the salinity and the activity concentrations of Cs-137 and Sr-9O were determined. In 1983» in addition, in 41 samples from 27 stations the content of Tritium was measured and 2 sample3 n i s fro station6 1 m e contenth s f transo t - uranic nuclides.

Altogether picture e activitth ,th f o e y dis- tributio artificiaf no l radio nuclides, compared with s hardlha 1981y, changeBaltie th n ci de Seath n I . western Baltic Sea and the Baltic Proper there exists a clearly recognizable relation betwee e salinitth n y Cs-13e th d 7 an concentration; high salinitiee ar s linked with high Cs-137 activity concentrationsn I . the cas Tritiumf o e , this relationshi practicalls i p y the reverse; that means, the lower the salinity — then the higher the Tritium concentration. The content of Sr—90 is relatively independent of the salinity content. It may, almost exclusively originate from the worlwide fallout f transuraniO . c nuclides, practically only Pu-239+2^0 is detectable, from which, as a result of Parallel to the Cs-137 activity concentrations the relatively slight number of measurement values, which have again been decreased since 1980 ,decreasa e so that n totali , , this permit o clean s r distribution can als e observe b oKattegate th n i d . This corresponds pattern to be recognized. with a reduced introduction of Cs-137 in the western n totalI e activitth , y concentration Tritiuf so m Danise regioe th th f n Baltihno i Straitsa Se c . d Cs-137an , especiall n surfaci y e water, sho clearla w y The Cs-137 introduced in this manner could be reducing tendency when compared witprevioue th h s years. measured predominantly in the deep water of the western In the few bottom samples investigated from the Baltic westward Darse th sf o sfro- Sill d m ,an 198O western Baltic Sea, only Cs-137 could be detected by onward deee th - salsp Bornhol e n watei oth f o r m Basin. mean gammf so a spectrometry activits It . y concentra- 3. RESULTS tions showed strongly varying values dependent upon the type of the sediment (Table 2). e measuremen3.1Th . te salinit th dat f o a y con- activite ten th s wela ts a l y concentration f Cs-13o s 7

2. GENERAL and Sr-90 are given in Fig. 6 to 8 for 1982, and for whic, 19817 Fign ho i 3 t als 9 . o includ concene th e - As before e maith ,n quantit e artificiath f o y l tration of H-3 and Pu-239+2^0. In the following sections radio nuclides Baltie presen watee th a th f Se co rn ti the individual radio nuclide handlee ar s d separately. originates froe globath m l fallout e discharg.Th f o e such nuclides with the waste waters of the nuclear 3.1.1. Caesium-13) 15 d 7an (Fig0 1 , 7 . Owing to the temporally changing influx of North power plants present in the Baltic Sea region, however, sea water with higher Cs-137 content especiall- s y on the contrary can be viewed as being insignificant. through the Great Belt - into the western Baltic Sea, Only in the region of the western Baltic Sea, with in the region westwards of the Darss Sill, temporally the more saline Nort watea Se h r flowing througe th h strongly varying activity concentration valuef o s Danish Straits, mainldepthse th n i y, since 197- 9in Cs-137 in the deep water are to be found. Conversely, creased quantities of Cs—137 are introduced. This the region eastward of the Darss Sill, is less affected Cs-137 originates essentially frowaste th m e waters by these variations conformitn I . y with Danish investi- nucleae oth f r fuel reprocessing plant, Sellafield for Works, neaIrise th r h Sea n essentia.A e l th par f o t gations / 3_7i the first time, in 1979» a clear introductio Cs-13f no 7 wite inflowinth h g Norta Se h Cs-137 quantities released from ther s transportei e d water in the depths could be observed in the southern with marine currents throug Norte a intth he Se hth o Kattegat and in the western Baltic Sea, westwards of Kattegat e highes.Th t activity concentrations could be measure Norte th a durin n hSe i e year d th g s 1978 the Darss Sill /~1_7- and 1979. and in the deep water of the Kattegat In 1977, there were still only insignificant during the years 1979 and 1980. differences in the activity concentrations of Cs-137 (Fig. 1) measured in the surface and deep water east- Ill wards of the Darss Sill as far as the Bornholm Deep. Thenfirse th n 1980 ,i tr fo tim, deen i e p water concentrations than in the deep water, at all other Bornhole oth f m Deep higher Cs-137 activity concen- station highee th s r measurement values occuren i d tration values were detected. They arounla y d double the deep water. The highest values are to be found so high as those in the surface water. They could deee th p e souther n watei th f o r n Kattegan i d an t als e observeo b e samth e n fori d n 198i md 198 an 13 th eBothniae wateth f o r n Sea. (Fig. 1). Altogether, though, the number of measurement n 1981I activite th , y concentration valuef so values were not sufficient to draw up a sure distri- the bottoe Cs-13th n mi 7 Gotlane wateth f o rd Deep bution picturPu-e th 2 f Baltie 39+2^*o eth a n i Se 0c w abou abov3 no 1/ y t ela surface thosth f o ee water region or to be able to indicate a relationship to / 2_7; in the year 1983, they were around about 50 % the salinity. higher (Fig. 10). e activitTh y concentration e valueth f o s Conversely e activitth , y concentration values Pu-239+240 sho comparew- d with 1981- £~zjto a - surface th n i e regio e wateth n i nr eastware th f o d tally decreasing tendency. Dars s intBornhole a th osr fa Sil s ma l resp. Gotland 3.1.4. Tritium (Fig. 13 and 17) Deeps showed practicall variationo - yn in e th n i s Tritium is introduced into the sea either with dividual years (Fig. 1). However, compared with 1977, the precipitation direc r indirectlo t y ovefreshe th r - they have clearly decreased (1977 about 20 Bq/m , water flowing 5_/fro, lane 4 thar th md/ .Fo t reason, 1981 about 15 Bq/m3, and 1983 about 13 Bq/m3) that in the sea areas in which the "freshwater portion" - average meansth n annuan ,o a e l decreas abouf o e t recognizabl salinitw lo particularls e i th y- y eb y 1 Bq/m3). high, one also finds a higher Tritium content. 3.1.2. Strontium-90 (Fig. 8. 11 and 16) Thus Tritiue ,th m activity concentratioe th n i n See section 3.2.2. Baltic Sea water, outwards from the West in the region 3.1.3. Transuranic nuclides (Fig. 12 and 17) Danise oth f h Islanddirectioe th Northe n th i s f -no east, constantly increase d attainsan highese th s t During the measurements of the transuranics in northere th n valuei ne ) th par17 s f d (Figo t an 3 1 . th eBaltie wateth f co r Sea, practically only Pu-239+2^0 Bothnian Sea. Ordinarily activite ,th y concentration could be detected. Only at the northernmost station in Tritiue more ofth th e n salinmi e near—bottom water the Bay of Bothnia, in the surface water, an activity is clearly lower than in the surface water. This concentration of Am-241 was found, which lay just appears particularly clearly in the region of influx withi limite th n detectiof o s r measuremenou f o n t and outflux through the Danish Straits. The reason method (about 2 mBq/tn ). therefor is viewed as the inflow of Tritium poor and Witexceptioe th h stations3 f no whict a ,e th h saline rich deep water from the Kattegat into the surface water contained higher Pu-239+2^0 activity Balti outfloce th Sea d Tritiuf an wo , m ric d lowehan r present in the water of these regions originated saline surface water from the Baltic Sea into the almost exclusively frofalloue th m t (Fig TABL, .2a E Kattegat. I). For the measurement values given in Fig. 13 and On the other hand, in 198O, the introduction e measuremene erroth 17th »f ro r Tritiufo t m concen- of Cs-137 with the more saline water originating from o trations smaller tha kBq/m5 n betweed e an li J % 5 n th ed flowin an Nort a oven westergi e Se h th r n Baltic 12 % for concentrations greater than 5 kBq/m^ between Sea is quite clear to recognize because of the in- Thes. % 5 e 3. error d an measurementf so % 5 come ,ar - crease of the slope of the activity to salinity curve piled from the quadratic mean of Z (3 counting error •(Fig. 2b, TABLE I). (95 % statistical confidence) and the error of the Baltie wholn e 1983 th I regioa th f Se co en i , n analytical' % metho 3 f o d an extensive dependenc e activitth f o e y concentration 3.2. Relation between radio nuclide concen- uposalinite th n observes ywa d (Fig TABL, 3 ., EI) tratio salinitd nan y that means, the higher the salinity then so higher is the Cs-137 concentration For closer observation of the relation between salinity and activity concentration, the measurement This phenomenon may rest upon two different value e enteresalinity-activity-diagrame ar sth n i d . reasons. In the Southwest, saline rich water with r TritiuFo measuremene th m t point markee ar s d with higher Cs-137 content is applied to the Baltic Sea correspondine th f tho e) letterZZ - g A samplin( s g via the Danish Straits. This spreads, with general position (from d Fig17)an .3 ,1 whereb e capitath y l dilution, towards the Northeast (Fig. 3 I). On the letters mark the values in the surface water and the other hand one can recognize the influx of Cs-137 small letter snear-bottome thosth f o e r Cs—13.Fo 7 poor freshwater from the land into the Bay of Bothnia and regione Sr-90th r ,fo s Danish Strait Bornholo t s m causing a dilution of the higher Cs-137 activity Beep (circa 56° N), Gotland Deep as far as 60° N, concentration presen watea se tre therorigith n i e - Bothnian Sea (60° to 63°30' N) and the Bay of Bothnia nating from the fallout (Fig. 3 IV). The course of (northwards of 60°30' N) the data of the stations Figf tho eV . I curvee indicatesslope3 o th t f I so s , were used, and for different regions were marked with that the influence of these two effects extends to different symbols. The results of the regression the central part of the Baltic Sea (Fig. 3 II, 3 III). calculations belonging thereto are reproduced in TABLE I. In this area activity concentrations are to be found, which may practically exclusively originate from the 3.2.1. Relationship Cs-137 - salinity (Fig 2, 3,) global fallout. n 1977I activite th , y concentration Cs-23f o s 7 e surfacth d deen i an ep water eastward Darse th sf o s 3.2.2. Relationship Sr-9 salinitO- y (Fig, .k Sill showed only insignificant differences. There is TABLE I) also hardl connectioya n witsalinite th h y recog- The activity concentration of the Sr-90 in the 110 nizable. That signifies tha t thaa t t timCs-13e th e 7 water of the southern and central part of the Baltic 114 TABL Activit» EI Salinit- ) (A y) relationshi (s y Baltie th a n Se ci p - calculated regression equation- s

Isotope Date Area Fig. Number of Equation Corrélation samples A-Bq/m3| S-°/oo coefficient

7 13 - Cs 1977 Sila s Gotlano r lt Da d 2 30 A .15-9 + 0.439 S 0.49 Cs-137 1980 Dar s s Sill to Bornholm 2 14 A • o.4i7 4- 2.02 S 0.98 Cs-137 1983 Kattegat to 56°N 3 I 81 A .-1.74 + 2.05 S 0.99

Cs-137 1983 Gotland Deep to 60°N 3 II 104 A • 2.45 + 1.4l S 0.95 Cs-137 1983 Bothnian Sea to 63°30'N 3 III 58 A » 6.54 + 0.839 S 0.60 Cs-137 1983 Bay of Bothnia 3 IV 27 A m 4.69 + 1.43 S 0.88

Sr-90 1981 Kattega Gotlano t d Deep 40 A „ 20.3 + 0.017 s 0.047 Sr-90 1983 Kattegat to 56°N 4 I 80 A m 18.8 + 0.0233 s 0.16 Sr-90 1983 Gotland Dee 6o°o t p N 4 II 104 A m 18.6 + 0.0881 s 0.15 Sr-90 1983 Bothnian Sea to 63°3O'N 4 III 58 A m 10.70 + 1.40 s 0.66 Sr-90 1983 Bothnif o y Ba a * IV 27 A « 7.88 + 2.25 s 0.81

H-3 1980/81 Kattega Gotlano t d Deep 16 A m 9780 - 249 s -0.98 H-3 1983 Kattega Bothniao t a nSe 5 36 A m 8020 - 212 s -0.98

H-3 1983 Bay of Bothnia 5 4 A B 5135 + 707 s 0.99

variatione Th individuae th f so l measurement Sea in 19&3 was largely independent of salinity and values around the mean value, which are significantly geographica meae arounth t na l n i location dy la d ,an higher thameasuremene nth t errorexplainee b n ,ca d 19 Bq/m (Fig. 4 I, 4 II). The activity concentration by the temporally and locally strongly changeable originates froaccumulatioe th m Sr-9e th 0f no fallou t supply of Sr-90 over the rivers and the precipitation activity in former years. /~3 8_7, ,7 . Similar to the H-3 and Cs-137 distribution, the Compared with 1981, the mean Sr-90 activity con- suppl Sr-9f yo O poorer freshwater frolane th md into centrations decreased lightly (TABLE Ï). the northern Gul Bothnif fo recognizabls i a e th y eb strongly marked reductio e Sr-9th Of n o activity con- 3.2.3. Relationship Tritium - salinity (Fig. 5) centration with decreasing salinity (Fig. 4 III, 4 TV) The diagram (Fig TABL, 5 . show) EI largela s y in this area. linear connection between salinit3 activitH- d yan y concentration, independent of the sampling position considerabl watera se e . th parThi f o ts "younger", and depth / 9_7* From that, can be deduced - referred and for that reason Tritium—poorer freshwater, mixed to Tritium — a stationary distribution process be- with that from earlier year d thereforsan e more Tritium tween the inflow and outflow, precipitation and eva- containing Baltic Sea water. Thereby, there occured poration. a reverse of the inclination of the mixing lines (Fig. 5, TABL. El) r judgemen Fo temporae th f o t l changine th f go Tritium content in the Baltic Sea, one can call upon 3*3* Sediment samples an investigation made 2 1/2 years ago in 1980/81, The sediment samples taken at 6 positions in which extende Gotlane th d s froa Kattegae d th r m fa s a t the Baltic Sea coastal region were gamma spectroscopi— Deep /~10_7 (TABL. EI) cally investigated. For that, each time 200 g of dried The comparison of the Tritium - salinity re- sediment was measured in a ring beaker with a semi- lationship of 1980/81 and 1983 showed that the elements conduction detector (GeLi r ove)fo r 3«000 minutes. of the equation decrease more quickly than can be ex- Apart from Cs-137 otheo n » r artificial radio nuclide plained by radioactive decay only, that means that, at could be detected. The height of the measurement values present, more Tritium must escape from the Baltic Sea, varied strongly and depended quite clearly upon the owing to outflow and evaporation than is supplied by type of the sediment. Sand contained essentially inflow and precipitation. slighter quantitie Cs—13f so 7 than slick measuree .Th - ment values are compiled in TABLE II. e scatterinTh measuremene th f go t points around the linea rdiagrae showth n ni m clearl(Figs i , .5) y larger thameae th nn erro measurementf ro indit I . - catee smal value th th slf eo scal e local unevenness TABLE II» Content of Cs-137 in the sediment samples mixine ith n waterf go differenf so t origin. This effect emerges particularly conspiciously at the sta- Position Type of sediment Cs-137 tions X - ZZ in the northern Bay of Bothnia. It permits E N mBq/y gdr explanatio e followinth n i n g manner: $ 2 54°24- 5 '8 10°12' blac d kmu Sinc e endinatomie th eth - be f cg o e testth t a s ginning of the sixties, the Tritium content in the $ 2 5k°lt9,9'- 8 7 09°5k' blac d kmu precipitation, and thereby also in the inflows from 54°3O,1' 10°30" coarse varicoloured + , ^ land, constantly decrease 6_/_ dj . sand; shells e facOwinth to gt tha e timinth t f thesgo e 54°33,9' ,1' black mud kk investigations in the year 1983 was shortly after ' 11°13i9' gray sand; black mud; L + the snow thaw, comparatively large quantitief so 5 - shells "younger" freshwater flowed from land into this shal- ,7' 10°45,4' fine gray sand+ ; k gray 115 low part of the Baltic Sea, and thus represented a mud; shells ~ 3 k. ACKNOWLEDGEMENT / 7_7 JACOBSEN, T.S., Sea water exchange of the Baltict measurements and methods. The Authors would like to thank the Command and the Crew of R.V. GAUSS for the excellent support during The National Agency of Environmental Protection, the wor e colleaguet sea a kth wels a ,s a l s Messrs. Denmark (1980). Bergheim, Främcke, Gabriel d Goronc,an their fo y r /~8_7 Institut Radiatiof eo n Protection, Helsinki« special rapie efforth dn i tworking-of extene th f -fo Studie environmentan so l radioactivit Finlandn yi . sive sample material. Last, but not least, our thanks Annual Report STL-A 40 (1982). Mrso t .e Petersitzkedu e ar translatioe th r ,fo f no /~9_7 FRÖHLICH HEBERT . LANGD . D d Ver, r Eun ,K. Zu - the original German manuscript into English. teilung von Tritium in der Ostsee im Jahre 1980. Beitr. z. Meeresk. 49 (1983) 77-81.

5. REFERENCES /~10_7 WEDEKIND, CH., Tritium distributio spreadd nan - Baltin e i th a d Se c Nortan e th a hSe n i g in £~lj KAUTSKY, H., Radiological investigations in the 1980/81, as well as in the surface water of western Balti includina Se c g Kattegat during the North Atlanti n 1979i c . the years 197 o 1980t 5 . Deutsche Hydrogr. Z. 35 (1982) 177-186. Deutsche Hydrogr 4 (19813 . .Z ) 125-149. £~ZJ KAUTSKY H.-Fd an . . ,H EICKE , Radiologica- in l vestigation westere th e n th i s n d Baltian a Se c Bibliography n radiologicao : l investigation regioe th n ni s Baltic Proper includin Danise th g h Straits, Federae Baltie oth th f a carrie n i Se cl t ou d during 1981. Republic of Germany. Deutsche Hydrogr . (1982.Z ) 211-221. ^~3_7 AARKROG, A. et al., Environmental radioactivity H. KAUTSKY, Untersuchungen über die Verteilung des radio- in Denmark. aktiven Fallou Bereicm i t Nordseer hde s ,de Annual Report RIS0-R-487 (1982) 51, 61. Skagerra westlicher de d kun n Ostsee. /~4_7 WEISSROETHE. W , DREISIGACKERd ,W. an R , Tritium Deutsche Hydrogr. Z. 2k, 202-267 (1971). in the North Atlantic Ocean. C.N. MURRA H.-Fd Yan . EICKE, German coastal survey,a Internat. Atom. Energy Ag. IAEA-SM-232/98 (1979) compariso distributioe th f no behavioud nan r 315-336. of caesium and some transuranic isotopes. / 5_7 ÖSTLUND, H.G., The residence time of the fresh- Deutsch (1977)8 e 1- Hydrogr , .30 . .Z water componen Arctie th n i ct Ocean. . KAUTSKYH Gehalr ,de Caesiun Bodensedimenten a ti 7 13 m n J. Geophys. Res (1982? 8 . ) 2035-2043. der Ostsee. environmenta7 e TOMCZAK6_ th al, t / n e O ,. ,J l con- Deutsche Hydrogr 54-5, 30 9. .Z (1977). ditions affecting recent levels of Strontium-90 H. KAUTSKY, Radiological investigations in the western and Caesium-137 in the southern Baltic waters. Batli a includinSe c g Kattegat durine th g 11th Conferenc Baltie th f ceo Oceanographers Years 197 o 198Ot 5 . (1978). Deutsche Hydrogr. Z. 34, 125-149 (1981). CH. WEDEKIND, Tritium distribution and spreading in the n 1980/81Baltie i th a d Se cs an Norta , a Se h well as in the surface water of the North Atlantic in 1979. Deutsche Hydrogr. Z. 35, 177-186 (1982). H. KAUTSKY and H.-F. EICKE, Radiological investigations westere i th nBaltie th nd cBaltian a Se c Proper including Danish Straits, during 1981. Deutsche Hydrogr. Z. 35, 211-221 (1982). MÜLLER. G DOMINIK, ,J REUTHER. ,R MALISCH. ,R . SCHULTE,E , FTCIFRF7 1 - S1 L. ACKER, G. IRION, Sedimentary record of environmental pollution in the western Baltic Sea. Naturwissenschafte 7 (12)6 n , 595-600 (1980). E. SUESS and H. ERLENKEUSER, History of metal pollution and carbon input in Baltic Sea sediments. Meyniana 27, 63-75 (1975).

117 Okt. 1977

30 r 20

Cs-13o - n Surfaci 7 e Water 20- • ————• Cs-13 n Depti 7 h • 10 K...... X Salinity in Depth

10

Apr. 1981

30 - 20

20- -10

10 o c/>

-liroe uli o

30 - X' \ • 20

20 - • 10

0- ———— - ______o————————— -O -———— n

N 54'45' 54'45' 5450' 55-15' 55'20' 55'45' 56'30' 57'20' 57'SO' 5B'35' E 12-45' 14'45' 15-30' WOO' 17'30' 18'35' 19-30' 19'55' 19-55' 20'05'

Position Fig 1 . Cs-137 Distributio Regioe th n ni n Darss Sil Bornholo lt d Gotlanman d Dee n 197i p o 19837t .

< 30- <30-

Sali y t °/o i n 0 S a I ! n i I y °/oo

Pig. 2 Increase of the Cs-137 Inflow from the North Sea into the Baltic Proper between 1977 and 1980. ActiTity - Salinity Relationship.

) Darsa s Sil o Gotlant l d Okt.1977 b) Darss Sill to Bornholm March 1980 ( 56°20'N 18°30'E ) ( 54°50'N 15°30') E BaltiCs-13e th a Wate n Se c 7i n 1983 ri . 70- Activit Salinit- y y Relationship.

Kattegaa — la —— Bornholo t m Deep 56°N III»———» Bothnlan Sea to 63°30'N Gotlan• — dI—— I. Dee 60°o t pN IV o———o Bay of Bothnia 60-

É 50 s

40-

30-

20-

IV III 10-

10 15 20 25 30 Salinity O/oo

II 20 -

IV

V5

IT CO

- 5 Fig. 4 Baltie Sr-9 th Watea n Se 0ci 1983n ri . Activit Salinit- y y Relationship.

I o- -»Kattegat to Bornholm Deep 56°S III»———x Bothnian Sea to 63°30'S II •- -• Gotland Dee 60°o t p N IV o———Bothnif o y oBa a

10 15 20 25 30 35 Sali nit °/oo 120

E X

> 4

10 15 20 25 30 35 Salinity °/oo

H-3 in the Baltic Sea Water in 1985. Activit Salinity- y Relationship.

Letter Positioe ar s n Symbol; refe Jig.1o t r d Fig.13an 7 Z SurfacZ - A e Water w Botto- a m Layer SoJmiiy Tebmoytj 1382 5uv|ace awe/ bottom

124

Sctiim'uj /May-June/983 • surface 40 neat wo r bottom bottom stews "Fij. 10 Caesium 137 /Hae 138y3Ow ""Results in Evrortenns: between /.5fo3%

OH tkekvtl measured} 0 va/ue

40 down tönen,* bottom i« ^(?*H steps

125 126

StrcmtiuwSO "Results i EvYorterws: between l.5totä countin6 1 g erroir c/ej<**cfiM$ Hie level of measured value

ov «e&r bottom 127 HTDHOOIUralSCMeM INSTtTUT Ku»lM»« 128 nea4(?(v o « r bottom downû Ht o t Erwferuu between I.5to3% 16 courtitw) eimf depMdin^ CM Hielevt waiured/ io valut • Sulfate Error tef mi, between [,5to^% \ 6 counting er tor OH Mie levé/ o| measured valu • surface I Wm or nt&r bottom v down fo near bottow

Herausgegebe DEUTSCHEm nvo N HYDROGRAPHISCHEN INSTITUT Hamburg Error tcms'2o opt enov between tte /eve/ o/

Herausgegeben vom DEUTSCHEN HYDROGRAPHISCHEN INSTITUT Hamburg RADIOACTIVIT FucusYN I vesiculosus ALONG THE NORWEGIAN NORTH SEA AND SKAGERRAK COAST 1980-1983

G.C. CHRISTENSEN Institute for Energy Technology, Kjeller, Norway

Abstract

ANNEX6 e browSampleth nf o sseawee d Fucus vesiculosus have been col- lected fro place4 1 m s alon Norwegiae th g n coast e froUSSth mR NORWAY border in the north to the Swedish border in the south during the years 1980 to 1983. The sampling has mainly taken place once a yea Augusn i r r Septemberto n 198i d 198t 1an ,bu 2 samples were taken more frequently at some selected sites. This report pre- e samplinsent th resulte analysee s froC l th sth al m g f so f so points and *Cs, Co, K, and * *°pu from the points along 13 60 4C 239 2 the North Sea and Skagerrak coast. This part of the Norwegian coas mosf regardes o ti te b interes o t d o thit s IAEA co-ordi- nated research programm Baltie th n ceo Sea.

1. INTRODUCTION

Samples of Fucus vesiculosus (F. ves.) have been collected yearly at ten or more sampling points along the Norwegian coast e yearth in s 1980-84 mosf .O t interes e IAEth A o tBaltit a cSe coordination research programm sampline th e ear 4 g 1 pointo t 0 1 s along the North Sea and Skagerrak. The water masses which enter or leave the Baltic Sea will have to pass through this region, and samples from these points might give useful information in addition to the samples taken in the Baltic Sea itself.

The sampling programme has been continued also in 1984, but at the time of this meeting the analytical work on the samples from this yea s stili r ld onl an goin y, resulton g s from 1980- 133 e reportear 1983 d below 2. SAMPLIN MEASUREMENTD GAN S TABL . LocatioE2 sampline th f no g point Fucur sfo s vesiculosus 134 alon southere gth n Norwegian coast e samplinTh g points have remaine same mosr th dfo e t loca- No, Name Location Local name Year tions during these years samplee .Th s have generally been col- 10 Karm#y 59° 17 'N 05° 11 'E Mannes 80 lected in August/September each year. Bad weather or other unfo- 10A Utsira 59° 18 'N 04°54 'E Sk]evika 81,82,83,84 reseen reasons have led to later sampling a few times. The samp- ling points shortese ,th t distance betweee th n d thet seaan (a )m 11 Lista 58°04 'N 06°, 44'E Havika 80 58„07 'N 06 34'E Sevika 82,83 collection dates are listed in Table 1, and the locations are 58°06 'N 06° 35 'E Vâgsvollvika 81 show n e locatioi FigurnTh . 1 e n coordinate pointe th , f 10 so 12 Tromtfya 58°29 'N 08°55 Skare 80,81,82,83 10A, 11, 12, 13, and 14 are given in Table 2. 'E 13 T;j0me 59°04'N 10°25 'E Verdens Ende 80,81,82,83,84

The water at point 14 has lower salinity than at the other 14 Hvaler 59°03 'N 10°55 'E Brattest0 80 points, normally les so influenct thae o/oo0 du n2 , e e froth m 51°02 'N 10°57 'F Vikertanaen 81.83 rive rothee Glommath rl watee pointal .Th t highes ra sha r sali- nity tha o/oo5 2 n . All the Fucus plants taken were firmly rooted to the rock or large middlstonee th f n theiseo i r e zonf th growto e n i h freshr tida(o t l) we weigharea d e an normalls Th .tg wa k 5 y4- TABLE 1. Sampling points for Fucus vesiculosus along the Norwegian coast determines wa d afte plante rth d bee sha n d welri l t shakege o nt Sampling point Distance Collection date of the sea water. The sample was dried at 105 C until constant N o. Name (points, km) 1980 1981 1982 1983 1984 weight (the dry weight). It was then finely grinded and stored 1 r G Jakobselv 1-2,40 1-3,55 11 08 25 .08 21 .09 . _ in 200 closel 0m d plastic containers 2 Vads0 2-3,40 12 .08 24 08 - - - 3 Vard0 3-4,300 12 08 04 11 24.10 22 08 27.08 4 Ingtfy 4-5,320 - 07 .12 03 .08 22.09 04.09 The analytical wors includeha k d determinatio gammf no a 4A Hammerfest 4A-5;290 15 .08 - - - - emitter plutoniud san samplese th n i mgamme .Th a emitters were 5 Senja 5-6;195 17 .08 27 .09 - - - 6 Vestvagtfy 6-7A.270 5 6-739 ; 20.08 27 .08 30.08 29 .08 - % efficienc 5 2 detecte a yy b Ge(Lid ) detector with counting 7A Alstahaug 7A-7B.80 23 08 - - - - times of 150 000 seconds or more. The detector was carefully ca- 7B Kval^ya 7B-7.45 23 .08 - - - - 7 Vikna 7-8,295 - 30.08 18 .08 16 .08 30.08 librated for the relevant geometry using certified activity 8 Bud 8-9,140 03.09 17 .08 10.08 15 .08 - standards. 9 Vags0y 9-10/10A,305 05 .09 08 .08 - - - 10 Karm0y 13 .09 - - - - 10A Utsira 10A-11;165 - 02.09 31 .08 08 .08 15.08 The analysis of Pu has been based on a standard procedure 1a 1t s Li 11-12;155 14.09 26 08 21 .09 15 .08 - 12 Trom0ya 12-13,110 15 09 28 .09 20.09 27.09 - using liquid-liquid extraction with TTA, then back-extraction 13 T]0me 13-14,30 15.09 21 .10 14 .09 05 .09 09 08 with dusopropylether. After electroplating, the stainless steel 14 Hvaler 26 .09 22.09 30.08 - dish was counted in an alpha spectrometer by a surface barrier o sampln - e detector for 12-40 hours. Either 236Pu or 24ZPu was used as ra- diochemical yield monitor. Figure 1. Sampling points for brown algae along the Norwegian coast 136 3 RESULTS e sampleThth e n s generalli concentratioswa s C y f o n highes n 198i t 0 whemeasurementr nou s s startethe- ha de d n an d 31 137Cs in the Fucus creased. This decreas concentration i e n reflect reducee sth - re d leases from the above mentioned reprocessing plants during the As reported earlier [1,2,3] the presence of both 134,Cs and last years. The 137 Cs/potassium rati samplen oi s from 198o 0t e sampleth n i 137s s 'C ,show s that this radioactivity originates 1983 are given in Table 3 and plotted in Figure 2. The fallout from Western European nuclear reprocessing plants It shows that contribution to the Cs concentration has not been subtracted. the released radiocesiu transportes i m awar fa dy froe releath m - This contribution is estimated to be 0.038 Bq per gramme of pot- se points being diluted only to a small extent. Along the Norwe- e samplth assiu n ei m (1981) t wil I e .seeb l n thae th t gian coast from Lindesnes to North Cape, a distance of nearly concentration at the sampling points in the far north (1 to 4) e resultth 200 , 0skm from 198 d 1980an 1 show tha e concentratth - has not changed to the same extent as further south. e algath n ei decreases C tio f 3 dno a 2- factoonl y f b yo r similaA ] [2 r behaviou] [4 bees c ha rT n foun r fo d

e TABLTh Cs/potassiu . E3 m rati Fucun oi s vesiculosus along Norwegiae th n coast 1980-198 q 137-Cs/(B 3 . K) g US8* H«(th Cap«

i i

0,6 - O 1980 1980 1982 1983 D 1981 ° A 1882 8 ° ° ° '_ 1 0 22 0.16 0.21 05 •fr 1683 0 0 2 0.22 0 19 - - - ° 0 . O O i Q 3 0.24 0.20 0.19 0.16 0.20 0.4 4/4A 0.26 0.18 0.20 0.17 0.20 D D G • " 5 0.32 0.29 - - - S 4 - 6 0.47 0.38 0.28 0.22 0.34 O + 7/7A/7B 0.51 0.37 0.31 0.30 0.39 Q 8 0.52 0.51 0.34 0 36 0.43 0.2 - - % | 9 0.50 0.44 - - 10/10A 0 53 0.49 0.49 0.43 0.49 0.1 - 11 0.54 0.44 0 37 0.36 0.43 Ct/potasilum ritlo 12 0 49 0 34 0.36 0.27 0.37 t ii i t i i ii ,1 iiiii 13 0 46 0 36 0.37 0.37 0.39 9 8 2 1311 10/10 47 1 A1 3 B 2 T 1 A 7 4/4 6 A 5 14 0 37 0 54 - 0 33

e FigurTh Cs/potassiu . e2 m rati Fucun oi s vesiculosus 1980-1983 - no sample For those points where samples have been taken every year TABLE 4. The content of radioactivity in Fucus vesiculosus 1980-1983, the mean value of the 137Cs/K-ratio is 0.20 (point along the southern Norwegian coast 1980-1983. 3), 0 20 (4/4A), 0.34 (6), 0.39 (7/7A/7B), 0.43 (8), 0.49 <10/ 10A), 0.43 (11), 0.37 (12) d 0.3,an 9 (13) south-wese .Th t coast Sample Coll Ratio Concentration (Bq/kg dw) shows the highest concentrations. The concentration decreases no.___date dw/ww Cs 137 Cs 60 Co K 239*240 Pu also along the east coast (Skagerrak area) from point 10/10A to lest bu poin s, tha14 t n going northwards. 1980 10 3 -13.0 9 0.251 0.81t-0.22 13.5+-0.7 0.49+-0.30 790+-40 0.12+-0.04 concentratioe Th e south th gives C r -Bq/ks fo na w f d gno 11- 3 14.09 0.237 0.79+-0.17 16.5+-0.8 0.60+-0 25 950+-50 0.12+-0.04 ernmost points is shown in Table 4 and Figure 3. The low salini- 12- 1 15.09 0.256 0.67+-0.18 11.6+-0.6 0.79+-0.26 740+-40 0.09+-0.03 ty and influence from water from the Swedish west-coast may be 13 4 -15.0 9 0.216 0.60+-0.15 13.1+-0.7 0.59+-0.24 890+-40 0.07+-0.03 the oftee reasoth nr nfo hig h values foun samplen i d s from point 14- 4 26.09 0.159 0.74+-0.25 13.5+-0.7 1.10+-0.27 1130+-60 0.07+-0.03 14. 1981 10A-5 02.09 0.270 0.29+-0.12 11.1+-0.6 0.25+-0.12 710+-40 0.12+-0.04 3.2. Other radionuclides 6 26.0 - 11 8 0.203 0.73+-0.21 16.3+-0.8 0.25+-0.15 1150+-60 0.04+-0.02 4 28.0 - 12 9 0.181 0.54+-0.15 14.1+-0.7 0.31+-0.16 1280+-60 0.14+-0.04 Table 4 also gives the concentration of 1 *Cs,6 Co K and 13- 7 21.10 0.176 0.41+-0.15 15.4+-0.8 0.81+-0.40 1320+-70 0.16+-0.05 Qf furthermore given 9 22.0 - 14 9 0.170 0.67+-0.23 16.9+-0. 6 +-0.1. 9 7 970+-50 0.24-t-O.O? in Figur Lik. 4 e e 137 Cse conten,th 13f to *Cdecreases sha d dur- ing these e fouotheth r r years fo nuclidest ,bu o marken , d 1982 trend can be seen. High values of Co at the sampling points 10A-14 31.08 0.253 0.36+-0.12 10.9+-0.6 0.25+-0.06 690+-30 0.10+-0.04 east of Lindesnes may be due to releases from nuclear power 11- 8 17.08 0.197 0.62+-0.20 15.0+-0.8 0.66+-0.13 1260+-60 0.09+-0.03 Swedise plantth t a sh west-coast. 6 20.0 - 12 9 0.199 0.39+-0.15 9.7+-0. 5 +-0.1. 6 2 850+-40 0.09+-0.03 13- 9 14.09 0.236 0.36+-0.12 10.2+-0.6 0 86+-0.13 870+-40 0.27+-0.08 The plutonium found in the samples originates mainly from 14 no sample nuclear fallout, as the plutonium released from the reprocessing plants generall mucs i y h more rapidly sedimented thae radioth n - 1983 therefors cesiui d an mtransportet eno faro s d . 10A-20 08.08 0.228 0.35+-0.10 11.7+-0.7 0.6H--0.12 840+-40 0.18+-0.06 11-10 15.08 0.242 0.42+-0.13 10.1+-0.6 0.94+-0.12 870+-40 0.13+-0.04 12 8 -27.0 w n 9 0.64+-0.19 9.7+-0. +-0.5 1. 6 2 1110+-60 0.15+-0.05 13-11 05.09 0.165 0.19+-0.07 10.5+-0.6 0.72+-0.12 890+-40 0.05+-0.02 14-11 30.08 0.131 0.49+-0.1S 14.2+-0.8 1.6 +-0.2 1330+-70 0.18+-0.06

nw - no wet weight 137 Figur. 3 e Concentratiof no FucuCn si s vesiculosus 1980 -1983 (Bq/kg dw) Figur. e4 Concentration of 239*240 Pu o.n Fucus vesiculosus 1980 -1983 (Bq/k) gdw 140 3.3. Annual variatio e tadiocesiuth f no m conten Fucun i t s In 1984 sample takee sar n every mont e point ha th t bu 10A, analyses are, as mentioned above, not finished, and the results At some sampling points, samples have been taken several wil reportee b l d later. times a year in 1981 and 1982. The results for 13?Cs are given in Figure 5. It will be seen that the algae show similar behavi- e th northr t a fa s wele ,a s a th l n i 4 e point d th an ou t 1 sa r points 6 and 7 half distance between south and north. Generally 4. REFERENCES the highest concentrations are found in the summer. This is es- pecially well pronounced for the Cs/K-ratio, and one may con- 1. G C. Christensen, Radioactivity in Fucus vesiculosus along clude from this that cesium and potassium behaves biologically the Norwegian coast 1980-1981, 3rd Nordic Seminar in Radio- differen e algaeth resulte n i .Th t s show also thaannuae th t l ecology, Hyvinkaa (Finland) n Norwegian) ,(i y 19811-1Ha 2 3 . variation of this ratio is much less pronounced in the far north compare furtheo t d r south alon coaste th g . 2. G.G. Christensen, Radioactivity in Fucus vesiculosus from Norwegian waters, IAEA Coordinated Research Programme on the •Stud f Radioactivo y e Material Baltie th n csi Sea", Vienna Bq/kw gd Bq/gK (Austria) Jul9 ,5- y 1982. x 1 04 06 3. G.C. Christensen, Radioactivity in brown algae along the Nor- 07 + 10A wegian coast in 1982, IAEA Technical Committee Meeting on the 15 "Stud f Radioactivo y e Material Baltie th n i sc Sea", Stock- holm (Sweden), 22-26 August 1983.

4.E Holm Riosec. ,J G.Cd .oan Christensen, 99 TFucun ci s from Norwegian waters, Symposiu e Behaviouth n o m f o Long-liver d

10 Radionuclides in the Marine Environment, Lerici (Italy), 28 -30 September 1983.

t i i i i i i 5 ACKNOWLEDGEMENTS j r u 1981 19B2 1983 1981 1982 1983 This work has been supported by grants from the Nordic Figure 5. Annual variation of the 137, Cs concentration in Fucus Liaison Committe Atomir fo e c e EnergNorwegiath yd an (NKAn ) vesiculosus at the sampling points 1, 4, 6, 7 and 10A Counci Humanitiee Sciencr th fo l d ean s (NAVF). MONITORIN RADIOACTIVE TH F GO E MATERIALS BALTIE INTH A CSE

JAWOROWSKI*Z +,A BARANSKI*,D GRZYBOWSKA*, A PAWLAK*,J TOMCZAK**,A PIETRUSZEWSKI*, M SUPLINSKA*'**,D SKIBA**, T WARDASZKO* * Central Laborator r Radiologicayfo l Protection, Warsaw ** Marine Department, ANNEX 7 Institute of Meteorology and Water Management, POLAND Gdynia Poland

Abstract Between 197 198d 5an measuremente 4th concentrationf so Sr-90f so , Cs-137 Pu-239, 240, H 3, K-40, Ra-226, Ta-232, Ti, Mn, Fe, Zn, Rb, Pb, Cd and Sr have been determined in various components of the Baltic Sea radionuchdee Th s were determine radiochemicay db gammd an l a spectroscopic methods, and the stable nuchdes by differential pulse anodic stripping voltametry and by energy dispersive X-ray fluorescenc concentratione Th e f Cs-13 so Baltie th time7 7 cm o seawatet sp loweu s rwa time 0 Northere 2 tha t th sn bu i highe a nse rwate e thath nrm from Polish nverconcentrae Th s - tions of Cs-137 were related to the salinity In sediments Sr-90 levels were 1-2 orders of magnitude lower than thos f otheeo r nuchde radioactivite Th s founs fisf yo hwa orde 1 d f ro magnitude higheBaltie th n ri c tha Polisnm h lake nverd san s

INTRODUCTION Since 1975 Central Laboratory for Radiological Protection in /arsaw, in coooeration jiti tie Institu- f 'eteorologo e t d //atean y r "lanage-nent, Marine Depar- tmen Gdynian i t , e systematicarrieth t ou d c measure- ment radioactivitf o s f Soutnero y n Baltic. a Tn^ s swa continuation of a monitoring wnicn was started in 1960 whicn i d h an took paro othetw t r institutions, i.e.

141 + Chief scientific investigator 142 Marine Institut Fisherief o e Gdynin i s d Institutaan e SAMPLING AND ANALYSIS of Oceanology, Polish Academy of Sciences in Sopot. Water, samples Between January 198Decembed an 2 r 1984, this wors ha k The volume of water samples collected by KAHLSICO bee ne framewor th donIAEe n th i eA f Cooperativo k e batometer was about 50 kg. Immediately after collection Programm e Stud th Radioactivf o yn o e e Materiale th n i s the samples wer e2 wit- acidifie 1 h H hydrochlop o t d - Baltic Sea under the Research Contract No. 3037/RB. carriers C d an s, werSr c acid eri an dadded . Cs-137 This Research contract consis n monitorini t f o g was first obsorbed on ar.imonium molybdenophosphate 'WP) several radionuclides and stable heavy metals in water, d Sr-9ma an ts precipitate 0wa s oxalatea d . Cesius mwa sediments, seaweeds and fish from Baltic Sea and in few further purified by repeated adsorption on AMP mat, sampless from other regions monitorino t e Du . g cara- ion exchange chromatography on 3io-Rex 40 resin, and cter of this contract we refrein in this report from finall precipitates ywa d as~a cesium chloroplatinate. oceanographical and radiological interpretation of the Activit bacgrounw measures lo ywa a n i dd beta-counter results, which wil subjece lb othen a f ro t publication. in anticoincidence system. Recovery of cesium was

determine y weighinb d g Cs2PtCl,-.

13° K° 15° 16° 17° 19° 20° 56° 56°

OP40

OP2 O P5 >P3

55 55°

op 39

4° FIGURE 1.

POLISH SAMPLING SITES FOR RADIOACTIVITY MONITORING OF BALTIC SEA.. 13° 16° ' 19° Strontiu precipitates mwa d with oxalic acid dan -1 and deposited electrolitically on stainless steel. ammonia, together wit naturalla hC - y wa presene th n ti Activit plutoniuf o y s measuremwa y alfdb a spectrome- ter. The precipitate was dissolved in nitric acid and try. This method had, however, poor reliability, with purified by precipitation of Fe(OH), and BaCrO^ Final- the analytical erro abouf o r t 200% Ra-22. deters 6wa - ly SrCo, was precipitated from which Y-90 was milked mined after coprecipitation with barium, de-emanation after 3 weeks as oxalate and counted. of its ZDTA solution and subsequent counting of Rn-222 Tritiu s determinemwa y liquib d d scintillation i na scintillatio n cell, wit meaha n analytical error counting afte s electrolytirit c enrichmentw fe n .I of about 10%. Cs-137, Ra-226,Th-232 and K-40 were also seawater samples plutoniu determines mwa d usine gth determined in dried sediment by gamma spectrome-try of method developed for analysis of sediments. Pb, Zn and 5 cm thick core sections, with a Ge(Li) 32 cor detector Cd were determined in few separately collected small (mean error 10%). Ti, Mn, Fe, Zn, Rb and 3r were also volume samples with the differential pulse anodic stri- determined in the bottom sediments by energy dispersive pping voltametry. X-ray fluorescence', with the mean analytical error of The mean analytical erro Sr-9r fo rCs-13d 0an s 7wa about 15%.

- 1.0%, for H-3 - 15%, for Pb, Zn and Cd - 5%. Seaweeds and fish Se di Tient s Enteromorphn I a sp., Cladophor Chaetomord an . sp a - The core samples were collected with a spinster pha sp. collecte-d near Jastrzçbia Cora and Kuznica coas- corer and divided into 2 or 5 sections. The superficial d (Gaduco n i s d morrhua)an s t , herring (Clupea haren- samples were also collected with Van Ween grab sampler. gus flounded )an r (Pleuronectus flesus) 3r-9 Cs-13d 0an 7 0 Aftegram10 o r t sample drying9 5 e sth , wer t asheewe d were determined after dry ashing at 500°C, using the in nitric acid and hydrogen peroxide. 5r-90 and Cs-137 methods described above. was determined using the same methods as for water ana- lysis. To the samples used for plutonium determination RESULTS Pu-242 tracesamplee th s adde rd wa san d wer ashet ewe d geawater with nitric and sulfuric acid, and the silica was remo- The results are presented in Table 2 to 7. Concen- ved by evaporation with fluoric acid. After Mnerali- tration Sr-9f so Cs-13 d 0an 7 decreased steadily during 143 zation plutonium was separated by ion exchange on DOWEX e lasth t decade th Gule Gdansn th f boti fo n d hi kan Table 1. Monitoring stations for water and sediments samples in the Baltic Sea.

Station Coordinates Depth (m)

Zl i 2 54°23'U 18°57. 5'E 15

p 110 54°30'N 19°06. 8'E 70

p 116 54°39'N 19°18' E 88

p 1 54°50'N 1 9°20 ' E 107

p 'iO 55°38'N 18°38' E 95

p 2 55°18'N 1 8°00' E 75

p 3 55°13'N 7°01 4• E 91

p 5 55°15'N 15°59' E 89

p 39 54°45'N 15°08' E 63

B 12 54°2O'N 14°25' E 9

B 13 54°04'N 14°15' E 13

Tabl . Concentration2 e f Sr-90so , Cs-137Pn-239,24d an wateH e ,th f Souther o rn 0i n Balti. ' ' a (cnFi" Se ckg q

Depth y t Sa m ]i No. of Date br-90 Pn station (m) Cs-137 xïo' '^2

1982 ZN 2 82.06.03 0 0.6 19.6 11.4 1.5 82.06.03 14 7.7 25.9 14.1 2.9 P110 82.06.03 0 7.2 27.3 12.7 0.4 62.06.03 67 9.4 18.6 15.5 P116 82.06.02 0 7.7 21.2 13.1 a.o 82.06.02 85 10.5 21.8 18.9 1 P 82.06.02 0 7.6 20.8 14.3 6.6 1.5 82.06.02 105 10.6 20.9 20.6 P 5 82.05.28 0 7.7 21.0 17.0 2.8 82.05.28 87 14.7 17.4 32.2 P 39 82.05.27 0 7.7 20.4 14.2 4.5 82.05.27 60 11.9 35.4 1 8. 4 B 12 82,05,27 0 7.3 25.9 15.6 82.05.27 6 7.3 24.9 14.1 B 13 82.05.26 0 6.7 18.9 13.5 82.05.26 11 7.6 23.1 17.4 P 3 82.05.28 0 7.6 24.1 13-2 6.0 2.1 82.05.28 87 12.5 20. Ü 23.3 P 2 82.05.29 0 7.7 18.1 '16.6 9.7 82.05.29 74 11.3 29.4 31.4 P 40 82.06.01 0 7.7 14.6 19.1 6.9 6.1 82.06.01 89 10.6 20.8 16.3 1983 ZN 2 83.05.27 0 4.5 12.6 7.6 83.05.27 12 7.1 17.0 11.9 83.08.15 0 4.7 12.9 10.2 4.4 83.08.15 12 7.2 21.4 13-7 8.7 P110 83.05.27 0 7.1 19.5 11.7 4.4 83.05.27 68 9.2 19.0 13.3 83.08.16 0 7.8 20.1 12.1 83.08.16 66 8.9 22.2 15.2 collected 02.10.06 Tabl Continuation. a2 .

Ho. of Date Depth Salinity ür-90 Cs-1 37 station % XÏ05 Pn-239,240 (m) lOx"*

P116 83.05.28 0 7.0 20.2 12.2 7.1 83.05.28 86 10.5 19.1 13.4 83.08.16 0 7.7 19.6 15.7 83.08.16 86 10.8 22.0 16.2 1 P 83.05.28 0 7.5 21.9 15.3 7.7 83.05.28 105 12.1 24.2 22.7 83.08.16 0 8.0 22.2 18.3 83.08.16 106 11.6 22.0 19.8 P W 83.05.29 0 7.9 20.4 16.3 5.4 83.05.29 93 10.6 21.6 21.6 83. OU. 17 0 7.6 23.0 20.7 83.08.17 93 11.6 22.0 24.1 P Z 83.05.30 0 7.7 20.8 14.6 7.6 83.05.30 73 12.0 24.2 22.8 83.08.17 0 7.8 22.4 15-8 83.08.17 70 11.9 20.7 19.7 P 3 83.05.31 0 8.0 19.9 14.0 Li.O 83.05.31 89 14.7 26.5 31.8 83.08.18 0 7.8 17.2 15.5 83.08,18 88 12.7 23.5 25.9 P 5 83.05.31 0 7.0 23.8 19.0 4.0 83.05.31 87 16.3 26.3 34.2 83.08.18 0 8.0 23.7 16.6 83.08.18 87 12.7 25.7 38.6 P 39 83.05.31 0 7.9 19.1 14.1 3.7 83.05.31 61 10.8 21.4 20.1 83.08.18 0 8.0 21.8 15.7 83.08.18 61 13.8 24.6 23.1 ß. 32 83.06.01 0 8.4 21.1 25.3 83.06.01 6 8.4 20.4 14.3 83.08.19 0 8.3 17.5 22.8 83.08.19 7 8.3 17.1 16.1 8 13 83.06.01 0 6.0 17.5 10.5 83.06.01 11 8.2 18.6 14.8 83.08.20 0 7.6 19.1 14.1 6.4 63.08.20 12 8.0 17.2 13.8 6.6

Tabl . Vertica3 e l distributio f Sr-9o n Cs-13d 0an t 7Bornhola Gdansd an m) k 39 Dee) Dept1 P ( pp ( h n 198 i bracketn I 3 . (mB) g sqk dept t samplinha g site.

Salinity Station Da te Depth Sr-90 Cs-137 (m) *

1 P 83.05.28. 0 7.6 21.9 15.3 (l 07m) 20 7.9 22.5 15.8 40 B.O 21.6 16.2 60 8.3 20.7 16.5 80 10.2 22.3 20.1 100 12.0 24.2 21.8 105 12.1 24.2 22.7

P39 83-05.31. 0 8.0 19.1 14.1 (G?m) 20 8.1 19.9 16.6 40 8.5 18.5 14.8 55 9.2 ' 19.5 14.8 61 10.9 21.4 20.1 Table 4. Concentration of Cs-137 in surface oceanic water in October 1983.

activity concentration Location Date mBq kg"1

Spitsbergen 76°10fN 10°b6'E 83.10.05. 0.2

Norwegiaa 5e n 75°02'N O5010'u; 83.10.08. 7.1

Norwegian Sea 70°00'N 05°05'E 83.10.09. 13.8

Nnnthorri Sea 57°11'N 05°15'.E 83.10.12 88.6

7 06' 5 6 27'0 NNorther E a Se n 03.10.13 69.9

Tabl . Averag5 e e mounthly concentration f Sr-90o s , Csr-137 andH-3in surface water from Vistula river at Swibno (Sr-90 and Cs-137) and Warsaw (H-5) in 1983. In mBq kg"1.

H-3 3 Period Sr-90 Cs-137 x10

January 13.2 0.9 10.1

February 9.1 0.9 6.4

March 8.5 1.1 4.4 April 9.7 0.9 5.9 Hay 19.1 0.8 5.1

June 11. U 0.7 1.6

July 10.7 0.8 1.3 August 11.0 1.5 2.1

September 10.2 1.4 4.6

•October 8.2 0.9 2.4

Average 10.2 ± 1.5 3 1.0. 0i 4.4 i 2.7

Table 6. Concentration of Pb, Zn and Cd In the water of southern Baltic in August 1983. (/ug kg" }

Station Depth (m) Pb Zn Cd

P S 0 0. ÎO 't.B 0.13 k'i 0.40 5.7 0.03 65 0.76 2.9 0.07 85 1.02 4.9 0.30

B12 0 0.17 2.1 det.lim. 6 0.35 4.2 0.15

P39 0 0.15 i.8' det.lim. <|0 0.15 2.2 det.lim. 6Z 0.30 1.8 det.lim. TABU- . Averag7 : e concentration f Sr-9o sCs-13 d 0an n wate7i n Southeri r n Baltic during 1975-1983 (in jnBq kg" ).

('pea se n Gulf of Gdansk year Sr-90 Cs-137 Sr-90 Cs-137

1975 27.6 20. It 26.it 18.4 1976 26.7 18.0 24.9 16.5 1977 33.3 26.1 26.4 18.4 1978 27.6 18.8 25.6 15.6 1979 23.2 18. 4 19.1 15.2 1900 23.0 19.3 22.0 15.2 1981 22.7 19.7 18.0 11.9 1982 22-5 18.7 22.0 15.1 1905 21-5 19.8 19.7 14.3 198<)

Tabl . Concentratio8 e f Sr-90o n , Cs-137, K-40, Ka-226, Th-23 Pn-239,24d an 2 n bottoi 0 m sedimentf o s southern Baltic Sea (Bq kg d.w.)

K-40 Depth in Ra-226 Th-232 Pn-239,2 Station Date core(cm) Sr-90 Cs-137 x103 (y) —————(y p———— ) — 1982 P 5 82.05.28 0-5 0.7 9.5 P 39 82.05.27 0-5 0.4 E.9 P 2 82.05.29 0-5 0.3 6.5 P 1 82.06.02 0-5 0.4 11.0 ZN 2 82.06.03 0-5 0.6 26.7 P 40 September 0-5 73.0 0.8 81 113 5.6 5 - IQ- 60.0 0.9. 48 77 1.9 5 1 1 - 0 19.0 1.2 51 90 0.7 15-20 10.0 1.3 47 88 P 2 5 2 2 - 0 7.0 0.9 54 67 P 5 0-30 6.0 0.9 38 50 0-5 45.0 1.0 49 72 7.7 5-10 15.0 0.5 44 45 2.9 5 1 1 - 0 11.0 1.1 66 104 1.0 15-20 7.0 1.1 59 77 0.3 P 3 0-5 27.0 0.71 43 66 5.9 5-10 7.0 0.8 63 80 0.9 5 1 1 0- 7.0 0.9 81 101 0.4 P 39 0-5 73.0 0.8 33 not coll. 3.4 5-10 70.0 0.7 - 43 not' coll. 2.0 10 - 15 30.0 1.0 45 66 0.3 15 - 20 26.0 0.7 44 75 ZN 2 20 - 25 7.0 0.0 31 71 0-30 22.0 0.3 27 not coll. P110 0-5 126.0 0.72 59 not coll. 6.6 5-10 124.0 0.59 45 77 2.1 10 - 15 59.0 0.90 49 64 0.4 15 - 20 7.0 0.8 45 86 P116 0-30 50.0 0.9 51 98 1 P 0-5 148.0 0.7 83 106 9.1 5-10 71.0 0.8 74 94 1.7 10 - 15 17.0 0.9 80 not coll. 0.5 15 - 20 7.0 1.0 02 80 0.3 20 - 25 7.0 1.0 59 130 1983 P 40 83.05.29 0-5 0.20 21.4 P 2 83.05.30 0-5 0.33 16.7 P 3 83.05.31 0-5 0.44 18.1 P 5 83.05.31 0-5 0.65 27.2 P 39 83.05.31 0-5 0.74 25.0 ZN 2 83.05.27 0-5 0.81 21.5 P110 83.05.27 0-5 0.50 57.1 P116 83.05.28 0-5 0.33 20.4 1 P 83.05.28 0-5 0.52 41.2 B 13 83.01.01 0-5 0.15 13.2 148 open waters of the Southern Baltic(Table 7), Concentra- netals are similar to crustal abundances, except for tions of Sr-90 and Cs-137 were related to salinity of r whicS d h Ran be loweb see y o factob t r. m 2 f ro the wate d weran r e always higher neabottoe th r m than The concentratioe valueth f o s n factor r Sr-9sfo 0 surface th t a e (Tabl Ther, a strikin 3) es i e g differen- and Cs-137 in Gulf of Gdansk seem to be higher than in ce in the content of radionuclides in the waters of ehe otheo thtw e r localities studied (Tabl. e9) Baltic Sea, ocea d Vistulnan e seeab n y ni river ma s A . Seaweeds and fish contene th 5 f 5r-9 to d onl s Tablean 0wa y 4 twic, s2 e Concentration of Sr-90 in seaweeds are similar to as high in the open waters of Southern Baltic and Gulf thos f Cs-13o e d the7an y see exhibio t m t some geograp- Gdansk'af o Vistule th n i sa river, wherea Cs-13e th s 7 hical differences. The concent of Cs-137 in the fish content was 20 times higher in the Baltic. On the from Southern Baltic (range 1.1 to 6.6 Bq kg ) is one other hand the concentrations of H-3 in 1983 were si- orde magnitudf o r e highe rfise th tha hn ni fro e th m milar in Vistula and the Baltic Sea. However, the Cs-137 Polish lakes and rivers (0.1 to 0.37 Bq kg wet concentration Northere time7 th o n t wera si s p Se nu e weight). higher than in the Baltic, e concentrationTh f stablso e heavy metals exhibit a gradient increasing with depth (Tabl. 6) e

Sediments seee b Tabln ni y A ma sconcentration8 e Sr-9f so 0 in sediments were in 1982 and 1983 two orders of magni- tude lower than tha Cs-137f o t , Ra-22 Th-23d 6an d 2an abou 1 ordet f magnitudo r e lower than thaf o t Pu-239,240. Concentratio K-4f no 100s 0wa 0 times higher' than tha f Sr-90o t highese .Th t activit Cs-13f o y d 7an Pu-239,24 bottoe 0th werf mo euppem e c founth 0 n 1 ri d sediments, what is not the case with the natural radio- nuclides studied. Concentration e stablth f eso heavy Table 9. Concentrating Factors for Sr-90 and Cs-137 in the surface layer of bottom sediments in the Baltic Sea (sediments collected 27th May to 1st June 1983).

g Bk qd.w f sedimeno . t B

Region Station Sr-90 Cs-137

Gulf of Udarisk ZM 2 2235 P110 27 4293 P116 17 1519 P 1 22 1814

Gul f Poroorzo f e B 13 890

Open P 'iO 15 989

P 2 14 731 3 P 17 570 P 5 25 796 P 39 35 1245

Tabl . Heav10 elaye m c yf botto o rmetal5 0- m n i ssediment f southero s n Balti n Septembei c r 1982 (T!, Mn, Fe in % of dryweight and Zn, Pb, Sr in /ug g ). r S b K n Z e F n M i T Station

P 40 0.39 0.11 4.07 173 139 104

P 2 0.40 0.09 3.69 91 m 143 98

3 P 0.41 0.12 3.85 130 138 127

P 5 0.33 0.15 4.60 217 164 134

P 79 0.34 0.03 3-72 157- 135 120

P110 0.32 0.03 3.36 251 150 179

P116 0.38 0.03 '4.12 194 154 117

1 P 0. 38 0.03 4.47 338 141 93

ZN 2 0.31 O.OB 3-10 446 94 189

Table 11. Concentrations of Sr-90 and Cs-137 in seaweeds from wastal waters of Gulf of Gdansk in 19? d 19R 2kg"q an 3(R 1 d.w.)

Species Date Site Sr-90 Cs-137

Eiiteromorpha sp. 82. 07..29. Hozewie 2. 1 2..5

Cladophora sp. 82. 07. 29. Kuzni ca 2. 5 3. 3

Enteromorph. sp a 62. 07. 29. Kuznica 1. 7 2. 1

Cladophora sp. 82. 07. 29. Rozewie 3. 7 6. 3

Enteromorpha sp. 83- 07. 30. Jastrzcbia •1. 9 2. 0 Cora Cl^domorpha 83. 07- 30. Jastrzçbia 2. 1 2. 9 Gora

Cladomorpha sp. 83. 07. 31. Kuznica 1. 8 2. 1

Chaatomorpha sp. 83.07. 31 Kuzni ca 1. 6 1. a 150 Bibliography of Polish publications on radioactive Tabl . Concentratio12 e f Sr-9o n 0 a_Td Cs-13 n fis7i h from contamination of Baltic Sea. Southern Balti n 1962i c , 193 1984d 3an .

Cs-1 37 Sr-90 BOJANOV/3K PEMPKCWIAK, . I,R Akuraulacj, . ,J a Sr-90, Cs-, 137 Tissue Species data 1 fresBg" q h g Bk q fresn weignt weignt Ru-106, Ce-144 i Fu-239,240 w roslinach wodnych polu-

Cod Octooer muscle 1.9a dniowego Baityku. Oceanologia 7 (1977) 89-104. (Gadus 19S2 >.7b norrhua) 1.9C BCJANCV/SKI.R .3KIBA.D., , TCMCZAK,J e recenth n C t ., bones 10.6" levels of or-90 and Cs-137 in the Baltic Sea. Procc. April muscle 2.3 X-th Cont. Baltic Gceanographers, Göteborg (1976). 1983 bones 0.77a 0.84° BOJANCWSKI,R., SKI3A.D., TCMCZAK.J., Cs-13 Sr-9d 7an 0 January muscle 7.4 0.037 in Southern Baltic bottom sediments, Procc. XI-th 1983 bones 3.4 Conf. Baltic Oceanographers., Rostock (1973). Herring October muscle 1.6 (Cleupea 1983 bones 5.2* BILKIEWICZ,J., (Ed.), Procedure Radiuchemicar sfo d lan harengus) Aoril muscle 6.6 1983 Chemical Analysis of Environmental and Biological bones 0.75 Samples, Rep.No.CLCR-110/D, Warsaw (1978). January muscle 2.0 0.037 1984 bones 2.04 TQMCZAK,J., Radiochemiczne badania Poiudniowego Baityku. Flounder October .muscle 1.1 (pleurone- 1982 Instytut Meteorologii i Gospodarki Wodnej, Gdynia (1978) X ctes bones 5.9 flesus) April muscle 1.3 TOMCZAK.J., BOJANOWSKI.R., SKIBA,D., On the environ- 1933 bones 0.85 mental conditions affecting recent levels of strontium -90 and cesium-137 in the Southern Baltic waters. Procc. a,b, - parallec l determinations - xBq/dr y weight XI-th conf. Baltic Oceanographers, Rostock (1973).

ROSINSKI ,C.E., GMAZDOWSKI.B., SOSZKA.G .SAPIECHA.M, ., Method of calculation of individual and collective ra- diation doses due to utilization by population of the sea water, beaches and seafood taking into consideration the global and local sources of radioactive contamina- tion of the Baltic Sea. Report ORB No.7, Soviet Ekono;ni- cheskoi Vzaecnopomoshchi, Moscow (1979) in Russian.

3 JANCVSKI.R., SKIBA,D. , TCMCZAK. -S. , Rozmieszczanie or-9 0Cs-13i 7w osadac h Jennych Poludniowego Baltyku. ötudia i Materiaiy Cceanologiczne, Nr.25 (1973) 53-76.

TCMCZAK,J., Pole radioaktywnosci sztucznej Poludniowego Baltyku. Przegl^d Geofizyczny, XXVIII, z.1, (1983) 65-73.

TCMCZAK.J., Rozmieszczenie Sr-9 0Cs-13i 7wodacw h Morza Baltyckieg olatacw h 1975-1930. Studi Materiai a - ly Oceanologiczn 4 (19844 r H ), e 121-144.

KNAPI«rSKA-3KI3A,D. , BCJANOW3KI ,R. , FALKOWSKI ,R. , Pio- nowe rozmieszczenie Cs-137, naturalnego cezu i Sr-90 w wodach Poludniowego Baltyku w latach 1980-1981. Studia i Materialy Oceanologiczne 4 (19844 r ,N ) 21-33.

151 152 RELEASES DISTRIBUTIO PATHWAYD NAN R SFO RADIONUCLIDE BALTIE TH A N SCI SE

E. HOLM** . DUNIEC*S , . HALLSTADIUS*L . , S. MATTSSON***, J. RIOSECO*, C. SAMUELSSON* * Departmen Radiatiof o t n Physics, Lund University, Lund, Sweden ** International Laborator f Marinyo e Radioactivity, Océanographie Museum, ANNEX 8 Monaco-Ville, Monaco SWEDEN * Departmen** Radiatiof o t n Physics, University of Göteborg, Göteborg, Sweden

Abstract

Fission, activations product transuramd san c elements concentrations were measuredm water, sedimen resulte Th Baltie biot d f lon th so a an t n agci Se ter seasonad man l variationr sfo 137Cs, "Tc,235 «40Pu and M1Am are presented and discussed

Introduction

Artificial radioactivity in the Baltic Sea originates from fall-out, run off from land, nuclear power plants and inflow from the North Sea. r differenFo t radlonuclides different source differenn si te th area e sar most important.

The concentration levels in water also depend on dilution, evaporation, removing processes such as sedimentation biological uptake and outfloNorte th ho t wSea .

Durin lase yearw gth fe t e hav sw e concentrate n studieo d lonf so g 137 term and seasonal variations for Cs, 99fc, 239+240pu and 241 AJ,,

Samplin analysid gan s

Samplebrowe th nf so alga e Fucus have been collected occasionally from 1967-1978 and after 1978 on a more regular basis at fixed stations. During 1982 and 1983 Fucus collection took place along the Swedish west, sout d easan ht nortr coastfa possibles s ha sa collaboration I . n with the Institut Energr fo e y Technology, Norway sample f Fucuso d san Ascophyllum taken froNorwegiae th m n coas 1980n i t , 198 d 1981an 2 were also analyzed. In collaboration with DHI, Hamburg sampling expeditions in water and The 24lAm/239+240pu activity ratio was around 0.10-0.12 in all sediments were undertaken from the North Sea into the Baltic Sea in 1981 samples compared to 0.41 in Sellafield discharges (1980) and 0.30 (1981) and in the Baltic Sea in 1983. Many of the sediment and water samples in integrated fallout. from 198 stile 3ar l subjec analysisr fo t . In Figure 1 the results for plutonium and americium in Fucus along 137(; measures wa s d with Germanium-y spectrometry. the Swedish coas n 198 i te presented 3ar . Plutoniu d americiuman m were determine alphy b d a spectrometry with surface barrier-detectors after radiochemical separation. 10 9^Tc was measured by g-counting (GM-multicounter Risj/ system) after radiochemical separation. FINLAND

During the last 2 years a rapid and reliable method for ^^Tc 60 determinatio s beenha n developed.

Durin e samth ge tim have w e e also worke methoa n r o d fo d determination of 63jji an

RESULT D DISCUSSIOSAM N

Plutoniu d Americiuan m m

Activity concentrations of 239+240pu in Fucus vesiculosus from the south west coast of Sweden have decreased from SOOmBq kg"-1- dry weight in kg~197q abouo 1984n mB t 0i l 0 6 t. 24lAm concentrations have been more variable durin same th ge period (10-4 kg~l)q 0mB .

The activity concentration in water has been low during the whole examplr 197fo n i s (iB3 1 perio8 ewa d q1~ aboud an an d1 5 fiB 1 t1~ q for 239+240pu ancj 241^m respectively. In 1983 the corresponding activity concentrations were 7 /uBq 1~1 and 2 uBq 1~1. The observed activity concentration ratios Fucus/wate s 9000-1400rwa plutoniur 0fo d an m 10000-1800 americiumr 0fo .

In December 1981 we participated in a sampling cruise in the North and Baltic Seas organise I HamburgDH y b d .

From large volumes of seawater samples we determined the activity ratios 238Pu/239+240Pu 134Cs/137CS) 237Np/239+240pu and 241Am/239+240Pu.

The 237Np/239+240pu activit s 0.25-0.3y wa Nort e ratia th Se hn i o0 compared to 0.003 in global fallout and a few percent in the releases from Sellafield. We would lik divido et resulte th e s int groups2 o e ) thosth :1 n eo The 238pu/239+240pu activity ratio was about 0.15 in the North Sea west coast of Sweden with higher salinity water (7-15%o surface), and 2) decreasin Balti e 0.0o t th g 3n ci Sea. Plutonium from European those on the east coast with lower salinity water ( 5-8%o surface). reprocessing facilities could be detected as far as the Danish Straits For 239+240pu we fin(j a mean value of 100+30(1 SE) mBq kg-1 at the west and radiocesium as far as 55.2ON 20.QOE. coast and 171+50 mBq kg~l on the east coast in Fucus. 153 154 For 241Am we find the corresponding values of 14+2 and 25+5. Radiocesium

The mean Am/Pu activity ratio was 0.14 in both groups of samples. e sampleTh s fro cruise Baltid th man Norte a 198n a th ei Se c Se hn 1 i showed that i3*Cs was detectable in surface water to 55.2°N, 16.°E. The In October 1982 the results for Pu and Am on the east coast (Fig. 2) detectio 13*Ca,f no originating from European reprocessing plants, would were 91+14 and 19+6 mBq kg-1 which is lower for the May 1983 results for however be easier done in the deeper, higher salinity water which enters Pu but not significantly different for Am. from the North Sea. We hope to cover this subject more thoroughly during the expedition in 1983. The transit time of cesium from the Sellafield reprocessin 6 yearsestimates gBaltie 3- wa plan th e a b .o Se ct o t d

FINLAND orden I folloo rt lone wth g term variation measurement browe th nf so algae Fucus serratu Fucud san s vesiculosus were made. These sampled sha been collected since 1967 at a well defined sampling site at 56.76°N, 60 12.63°E.

e variatioTh 137ce th 8/Jn ni C rati Fucun oi s durin perioe th g d 1967-1983 is shown in Fig.3. In periods of more frequent sampling (1978-1983) a pronounced seasonal variation in the !37Cs/K ratio is seen with maximum value summen si minimud ran m value wintern si .

Our results show a significant increase in the 137Cs/K ratio starting in 1978 and reaching a maximum in 1981. e rati Th thes oha n decreased wit halha f lif approximatelf eo y 2 years.

The Figure shows a time delay of 4 years between the large releases of !37cs during the period 1974-1978 and their appearance at the sampling site.

From a collection of Fucus along the Swedish east coast in October 1 activity concentration 1982 (see Fig. 4) we found a mean value of 8.5+0.3 Bq kg" . This can be in Focus vesiculosus compared witfindinge hth May-Junn si e 1983 (Fig (11.8+0..) 5 kg~l)q 7B . during Oct. 1982 On the Swedish west coast the corresponding activity concentration was s 241flni cone, is given -1 137 4 Iteslashe th r , 13.8+1.3 Bq kg in 1983. The Cs/ OK activity ratio was very constant (neq kg"1 dry weight) (0.010 wese )easd th bottan t n ho coasts . The differenc resultn ei s between 198 198d 2an 3 might partle yb explained by the seasonal variation (June and October) of uptake of caesium by Fucus, and also by exceptionally high inflow from the North Sea.

The very close ratios on the different coasts in 1983 are only coincidences lowee Th .r 137cs activity concentratio ease th t n sidno e happens to be compensated to the same extent by a higher uptake due to It is obvious that the plutonium and americium values are higher in lower salinity. Fucus from low salinity water and to the same extent. In spite of that the activity concentration waten si r generall wese highes yi th t n ro not coast. This is not surprising and agrees with results for 137cs but e seasonaTh l variation shows thahighese th t t concentratio Fucun ni s for 99Tc. wese onth t coast occur summen si r when 137cs concentratio waten ni s ri lower. This shows that the uptake of cesium is metabolically We have not taken into consideration the large variability of controlled. It is also likely that a decrease of the salinity with a salinit eventuae th r yo l seasonan li variatiom A d an uptakr u nfo P f eo certain factor will result in a relatively higher uptake of Cs than with the plants. this factor. 0.7 FINLAND 0.02 0.6 13? activity ratio 60 in Fucus 0.5 •> 0.4

0.01 4 0.009 0.008 0.007

1.6/.22/7.1 .9/.12/7.5 Yearly released ! 137 ' 1.7/.24/7.1 Cs activity from I - Sellafield/PBq 1.3/.t6/3.2 Fig.4 0.1 "TC, Tc/Cs activity ratio, id !3'Cs activity concen 0.09 tratio Fucun ni s vesiculosus 0.08 during Ort. 1982 0.07 To/ §|/Cs (Bq «eighty kg"dr 1 ) 0.06

0.05

Fall-out level 0.04 North Atlantic "

4 8 2 8 0 8 8 7 6 7 4 7 2 7 0 7 8 6 Year

99Tc Fig.3 Ratio between 137Cs and 40K activity (left scale) and the 137Cs activity per unit mass potassium (right scale samplen )i Fucuf so s serratu Fucud san s The results from Fucu Ascophyllud san m collecte 198n i d 0 alone gth vesiculosus collected at Sardal (56.75 deg. N, 12.63 deg. E) on the west coast Norwegian coas showe tar fine Fign W n i decreas a d . 6 activitn ei y of Svreden during the period 1967-1983. The average potassium concentration was 23.1 ± 1.6 g per kg dry algae, which is.equivalent to 760 ± 49 Bq ^^K per kg concentration from 120 Bq kg~l at the south coast of Norway to 40 dry material reportee .Th d release 137f so Cs int ^ ioy r i sfroja e ,se m th B qnorte th kg~ ht l a coast . reprocessing plan spenr tfo t nuclear fue Sellafielt la d (formerly Windscale) are shown in the bottom half of the figure. A generally higher activity concentration occurred in 1981 and decreased again in 1982.

e activitTh y ratio Tc/C s ratheswa r constant s alon coaswa e d th g tan 5-8 for Fucus and 18-22 for Ascophyllum.

155 156 10 FINLAND _ -U 60 t - ï •

% 200 . • 'o> •• ' . & • S •° . " ^. 8P ° ° ! « S TOO- o • 1 ; o ° o • „ /Vf u O 0 .7/8.6 r tJ 8 8 50 o o .9/10.1 L> >1 v» 0 0 0 0 »r 3.u 0 y 0 0 <ö O Fucus vesiculosus ° , Fucu 'C, n i s s ^ dry weight and the,137Cs/40K 31 • Ascophyllum nodosum activity ratio xlO during 20 May-June 1983 , 500 1000 1500 2000 2500 3000 Distancm k n ei 99 Fig.6 Tmc activity concentration in Fucus and Ascophyllum in 1980 alon Norwegiae gth n coast. s r^ "^

The decrease of 99ïc activity with distance which depends more on For the transport of 99Tc from the North Sea into the Baltic Sea we dilution than biological removal or sedimentation, can simply be found a removal coefficient of 0.010 from south of Norway to the described as: southwest coast of Sweden during the summer of 1982.

A(x) A(o) exp-(ki x-exp-(x e resultTh r 99 Fucun sfo Tci s collecte Octoben i d r e 198th 2t a Swedish east coas e show tar Fign ni togethe4 . r witresulte th h s distanc= wherm x k n ei e for I37cs. mose Excepth t r southerlfo t y paractivite th t y dilutio= j k n coeff. km"1 concentration 99f vere Tso c ar y constant (1.3+0.1 Bqkg-1e th d )an k2 = biological removal coeff km~l activity rati 13?Cs i o s 0.15+0.04. sedimentatio= 3 k n removal coeff. km"-'- X = physical decay constant The results from the collection in 1983 are shown in Fig. 7. velocit= v f curreno y1 a" m k t The 99xc activity concentratio s 3.0+0. nwa Tc/Ce th kg"q 3B sd 1an activity ratio 0.27+0.02 on the east coast which is considerably higher We foun a totad l removal coefficien f 0.0005o t 5 km"1 alone th g than in 1982. We believe that this is due to some exceptionally high Norwegian coast. inflow of water from the North Sea during Spring 1983. 3 « Yea 1 r8 9 7 7 7 5 7 3 7 1 7 9 6 67 10 FINLAND

60

3.1/.37/ U.2/- .6X23) ?

2.5/ Fig. 7 3.1/40 3.0/.32 Activity concentratiof no 6.8/- m Fucus vesiculosus 3.9/.3 2 and theS^Ic/ ' * 'Cs activity 2.7/.17 ratio (afte slashe th r ) O/.36 Sanple . serratuF f so e sar narked wit. hS May-June 1983 (Eg kg" y weightdr 1 )

In 1983 durin Gause th g s expeditio wate0 1 n r samples were analyzed for 99Tc. For surface water we found a mean value of 68+11 Bq 1~1 and Year for botto 1~1q observee B Th . m1 1 wate + d r95 activit y concentration Fig 8. 99T c activity concentration (Bq kg- 1 dry weight) and the 99Tc ratio Fucus/water woulordee th Baltid44,00f e o r n th i the n e 0ci b n Sea. wesK ratie 56.7tth / t o12.6a Cs , coasn o 5 °N Swede E f t3° o n

e influencTh e from inflow f 99T fro e o Norte Fucun i th ca th m t Se hsa Swedish east coast is as expected much smaller than at the west coast. The results are shown in Figure 8. The activity concentration in Releases of 99Tc from Swedish nuclear power plants were not detectable in Fucus increased from ^3 Bq kg~l in 1967-1972 to 50-150 Bq kg-1 in 1983. Fucus. The activity ratio Tc/Cs in seawater was about 4-5 x 10~3 which is 20 times higher than the value in present integrated fallout. More During 1978-1983 a pronounced seasonal variation is also seen here water samples analyzee b hav o t e n ordei d certifo t r y this result. but with the opposite behaviour to cesium. For 99ic we have maximum in winter and a minimum in summer. The 99TC/(137cs/40K) ratio is also shown In the same way as for 137cs, the long term variation has been Figure.e ith n . This give n evea s n stronger seasonal relationshio t e pdu 157 studie a samplin t a d g site, 56.76°N, 12.63°E. the opposit. eCs behaviouo t c T f o r 99 158 80" We want to explain the results for Tc by the higher inflow from the Nort a durinSe h ge highe winteth d ran r outflow froBaltie th ma durin Se c g spring - summer. For technefum European reprocessing plants are the entirely dominant source whil r 13'Csfo e fallou s stili t f greao l t importance e e differenlevelTh th . f o s t e easvalueth t t a scoas f o t Sweden are indicated. It is also obvious that 99Tc is less or not at all salinity-dependent for the uptake in Fucus . The uptake is also less metabolically controlle 99r Tfo cd thar fo n

For the overall picture of the situation for in Fucus vesiculosus in the North Atlantic and Arctic waters results can be obtained from Fig. 9 .

Radioactivity in other biological samples

Biological material was collected in 1979-1980 from five different hydrological regions shown in Fig. 10. The results of measurements are 70°- shown in Table 1.

10

60

60°-

20 Kr- Fig. 10 Different hydrological régirais for sanpling. Result Tabln i s I e Fig.9._Activity concentration of Tc in Fucuc vesiculosus (Bq kg"1 dry weight) from the North Atlantic and the Arctic Ocean. For the Faroes and Iceland results for F. disticus ware also used. Results are from the Fareoes and Iceland in 1981, from Norwa 1982(below)d 198n an yi 1 , from Swede 1982n ni , from England and Scotland in 1982, from Ireland in 1983 and from Greenland during 1979-1982. The "TC/I^CS activity rati gives oi n afte slashe rth . Table I. Result from biological material from different hydrological e activitResultth r fo sy concentratio plaicd an codn ni l e ee , regions • collected during 1975-1982 are shown in Fig. Î1 . Bq kg dry weight Gadus irorrhua 239+240 241 30 137Cs pu

Bq kg (dry weight) Fucus 4.0 0.48 0.26 1« Mytilus (shell) 0.37 0.048 0.03 _Mytilus (soft parts) 3.7 0.41 0.04

Fucus 11 0.44 0.56 • 0 2

Mytilus (shell) ~ 0.007 - _ Mytilus (soft parts) 2.6 0.37 0.11 15 41 Pleuronectus f lesus Cod (meat) 16 0.004 0.007

Cod (bone) 5.2 0.004 - 10 _Cod (liver) 1.9 0.04 0.01

Fucus 4.0 0.44 0.11 flnqnilla anquilla 3« Mytilus (shell) - 0.04 0.03 Mytilus (soft parts) 2.2 - 0.07

Fucus 9.3 0.16 0.067 1975 -76 -77 -78 -80 -81 -82 Ar 4< Mytilus (shell) 0.04 -

kMytilus (soft parts) 4.1 0.096 0.03 activite Th 1 1 yg concentratioFi 137f no C thren si e different "Fucus 12 0.11 - fish species at the Swedish south west coast during 1975-1982 (from National Swedish Enviroratental protection 1693 n boarp v )dsn Mytilus (shell) 0.37 0.02 0.01

Mytilus (soft parts) 4.8 0.007 0.02

Cod (meat) 44 0.078 -

Cod (bone) 5.6 0.02 -

Cod (liver) 20 _ 0.01 159 160 Results for !37Cs In different fish species collected during 0.1 1979-198. e show13 1 ar d Fign ni an .2 1

Gadus morrhua

0.05 anguilla

Belone belone i i T i i i i i i i i l i i i i i i i i i i 111 i i i i i i i i i i 0.02 1980 1981 Mugil chelo

Gadus norrhua I 1 1 I II I I II I I Pleuronectus flesus

Pleuronectus flesus

Pleuronectus lunanda 1979 1981

Pig 3 .1 Cs/40K activity ratio fisn si h samples collecte 1979-1981n di . Pleuronectus platessa

References

0.02 0.05 0.2 The results in this report are mainly based on the following publications:

activite Th Fig 2 .1 y concentratio fisn i hK flesn / ratiCs h froo m different E. Holm, J. Rioseco, 1984 species collected during 1979-198 Swadise th t a 1h south west coast. Determinatio 99if no environmentan i V l samples. Nuclear Instruments and Methods in Physics Research 223 p. 204-207.

Duniec. S Hallstadius. ,L Holm. ,E , 1983 A study of the transport of radionuclides in the sea by use of isotopic ratios. In proceedings: Symp. on the Behaviour of Long-Lived Radionuclide Marine th n esi Environment a Spezia,L , Italy.

E. Holm Rioseco. ,J , 1983 99xc in carpets of lichen and soil. Seminar on the transfer of Radioactive Materials in the Terrestrial Environment Subsequent to an Accidental Releas Atmosphereo t e , CEC, Dublin, Ireland 193. ,p . E. Holm, J. Rioseco, G.G. Christensen, 1983. S. Duniec, L. Hallstadius, E. Holm, 1983 9$Tc in Fucus from Norwegian waters. In proceedings: Symp. on the A study of the transport of radionuclides in the sea by use of isotopic Behaviour of Long Lived Radionuclides in the Marine Environment, CEC, ratios. La Spezia, Italy. Behavioue Sympth n .o Long-Livef ro d Radionuclide Marine th n sei Environment, La Spezia, Italy,(in press)CEC S. Mattsson 1984. 137-Cs in algae from the Swedish west coast 1967-1983. Paper E. Holm, J. Rioseco, G.G. Christensen, 1983 presented at the 6th Int. Congr. of IRPA, Berlin, FRG. Fucun i sC fro"T m Norwegian waters. Symp on the Behaviour of Long-Lived Radionuclides in the Marine Environmnet E. Holm, J. Rioseco, S. Mattsson, 1984. La Spezia, Italy,(in pressC )CE Technetium-99 in the Baltic Sea. International Seminar on the Behaviou Technetiuf o r Environmente th n mi , CEC, Cadarache, France S. Mattson, 1984 (in press). 137-Cs in algae from the Swedish west coast 1967-1983 6th international Congr IRPf .o A S. Duniec, L. Carlsson, L. Hallstadius, E. Holm, 1984. Fucus vericulosus bioindicatoa (L. s )a Baltie th n ci r Sea. To be E. Holm, J. Rioseco, 1984 presente Internationae th t a d l Seminae Behaviouth n o r f ro Determination of 9?Tc in environmental samples. Radionuclides in Estuaries, Renesse, Holland. Nuclear Instrument Methodd san Physicn si s Research, 4 22320 ,. p Holm. E Rioseco. ,J Aarkrog. ,A Dahlgaard. ,H Hallstadius. ,L , 1984. E. Holm, 1984 Technetium-9 Algan 9i e from Temperat Arctid ean c Norte Waterth hf o s Review of Alpha-Particle Spectrometric Measurements of Actinides Atlantic. International SeminaBehavioue th n o r Technetiuf ro n i m Int. Journal of Applied Radiation and Isotopes, 35. p. 285 the Environment, Cadarache, France, CEC (in press). S. Duniec, L. Carlsson, L. Hallstadius, E. Holm, 1984 Fucus vesiculosu bioindicatoa s a ) Baltie s(L th a n crSe i International Seminar on the Behaviour of Radionuclides in Estuaries Renesse, Holland(in press) CEC Publications since 1980 relevant for the CKP. E. Holm Rioseco. ,J Aarkrog. ,A Dahlgaard. ,H Hallstadius. ,L , 1984 Technetium-9 Algan 9i e from Temperat Arctid ean c NortWatere th hf so Atlantic. Mattsson. S Nilsson. ,M Holm. ,E , 1980 Int. Semina Behavioue th n ro Technetiuf ro Environmente th n mi , Radioecological studie activatiof so n products released fro nucleama r Cadarache, France(in pressC )CE power plant intmarine oth e environment. 5th International Congr. of IRPA Vol III, p. 323 E. Holm, J. Rioseco, S. Mattsson, 1984 Technetium-9 Baltie th n c9i Sea. E. Holm, B.R. Persson, S. MAttsson, 1980 Int. Seminar on the Behaviour of Technetium in the Environment, Studie concentratiof so transfed nan r factor naturaf so artificiad lan l Cadarace, France(in press) CEC actinide elements in a marine environment. h t Internationa5 l Congr 1 IRPf III.l o 31 AVo , . p M. Nilsson, H. Dahlgaard, M. Edgren, E. Holm, S. Mattsson, M. Notter, 1981 Radionuclides in Fucus from Inter-Scandinavian waters. Impacts of Radionuclide Releases into the Marine Environment, IAEA, Vienna, p. 501

E. Holm, J. Rioseco, R.B.R. Persson, 1981 gg Surface barrier detector determinatioe th bet y b r asc fo T spectrometry f no . Method Low-Levef so l Countin Spectrometryd gan , IAEA, Vienna, p.227 Holm. E , B.R.R. Persson Hallstadius. ,L Aarkrog. ,A Dahlgaard. ,H , 1983 Radio-cesiu transuraniud man m element Greenlane th n s i Barent d dan s Seas. 161 Oceanologica Acta, i6, p. 457. 162 INVESTIGATIO RADIOACTIVE TH F NO E CONTAMINATION BALTI1980-198E N OI FTH A CSE 3

L.N. LAZAREV, Yu.V. KUZNETSOV, L.I. GEDEONOV, D.I. GUSEV, V.V. ANISIMOV, V.A. BLINOV, L.M. IVANOVA, T.E. ORLOVA, An.Vl. STEPANOV, N.A. TISHKOVA, V.P. TISHKOV, V.M. FLEGONTOV V.G. Khlopin Radium Institute, Leningrad ANNEX 9 S.M. VAKULOVSKIY, A.I. NIKITIN, I.Yu. KATRICH, UNIO SOVIEF NO T SOCIALIST REPUBLICS V.B. CHUMICHEV Institut Experimentaf eo l Meteorology, Obninsk O.A. PAVLOVSKIY, V.D. STEPANOVA Institute of Biophysics, Moscow Union of Soviet Socialist Republics

Abstract The content of radionuclides in the water of the Baltic Sea has been studied in the USSR since 1970. Durin perioe gth f 1980-198do investigatione 3th artificiaf so l radionuclides contents and distribution were carried out in different parts of the Baltic Sea. The objects of investigations were water, fish, bottom sediment seaweedsd san resulte Th . s obtainee dar presented in the paper.

INTRODUCTION

The investigation of the radioactive contamination of the Baltic Sea started in the Soviet Union in 1970 /1/« At ..that timradiatioe th e n situatio .the.-Baltin ni S WA a cSe fully determine globay b d l radioactive fallout nucleao ,n r power plant workin consequencee s coastth it t n g.o Bu f so the global radioactive contamination appeared to be great shalloa r fo w semi-closed Baltie basi th becausa f cSe no e of limited possibilities for water exchange and dilution of the radionuclides fallen out on its surface. In 1970 1. Radionuclides content watere th n si the contaminatio surface n th rat f o ee waterBaltie th f cso Baltie oth f prope a cSe r

f Sea by ° Sr and Cs was more than 6 time higher than the Tabl summarize1 e e resultd th san s f 'C so vSr, QQ 1 '3 7 contaminatio watere Atlantie th th f f so o n c e Oceath f o n tritium determinatio surface th deed n i nan e p waterf so same latitude zone /1/. The development of nuclear energy the mentioned regione Baltin 1980-1983i th a f cSe o s . e Baltith n i c countries e Baltinecessite th ,th e cus o t y The results for the year 1983 are also presented in fig. 1-4. Sea as a cooling pond for KPP's and the high global e determinationTh s showe de st-c th tha . n aquatorti y radioactive background in its waters attracted attention investigate distributes wa r S d 9d0 practically regularly to the investigations of the radioactive contamination durin whole gth e perio f observationso d . of this basi d latean n r stimulated annual systematic many- The concentratio f tritiuno e observatio th . ir m n points sided investigations of the radioactive situation on the e aquator Baltie th th n a propeo f Se co y s practicallrwa n o y Baltic Sea. the same level during the period 1980-1983. n connectioI n wit constructioe hth forthcomind nan g The obtained results demonstrate stable contentf so setting into operatio Leningrae th f no detaileP dKK d tritiuBaltie watere th th a durinf n cSe o si mperioe th g d investigations of the distribution of long-lived radio- in question and absence of a noticeable influence of any nuclide e Gul th Finlanf Baltie fo n th i swera f Se co de tritium sources on its contents. It is worth mentioning carried out in the Soviet Union in 1971-1973 /2/. later Baltie tha th parn neaa i tf straite Se co tn ri th d san the investigation radioactive th f o s e contamination both the bottom flow of water from the North Sea lowered of the Baltic Sea proper and of the Gulf of Finland were tritium concentrations were observed (1982, table 1). USSe th R carrie n annuallyi t extensivn a ou d d ,an e It follows from here that the water exchange through the experimental materia pase th t r periolfo timf s o d wa e straits leads to decrease of tritium concentration in the published e chronologica;th l lis f literaturto s i e Baltic Sea /12/. presented in the References /1-18/. Another picture is observed in the 1 ^'C"^7s distribution. During the period of 1980-1983 the investigations of Durin specialiste lass e showyearw th wa gth t fe y t nb i s s artificial radionuclides contents and distribution 7/ere of Denmark /19-2V, USSR /10-12/, GFR /22, 23/ that there carried out by Soviet specialists in different parts of is a supply of water with increased radioactive caesium the Baltic Sea: annually - in the eastern part of the concentrations froKorte intth ma Baltie hSe oth c Sea; Balti propera e Gule cSe th th Finlan f f o n n i ,i d dan it was marked that there is a danger of an additional mouths of the rivers inflowing into the Baltic Sea from contaminatioexpansion a f o d ^Baltithif e no an th s a f nco Se the territor USSRe th somn ; f i southo e ye th year n -i s- contamination. In 1980 the concentration of 1 37Cs reached western part of the Baltic Sea, in the regions of deep 86 Bq/nr'ln the bottom "water in the "south-western part of nollows and in the straits connecting the North Sea and the Baltic Sea, being under direct influenc watee th rf o e the Baltic Seae objectTh . investigationf o s s were water, supply froHorte bottoe th mBq/n0 th h 17 n Seami rd an , fish, bottom sediment sea-weedsd san obtainee .Th d water of the Skagerrak strait. Besides, together with an results are presented in separate sections of the increased contents of ^ CB, was also found. The 10* investigation» 164

Table 1. Concentration« of ^°Sr (Bq/m^) (kBq/nr' (Bq/nrH e e enter^ Balti th th d n f an I o )s)c Sea. 1900-1983.

Coordinate1 of s g. I960 1981 1982 1983 tie aatnpllng Bite 1 t "" June-July July July May-July v Lst. N Long* E I« •3. 90 •j 90 137 90 i 3x a « 37 1 — ß <3VCB 3„ oo Wi i B « r o «j Sr h C°/od o Sr °/C,o sr '«c. 3H Oreral l wmte r j CO ; depth , m | E-2 59°30' 23°00- 85 0 19,014.0 II,Ol2,0 6,7l2,6 I9,0l4,0 9,0t2,0 6,Ii2,5 7,0 20,0t4,0 I4,0i3,0 4,6il,8 6,3 22,014,5 II,5t2,0 S.0l2,0 E-2 59°30- 23°00- 85 40 7,7 20,0+4,0 13,512.5 E-2 59°30' 23°00' 85 80 10,6 15.013.0 I8.5U.5 E-A 59°00' 2I°30' 100 0 22,Qt4,Q W,0i2,0 I2,0i4,0 21,0i4,0 II,Ot2,0 6,8i2,9 7,4 22,014,0 I6,0ii,0 6,3il,6 7,0 22,014,5 I3,0t2,5 7,It2,0 E-4 59° 00* 2I°30« 100 50 8,0 17,513,5 15,012, 5 E-4 59° DO- 2I°30' 100 90 10,6 2I,Ol4,0 I8,5i3.5 E-« SS0 00- 20°45- 95 0 20,0l4,0 13,0+2,0 7.5+Z.4 22,0i4,0 I2,0t2,0 6,fli2,^ 7 5 2Q,Ot4,ß-19,0+3,0 6,4i2,I 7,9 22,0l4,5 I5,0i2,5 6,6il,8 E-6 S8°00' 20°45- 95 50 8,7 21,014.0 I*,5i2.5 E-6 58°00' 20°45' 95 90 10,0 2I,Ot4,0 I6,5i3,0 E-37 57°22- I9°57- 240 0 20,0+4,0 I4,0t2,0 6,6i2,5 22,0+4,0 I6,0i3,0 5,4iE,6 57, 22,0i4,0 I5,0i3,0 I0.6l2,3 8,3 Z0,0l4,0 13,012,5 5,0i2,0 E-37 57°22' I9°57' 240 75 9,2 2I,Ol4,0 I6,0i3.0 E-37 57°22- I9°57« 240 ISO 12,6 18.513.5 17,513,0

E-37 57°22' I9°57- 240 200 I9,0i4,0 I7,0i3,0 I9,n4,0 I9,0±3,0 5,4i2,7 59, 2I,Oi4,0 22,0i4.0 7,5il,9 ±

E-46 S6°06' I9°I4- HO 0 22,0i4,0 I4,OtZ,0 I9,0iii,0 I6,0i5,0 I0i4,0 7,8 20,014,0 15,0+3,0 6,2il,6 8.3 20,014 ,0 I5,0i2,5 9,0t2,5 E-46 56°06» I9°I4' HO 75 lo.n 19,514,0 18,513.5 E-46 56°06- I9°I4« HO 100 20,0+4,0 I8,0t3,0 I9,0i4,9 0 9, I9,0i3,0 23,n+_4,0 I7,f^t3.0 8.312.1 18,013,5 20.0t3,5 E-50 55°30- I8°53- 90 0 2I,Oi4,0 I7,0t3,0 7,3i2,4 19,0+4,0 17,0+5,0 5,5i2,4 7,8 22,0i4,0 I5,0t3,0 8.3l2,I 8,0 22,014, 5 15,513.0 7.H2.0 E-50 55°30- I8°53' 90 40 8,4 17,013.5 E-50 55°30- I8°53- 90 80 2I,Oi4,0 I8,0i3,0 21,0+4,0 I7,0t3,0 4,8+2,4 9,7 22,014,0 I8,0±3,0 *4,0 10,1 20,5t4,0 16,513,0 E-5I 55°00- I4°00- 45 0 8,2 20,0i4,0 I5,0i3,0 5,8tl,6 7,4 21,0+4,0 IS.Otf.O 1 B-SI SB^ÖO ' I4°00' 45 20 8,r 20,014,0 I5,0l3,0 6v5ll,8 8,9- 2I,Ol4,0 I3,0t3,0 E-5I 55°00- I4°00« 45 40 8,7 23,0t4,0 20,0l3,0 9,3t2,0 I8,0t3,0 E-52 54°43- I2°47- 22 0 7,9 21 ,0i0 , 4 I6,0i3,0 8.7 20,014,0 I8,5t3,5 E-52 54°43« I2°47- 22 10 8,1 2I,Ot4,0 I7,0l3,0 5,2tl,7 10,5 19,014,0 2I,5l4,0 E-52 54°43' I2°47- 22 20 8,5 2I,Oi4,0 I7,0t3,0 7.9H.8 13,8 I8,5l4,0 27,0t4,0 E-53 54°28- I2°I3' 19 0 9,6 22,0t4,0 2I,Ot4,0 Hl2,I 13,7 2I,Ot4,0 24.514,0 B-53 54°28- I2°I3' 19 8 10,0 2I,0±4,0 2I,Ot4,0 4f7t2,0 14,0 20,014,0 26,514,0 E -53 S4°28- I2°I3' 19 17 16,3 20,0+4,0 36,0+5,0 -.4,0 16,0 20,0+4,0 33,015.0 Salinity, o/oo. 1'983. In brackets-sampling depth, m.' I

Pig. 2. activitr S ° y concentration, Bq/ m. 1983 . In brackets-sampling depth, m.

r a " .t.u-,.w«.E—». • « c i * S 1 Fig. 3 + - -1 -jr-f 'Cs activity concentration. Bq/ m1983. . brackets—samplinn I g depth. jm

.S • Sampling oiteo

activity concentration, kBq/ro3. 1983. n brackets-samplinI g depth_ nu ,

* M * U IV ~ 6.«*M Ll^* II , 2C^~.Cn.»r * II V average value of -^Cs concentration in the deep waters of

the strait s 2.6+0.swa surface 8th Bq/mn i e d one'an - s 40- 0.1+0.0- 8 Bq/m3 /12/ evidens i .t I t thawatere th t s coming contaminatee froNorte ar th ma hSe d with radioactive wastes of technological origin. Durin same gth e period n 1980,i , 30 the influence of contaminated watc rs oi vnc North Sea wasn't observed in the eastern part of the Baltic Sea a proper e datth : a presente n tabli d demonstrat1 e e equal « distributio e point th f o n•*' l sy deptCsb al n 1i h 3 7 20 investigated, including the Gotland depth. In 1981-1982 a tendency appeare e s concentrationincreasC th o t df o e s 1 Ty in the deep waters of the eastern part of the Baltic Sea, e resultbuth t s haven' t exceedetye limite th d f o s 10. experimental erro rdeterminationse (tablTh . 1) e , carried ouy Finnisb t h specialist e Gottlanth n i s d dee n 198i p 1 didnH show any difference in the ^'Cs concentrations in the surface layer and at the depth 234 m /24/. And at the T10 M2 U ^° end of Kay, 1983, according to our data, in most Salinity, o/oo. Pig. 5. investigated pointe easterth f so nBaltie th par a f ctSe o Dependence of the concentration 137JI,Ca from the salinity. Baltic Sea. 1983. e bottoe concentrationth th n i m wateB C * • r layerf so s appeare muce b ho t dhighe rsurface th tha n ni e ones. Beside increasn a s watef o e r salinit same th e n i ypoint s and horizon s markeswa n 198i d comparison 3i n with 1982 Table 2. (tabl fig, correlatioA 1 e . .1) ns betwee^C e nth Concentrations of "''Cs and in the deep -waters of the Baltic Sea. 1983. concentration and the water salinity was clearly

manifested (fig. 5): the higher the salinity, i. e. the Serial Station Deeps Coordinate f o s Sampling Overall Sampling Salinity Sampling Concentration '37Ce greate contributioe rth Norte watersa th hSe f o ne ,th e samplinth g site . datNo Noe . water depth, m o/oo volume,! Bq/m3 higher the 13^'C7 s concentration. Lat.H long, E depth, m 137^ 134Ca '-^Co

Juln I y 198 bottoe 3th m waters were investigaten i d _ - I. 80 Arkona 55°00' I4°05' 18.07.83 46 0 7,8 1250 12,0 the deep-water Arconae deepth s- Borriholme ,th e th , 2. 80 Arkona 55°00' I4°05' 18.07.83 46 45 12,0 30UO 2Z,Q 0,32 70 f Gottlane o Gdans tu y d wa an ke d th one n o stha- e tar 3. 62 H Bornholm 55°IO' I5°57' 17.07.83 90 0 7,5 730 12,0 - - 4. 62H Bornholm 55°IO' I5°57- 17.07.83 90 88 15,0 3000 20,0 0,24 80 waters expansion from the North Sea. Water samples with 5. 55 Gdansk 54°55' I9°26' 27.07.83 :02 0 7,1 1210 11,0 - _ the volume from 23001 io 45'60 Iwere taken for 6. 55 Gdansk 54°55' I9°26' 27.07.83 102 100 11,2 3035 18,0 0,15 120 determinatio f n^'Co d -^Csan s contents resulte .Th s 7. 46 Gotland 56°05' I9°I4' 24.07.83 130 0 7,3 300 11,0 - _ 8. 46 Gotland 56°05' I9°I4' 24.07.83 130 100 9,0 4560 15,0 0,11 140 determinatioe ofth s presentee wa nar s C tabln i d : 2 e 9. 37 Gotland 57°22' I9°57' 22.07.83 240 0 7,1 600 13,0 - _ 167 deee deepe founth th p n sl wateri d investigatedal f so , 10. 37 Gotland 57°22' I9°57' 22.07,83 240 170 11,2 2300 18,0 0,12 ISO including the Gottland one. Its concentrations decrease 2. Radionuclides contents in the waters successione bth y Arcone :th Bornhola- Gdans- m k- e Gul oth f fFinlano f d Gottlan recessioe th y db deeps. ne fro. straitse ,i th m , 137r linn i epresence bus witth t™C increasen a h f o e d contente '-"Cd Ian n r resultstable S ' th ther 3 ef e so ar e unambiguousls C of y testify abou penetratioe th t f no determination in the surface waters of some parts of the contaminated waters from the Horth Sea by the system of Gul Finlanf fo 1980-1983n i d ; fig represent.6 e th s deep-water Baltie depthth f cso Sea e compariso.Th f n'o e resultalth l s n 198obtainei s 3u y showb d s thae th t Table 3. Concentrations of ^°Sr (Bq/m3) end 137Cs (Bq/m3n )i th« surface iraters of industrial radioactive contamination not only continues e Gul th f FiJilanâo i . 19BO-1983. to penetrate from the North Sea but it has occupied deep Ssntiling Index 1980 1 981 1982 1983 . layer vasa f to s aquator Baltie th f co y Sea, including region of fne ««j-Julj June-J IÜJ June—July Kay-Auguat

its easter north-easterd an n n region d wilsan l expand from sample 7 I37 *w "7Ce *>Sr »7C. °/00 *>Sr " C= "/CO 9°Sr C» the deep layers to the surface ones. In 1983 the increase 1 37 Ba f Her3 o - j ' »24,0+.4, 0 I,5tO,8 2*, 0+4,0 I.OtO.7 0, 5 28, Oil ,0 <3,0 1,0 27,0+>,0 <2,0 of Cs concentrations in the surface layers of the Baltic 5 - Z3,0t*,0 I,5tO,8 23,0*4,0 2,0tl,0 0,7 26,0±4,0 •0,0 1,0 27,0+4,0 < 2,0 Sea didn't manifest itself yet e comparisoTh . n wite th h -7 23,014,0 I,5tO,8 24,0+4,0 1,0+0,5 0,7 26,0+4,0 <3,0 1,0 25,0t4,0 2.0+.I.O -9 20,0+4,0 I,5tO,8 25,0+4;,0 2,0tl,7 0, 0 24,0+4,0 '3,0 1,0 26,0+4,0 .2,0+1,0 data of 1982 /18/ gives grounds to suppose that side by -10- 20,13i4,0 0,7 28,0+4,13'*' Vs.o side with the continuous inflow of water from the Korth AYtrag r regionfo e : 22,0+4,0 I.5+.0.8 24,0t4,0 I,5+.0,7 26,0+4,0, 8 0 •=3,0 0 26,0t4,1, 0 0 «a2, Sea', last year large-scalthera s ewa e intrusioe th f no Bay of »-26 22,0+4,0 8,0t2,0 22,0+4,0 5,0t2,0 2,8 27,0t4,0 '9,0ta,0 3,3 27,0t5,0 8,0tl,5 Korth Sea water into the Baltic Sea, that lead to such a Coporle »-27 2I,Ot4',0 8,0+2,0 22,0+4,0 6.0t2,0 2,6 23,0+4,0 5,0t2,0 3,3 27,0t5,0 I0,0t2,0 wide expansion of contaminated, more saline and, therefore, »-28 25,0±4-,0 7,0^2,0 23,0t4,0 6,0±2,0 3,1 28,0±4,0 4,0±I,S 3,4 25,015,0 6,'OtI.S »-29 23, 0+4;, 0 6,0+2,0 23,0+4,0 6,0±2,0 2,0 23,0+4,0 3,5+1,5 3',* 27,0+5,5 6,5±I,5 heavier waters in the deep horizons of the Baltic Sea. »-30 24,0t4',0 8,0+2,0 22,0±4,0 6,0+2,0 2, * 22,0+4,0 *,OÎI,5 3,3 28,0i5,5 5.0H.5 The information of Polish specialists-hydrologists proves »-3I 22,0+4,0 5,0t2,0 22,0+4,0 5,C*2,0 J.I 25,0+4,0 5,0+2,0 3,3 27,015,0 5,0+1,5 »-32 22,0±4,0 9,0+2,5 20,0+4,0 6,022,0 1,8 24,0t4,0 5,OÎ2,0 3,3 24,0t5,5 , l 0Oi , 6 this supposition: in November 1982 they marked an inflow »-Î3 22,0i4,0 8,0t2,0 21,0+4,0 6,0+2,0 2,9 26,0t4,0 8,0+2,0 3,4 25,0i5,0 6,011,5 of water froKorte th m h Sea volumen i , m k abou, 0 20 t »-34 23,0+4,0 9,0t2,0 ZZ, 0+4,0 7,0+2,0 2,4 22,0+4,0 9,0i2,0 3,3 22,014,0 4,0tl,0 that is comparable with the well-known inflow in 1951. »-35 24,0t4,0 5,0t2,0 3,2 27,0t4,0 5,512,0 3,2 29,0t6,0 S.OtI.5 Arerage for region : 23,0+4,0 7,5t2,0 22,0t4,0 6,0t2,0 2,6 25,0t4,0 5,512,0 3,3 26,0t5,0 6,0tl,5 Tne observations were carrie sinct ou d e Kovember 1982 till V-ay 1983. During this time the water masses from the Korth Eao tern »-II I8,0t4,0 8,0t2,0 24,0+4,0 6,0+2,0 1,5 28,0+4,0 3,0tl,5 2,7 24,0+4,5 8,0i2,0 part »-I2 22,0i4',0 8,0t2,0 24,0+.4,0 5,0t2,0 1,5 23,0t4,n 3,0tl,5 2,4 27,ni5,n 8,0+2,n Sea came by the bottom horizons from the straits to the »-I3 20,0±4,n 8,0t2,0 23,0t4,n 5,0±2,0 H, 4 25,0t4,0 3,5+1,5 2,2 22,014,0 5,5tl,n Gottland deep /25/ e determination.Th s were don oxygey b e n #-14 2I,0±4-,0 8,0t2,0 20,0t4,n 6,nt2,o 2,8 23,0t4,0 9,5+2,5 3,2 25,0+4,5 S.Stl.S »-I5 ig.o+i.'.n 6,0±2,0 22,0+4,0 6,0±2,0 3,0 24 ,0+4, 0 7,0i2,0 2,5 24,0t4,5 5,QtI,0 and salinity e dat.Th a obtaine e n 198i dth n 3o 134, Average for region : 20,0t4,0 7.5+2,0 22,5+4,0 5,5t2,0 2,2 25,0+4,0 5,0i2,0 2,6 24,0t4,5 6,5ll,5 contents in the deep horizons of the Baltic Sea, on the 1 37 Central »-I9 20,0+4,0 8,0l2,0 I8,0t4,0 9,0t2,0 3,8 23,0±4,0 12,0+3,0 3,9 23,n+4.5 V,5ll,5 increased concentration f e increasso ^'Cs th d f ,an o e and Bestem »-20 21 ,0+4', 0 8,0+2,0 23,0±4,0 I3,0l3,0 4,6 24,0+4,0 9,0+2,0 4,6 22,0+4,0 12,0+2,0 salinity in most regions investigated, fully agree with the part •-2I 23,0t4',0 8,0^2,0 19,0+4,0 II,Ot2,0 4,9 22,0i4,0 9,D±2,0 4,8 I9,ni4-,0 9,0ll,5 «-23 20,0+4,0 I0,0t2,0 I9,0±4,0 I2,0±2,0 5,2 27,0+4,0 8,512,0 5,1 21,0+4,0 10,0+2,0 -information /-2-5/ and give -evidence, about the-penetration of »-25 I9,0t4,0 I2,0±4,0 25,0t4,0 0+2, 12 ,0 t,s 26, Ot4,0 7,5+2,0 the North Sea water masses beyond the limite of the Gottland Averagr fo e region : 21,0+4'n 9,0+2,0 21.0+4,0 11,0+2,0 4,6 24,0+4,0 9,0+2,0 4,6 21,0+4,0 S,5tl,5 north-eastere th dee n i p n direction. Pig Gul. 6 Finland.f fo . Salinity (o/oo), 9 °S137d rCan s activity concentratio nsurfacee (Bq/th t a m.) 1983.

distribution of salinity, Sr and Cs contents in the In the Gulf of Finland this correlation can be observed Gule v.-ater th Finlanf fo f o s n 1983i d watee .Th r salinity vere th y o ulowest p tcontens C salinit ^ td valuesyan . 137

e Gul ith nFinlanf f o d decreases from 5o1°/00 irwese jth o t Systematic observations are carried out in the region 13? the values less than 1.0°/0oin the east and Ce of the Leningrad KPP, in the Bay of Koporie. The water concentrations decrease frota 10.0 Bq/m to 2.0 Bq/m sampling is done in the points situated at different e flo Th fresf o w (fig . h6) . river waters with lov.- contents distances from the Leningrad KPP: from 1.0 km to 12.0 km. 137 of Cs and simultaneous inflov/ of the Korth Sea waters During the whole period of observations the region of the with high salinit d greaan y t concentratiof o n 137Cs have Bay of Eoporie doesn't differ by the contents of 90Sr and determined the correlation of 137Cs content and water 1 ^'C37 s in its water from the neighbouring regions of the 169 salinity, observe Baltie present a th a n i cSe dt (fig. .5) Gul Finlandf fo investigatioe .Th bioindicatorf o n s- I/O Table 4. Concentrations of Co and in the algae e suspendeth n i o TablC t . Concentrationpar5 e d tan a C f o s of Coporle Bay and in thé solution of the water of the Coporie Bay

Distance Sample Samplint w y dr g Concentration, Bq/kg (dr) ywt Distance Sample Sampling Sampling Concentration, Bq/nr fro- mLe date volume 1 , ———————————————— fro - mLe date frest hw ningrader ningrader

Cs Co Mn power sta- ^ Cs DU 60 54

power sta- 137 Co tionm ,k tion, km

1 Algae 16 .06 .82 0,12 22 54 12 2 suspendet 16.06.82 1250 0,6 o,5 green part solution 750 6,0 0,7 2 Aj.gae 16 .06 .82 0,16 19 36 14 5 suspendet 2 2318 19. .06 0 0,1 0,08 green part 2 Algae 16 .06.82 0,27 16 93 34 solution 2170 4,0 brown 5 suspendet 20. 06. 82 1720 0,1 0,07 part (Fucus) solution 1720 4,0

brown and green see-weeds - carried out in the Bay of Koporie in 1982 in the region from the Leningrad EPP to the distance 5.5 km demonstrated the presence of 13^'C7 s and neutron Tabl. e6 activation product then si m (tabl /14/) e4 observee .Ih d Concentration 9°Sf o s r (Bq/m3), 137Cs (Bq/m H (kBq/m3 watere d 3)th an f n 3o s)i leve bioindicatorf lo s contamination gives evidence abtmt the rivers flowing intBaltie oth froa cSe m USSR territory. normal operation of the NPP. In the same region of the Bay Name of I960 r. 1981 r. 1982 r I983 r. of Koporie experiments were don determination eo e th f no river July-August July-August June-July July-August

suspended matte waten ri r samples resulte tabln .I th 5 e s 137- 3 90 Sr 0 a r HS I37 H 3 > C* a r *>Sr^s IÎ7H 3 C I37 H 3 Ca are presente determinatiof o d f no e th n o o C d an 8

suspensions and in the solution /14/. !he obtained data Neva 20,0t4,0 I,5±I,0 6,7±2,I 24,014,0 I, 0+0;5 27,0tl,0 0,7tO,3 27,0t4,0<2,0 Narva 21,0+4,0 1,5+1,0 9,0+3,0 I9,0t3,0 I,0±0,5 20,0+4,0 0,?tO,3 I9,5t3,5 <2,0 give ground o suppost s sprean ca e o thadC bott h with 1 37 Luga I3.0+.3.0 I.5+.I.O 9,0+3,0 20,0t4,0 I,OtO,5 20,0+4,0 0,7tO,3 the suspended matter and in the water phase; Cs, by Pirita 11,0+3,0 I,5+J,0 I4£4,0 11,0+2,0 O^+O.'a II,Ot2,0 *2,0 the dat mainls solutione tablf i ao th , 5 en yi . Daugava 20,0+4,0 1,5+1,0 12+4,0 18,0+3,0 0,5±0,3 I9,0t3,0 0,7+0,3 I9,5±3,0 -2,0 Venta I5,0±3,0 0.5±0,3 I3+.4,0 I5,0t3,0 0,5±0,3 8,0t2,0 0,7±0,3 13,0+2,0 *2,0 Bar ta 7,0t2,0 0,5+0,3 I6t5,0 7,0+2,0 0,7+0,3 _ _ _ _ . Content3 f radionuclideo s e rivere wateth th f o n sri s Dane 7,0t2,0 0,5tO,3 21+5,0 Neman 10,0*2,0 0,5±0,3 20+6,0 8,0+2,0 0,5+0,3 9,0+2,0 0,7tO,3 7,0±I,5 ^2,0 inflowing "to the Baltic Sea from the territory of the USSR Pregol II,Ot3,0 0,5tO,3 6,0t2.6 I4,0t3,0 <2,0

Of) 1-37 -3 The results of Sr, ^ Cs andd ^ in the waters of Average I3,5±3,0 0,7±0,3 12,5+3,5 I7,0+>,0 0,7±0,3 I5,0t3,0 0,7tO,3 I6,0t3,0 rive rperioe mouthth r d fo s 1980-198 e give3ar tabln i n . 6 e The analysis of the obtained data shows that the water of especially in the Gulf of Finland. And, parallel with this, 1 37 the rivers contain much more Sr than Cs, because the the inflow of water from the North Sea increases ^ Cs globally fallen-out nuclideearte th hf washee o ar st ou d content in the Baltic Sea. surface differently morr S e: intensivel90 y. Cs tha ^ n 1 37 The contents of tritium in the river waters ranged s changine IC nth fig7 .d averagef o gan r S d 90 137 from 6.0 to 21.0 kBq/m , giving an average value 12.5 kBq/m, concentration watergroue e shows th si th f po f n so ni according to the data of 1980. This concentration is rivers under investigatio perioe th r d nfo sinc e 1974 till somewhat higher than in the waters of the Baltic Sea 1983. In general, a decrease of 90Sr content in the waters proper, t bu-enougno t h to--infl-uence -essentially tha- . of the rivers is going on, and 1 ^3 7Cs concentrations have tritium contenseae th . n ti decreased to such an extent that are practically not observed. remarkabla Thi s si e peculiarit radiatioe th f o y n situation in the Baltic Sea at present: the flow of river 137 Radionuclide. 4 s content bottoe th n mi s sediments waters containing minimal concentrations of Cs dilute Baltie th a f cSe o the concentratior of this nuclide in the Baltic Sea, The determination of radionuclides contents in bottom difficulf sedimento e on s ti scomplee taskth n si f xo "investigations of the radioactive contamination of the determinine Baltith f o ce SeaOn g. conditions it r sfo solutio obtainine th s representativa ni f go e methof o d 20 - sampling. Ground sampling either with the bottom suspension or withou wit r partiao s hit , it t l losessentialln ca s y influenc resulte th e . In 1982 a special ground-sampling device, enabling to takuppee th e r laye sedimentf ro s wit bottoe hth m water layer, developed and designed at V. G. Khlopin Radium Institutee Gule s th teste ,Finlanth f wa n fo i n i dd an d north-eastern part of the Baltic Sea proper. Table 7 summarizes the results of a layer-to-layer, eachm c, ,5 determinatio e bottoth f n o n^'Ci m ssediment s 137 Gule oBaltie th Finlanf f o th prope a d Se can dn 1982ri . $———j The obtained results showed that the main quantity of 1971 1975 1976 1977 1978 1979 1980 1981 1982 1983 ^ Cs of the layer 0-15 cm is concentrated in the upper •Pie. 7. 5 cm layer. It was of interest to consider the upper laye detailn ri . Therefor samplee th n ei s take n 198i n 3 "'Cd an sr S activit " y concentration rivere waten th i s f sro the uppe layem c s divider5 r wa d layersm intc 1 o d ,an 171 flowing intBaltie oth c froUSSRe mth . 1974-1983. each laye s analyserwa r fo d 1 J3 7Cs contents. The results Table 7 Contents of caeeiuiB-137 in the bottom sediments of the Gulf of 172 Finland and the Baltic Sea proper in- 1982 - 1983 .

:ra Index Sampling layer »eight Contenta of caeaium-137 of the of the region sampling sampling of of the Bq /aample Bq/kg (of the Bq/m2 (In the 2 dxiea sample cc sampling eanple dry »eight) given layer) (from) -to cm3 aacpla cm (in the 5 • given volume) _ go i 2 3 4 5 6 7 8 9 10 11

0 Gulf of July 56,70-1 56,7 30 2,4+0,3 80,0+15,0 425,0+65,0 Finland 1983 56,71-2 56,7 77 2 ..0+0, 3 21JJ+5.0 _ 360,0+55,0

56,7 2-3 56,7 78 5,5I1,5 75,0+10,0 56,7 3-4 56,7 55 0,3+0,1 5,2+1,5 50,0+8,0 56,7 4-5 56,7 60 0,4+0,1 710+i.O 75,0+10,0

In nil in the layer 0-5 985,0 0 2 • Gulf of July 56,70-1 56,7 35 1,7+0,3 40,0+7,0 300,0+45,0 Finland 1983 36,71-2 56,7 35 1,430,3 40,0+6,0 250,0+35,0 36,7 2-3 36,7 29 1,0+0,2 33,0+3,0 180,0+25,0 15 O 12 0 56,710 0 8 0 6 3- 0 44 0 2 36,0 7 0 8 0 6* 0 224 0 2 6 0,5+0,1 ' 0 8 0 6 5 0 4 0 24,0+7,2 0 0 8 0 0 6 0 4 93,0+20, 0 2 0 09 8 0 6 0 4 0 2 0 5», 7 4-5 56,7 34 0,8+0,2 23,0+7,0 135,0+20,0 oaeBlum-137, J)q/kg (dry weight) 0-5 960,u»140,0 56,7 5-10 283,5 200 0,55+0,1 3,0+1,0 105,0+15,0 Distribution of ^'Cs by the depth of the bottom sediments 56,7 10-15 2B3.5 175 0,55+0,1 3,U+1,0 90,0+15,0 in the Gulf of Finland and the Baltic Sea proper. layee th rn i l Inal 0-15 1155 . 8,. 4 Gul -2 f o Jun$ f e 3 56,7 0-3 2aj,5 133 6,0+1,0 43,0+6,0 1060,0+160,0 riiu.und 1982 56,7 5-10 283,5 183 0,9+0,2 5,0+1,0 160,0+24,0 e alss markear wa o t I presented . 2 fign i . n d tabli dan 1 e 56,7 10-1? 283,3 155 <0,3 <40 in three thus analysed samples that the upper layer 0-1 cm "-Ï1 7 7 "3 1 J layee th rn i l Inal 0-15 ~1250 contained the most quantity of ^'Cs. Cs concentrations, related to a unit of surface at the depth of layer 0-15 cm, 2 3- Balti4 c July 56,7 0-5 283,5 75 7,3+1,5 100,0+15,0 1320,0+150,0 Sea 198256,7 5-10 283,5 100 1,3+0,2 1Î,0+3,0 230,0+35,0 gave the values within the limits from 1160 Bq/m to O proper 56,7 10-15 283,5 130 *. 0,2 obtaine173e 0 Th . Bq/md numerout resultd no an e t sar sye layee th rn i l Inal 0-15 -1550,0 don't enable to make a quantitative evaluation of ^ Cs in the bottom sediments of a great sea aquatory-; they 5 g -46 Baltic July 56,7 0-1 56,7 14 1,7+0,3 120,0+20,0 300,0+45,0 Sea 198356,7 1-2 56,7 13 1,0+0,2 77,0+13,0 170,0+25,0 characterize only separate regions. 90 proper 56,7 2-3 56,7 15 1,0+0,2 67,0+10,0 170,0+25,0 Sr wasn't determined in the thus taken samples, 56,7 3-4 56,7 11 1,0+0,2 90,0+15,0 170,0+25,0 36,7 4-3 36,7 17 1,3+0,2 75,0+13,0 220,0+30,0 because the initial amount of the bottom sediments wasn't 0-5 1030,0 sufficien determinations it r tfo . Accordine th o t g 56,7 3-10 283,3 67 3,2+0,3 5Ç, 0+8,0 560,0+80,0 worbotton i contente kr th S /13m / sediment f o se th f o s 56,7 10-15 283,5 146 0,8+0,2 513+1,0 140,0+i:0,0 Baltic Sea is 60-80 times less than that of e layeth rn i l Ial n 0-15 1730,0 5. Radionuclides contents in the Baltic fish and sea-weedB Tattle 8. Concentrations of •? Sr and " Cs in eatable and uneatable parts of The determination of radionuclides in the Baltic fish the fishes of the Baltic Sea. 1980-1983. is carried out annually. Different species of fish from Concentration, Bq/kg (fres' h »eight) fishery catches (cod, sprat, smelt, pike-perch, plaice, Year Sea fieh Lake fish whitefish, scad) are used for analysis. During the whole eatable part uneatable part eatablo part uneatable part perio f observationf artificiao o d s C ld an s r onlS y 90 5°Sr 0B 9°Sr 370. 9°Sr '"c. sr '"a. radionuclides were found in the Baltic fish» In table 8 137 1 1980 0,1-0,4 1,2-2,2 0,1-0,2 I,,2-2,4 0,1-1,4 0,5-9,2 0,5-13,5 0,8-3,0 ther presentee ar e e averageth d d value f theso s e radio- 1981 0,17-0,36 0,4-2,04 0,5-2,25 3,2 0,07-7,7 0,24-3,21 0,22-0,39 2,5-4,2 nuclide d freeh-wates an content a se n i sr fish livinn gi 1982 0,1-0,5 0,5-2,3 0,5-1,- - - 8- 0,8-2,- - - 7- the Baltic Sea and caught, in 1980-1983» 1983 0,12-0,67 0,48-2,7 lïie comparison of the data presented in table 8 shows that the concentrations of Sr and ^ Cs in the Baltic fise onlar hy partweightt we unitr o se Bq/kf th ;o s f o g Tabl Baltie algae Concentration. th 9 e th f ceo n i Sea s .C ^ ^°Sf d o s ran

the contamination of fish with these radionuclides staying Serial Algae Sampling Sampling Concentration,? Bq/kg Ko. region date e samo th ne observatio th leve r fo l n period since 1980 fresh w. 83 -R3R, L.N., Vorobjeva H.H., Stepin A.A. Russian)n (i 1972 . Manifestatio influence th f no releasef eo artificiaf o s l . Truso2 v A.G., Ivanova L.MZolotukhin, . a V.C. p.nd long-lived radionuclides seen against the background of Gedeonov L.I. global radioactive contamination of the Atlantic ocean "Atomnaya Energiya", vol. 39, issue 3, pp. 177-182, and related seas. 1975 (in Russian). In: Impacts of Rsdionuclide Releases into the Marine 3. Vakulovsky 3.M., Katrich I.Yu., Malakhov S.G., Environment. Rosliy E.I., Chumiche Shkurd v an V.B. o V.N. IAEA-SI,'.-248/143, Vienna, 1981, p. 223-238. "Atomnaya Energiya", vol. 39, issue 3, pp. 183-185, 0. Vakulovsky S.M., Katrich I.Yu., Krasnopevzev Yu.V., 1975 (in Russian) . Mikitin A.I., Tertyshnik E.G., Chumiched v an V.B. . Gedeono4 v L.I., Ivanova L.lvî. Shkuro V.N. Investigation into migration of radioactive substan- "Okeanologiya", vol. 21, issue 2, pp. 257-265, 1981 ces in aqueous systems and assessment of radioactive (in Russian). contansinatio Baltie th n cni Sea. 10. Gedeonov L.I., Gusev D.I., Ivanova L.l,*., Kuznetzov J. Radiocheroistry, vol. 26, issue 1, pp. 81-86, 1984, Yu.V., Oleneva U.A., Orlova T.F.., Grishmanovsky V.l., Russian)n (i . Julikov E.I., Haritonova S.S., Pavlovsky O.A. 18. Lazarev L.N., Gedeonov 1.1., Ivanova L.15., Orlova T.E, Radioactive contamination of water systep.s having in- Stepanov An.VI. and Flegontov V.M. ternational significance. J.Radiochemistry, vol , . issu651p .26 , 5 e, 198n (i 4 International Conf. on Nuclear Power Experience. Russian). Vienna, 1982, IAEA-CN-42/352. . A.Aarkrog19 , L.B0tter-Jensen, H.Dahlgaard, Hansen, 11. Lazarev I.N., Gedecnov L.I., Ivanova L.U., Oleneva J.Lippert, S.P.Nielsen and Karen Nilsson. N.A., Orlova I.E.,Vakulovsky S.U., Nikitin A.I., Environmental Radioativity in Denmark in 1980. Chumichev V.B. Ris0-R-447, 1981. J.Radiochemistry, vol. 25, N 5, pp. 669-675, 1983 20. A.Aarkrog, L.B0tter-Jensen, H.Dahlgaard, Heinz Han- (in Russian). sen, J.lippert, S.P.Nielse Kared nan n Nilsson. 12.Vakulovsky S.U., Katrich I.Yu., Krasnopevzev Yu.V., Environmental Radioactivity in Denmark in 1981. Nikitin A,I., Chumichev V.B. Ris0-R-469, 1982. "Meteorolog Hydrology"d yan 72-78 . pp , ,9 ,198N 3 21. A.Aarkrog, L.B0tter-Jensen, H.Dahlgaard, Heinz Hansen, (in Russian). J.Lippert, S.P.Nielse Kared nan n Nilsson. 13. Vakulovsky S.M., Nikitin A.I. and Chumichev V.B. Environmental Radioactivity in Denmark in 1982. "Okeanologiya", vol984-987. issu, pp .23 , e6 , 1983 Ris0-R-487, 1983. (in Russian). 22. H.Kautsky. Vakulovsk. 14 y S.I.Ï Nikitid an . n A.I. Deutsche Hydrographische Zeitschrift, 34, 1981, Heft 4» "Atomnaya Energiya", vol. 153-155issu, pp 56 ., e3 , 1984 125-149. Russian)n (i . 23. H.Kautsky, H.-?. Eicke. 15. Gusev D.I., Gedeonosr L.I., Ivanova L.M., Stepanova Deutsche Hydrographische Zeitschrift, 35, 1982, Heft 5, V.D., Pavlovsky O.A. and Smirennaya V.A. 211-221. "The sanitary and ecological estimation of the.- radio- 24. Studie Environmentan o s l radioactivit n Finlanyi d 1981, active situation based on the results of the investiga- STL-A40, 1982, Helsinki. tions of the specialists of the USSR. 1976-1980." . Wojewodzk25 , PiechurT. i . Y a 2-Conferenca of countries-CMEA membea on the problem of Inflow of North Sc-o Waters in the Baltic Sea during Novem- the providing of radiation protection connect with the ber 1982 - may 1983. exploitation NPE. The theses of the reports.p. 93, C.I,!. 1983/c:6 Hydrography Committee. Vilnus, UJSH, 1982. 16. Gedeonov L.I., Blinov V.A., Tishkov V.P. In: "Environmental Surv. around Nucl. Installation", . 235-241pp vol , 1 . , 1974, IAEA, Vienna. 17. Blinov V.A., Gedeonov L.I., Tishkov B.P., Anisimov 175 V.V. 176 REPORT INTERCALIBRATIOF O N EXERCISES ORGANIZED FOR THE LABORATORIES PARTICIPATING IN THE IAEA'S CO-ORDINATED RESEARCH PROGRAMME "STUD RADIOACTIVF YO E MATERIAL BALTIE TH N SCI SEA" IN 1981-1984

. BOJANOWSKIR . FUKAIR , . BALLESTRAS , S VA . D , International Laborator f Marinyo e Radioactivity, Océanographie Museum, ANNEX 10 Monaco-Ville, Monaco INTERCALIBRATION REPORT

1. Historical Background

Following recommendations of the Technical Committee on the "Study of Radioactive Materials in the Baltic Sea" formulated at the meeting in Vienn Februarn i a yMonace th 1980,o Laborator s organizeha y numbea d f ro intercalibration exercise r participantfo s above th en i sCo-ordinate d Research Programme. The objectives of these exercises were to offer the laboratories a possibility of cross-checking their analytical results, to discove d eliminatan r e possible systematic o giverrordate t th ed a an s common bas n ordei e ensuro t r e their overall comparabilitys wa t I . recognized from the start that analytical quality assurance control would e indispensablb e Programmth o t e n ordei e o takt r e full advantage th f o e data accumulated through the concerted efforts of numerous participants over the 4—year research period.

The intercalibration programme was launched in late 1981 starting with a North Sea sediment sample (SD-N-1/1) which was sent to eleven laboratories in seven Baltic countries. By June 1982, five laboratories had returned the results which, together with data from two other reference laboratories (Livermoore and Monaco), were evaluated and reported at the first Co-ordinated Research Meeting in Vienna in July 1982.

This preliminary report was included as Annex 3 in the Report of Consultant e "Studth f Radioactivn o yo s e Material Baltie th n ci s Sea", prepared as a Working Paper by H. Kautsky and P.O. Agnedal in May 1982 (1). course Iintercalibratioe th n th f 198eo 2 s continuenwa d usinga seawater sample (SW-N-2). Thi collectes swa latn i d e 1981 froe th m surface of the North Sea by the staff of the German Hydrographie Institut Hamburn i e g unde supervisioe . Kautskth rH . d Dr yan f no 90 contained elevated concentrationf Srso , 13?cs, 238pu> 239+240pu and 24lAm. Thank rathea o st r long time analysise alloweth f o r fo l d ,al the eleven participants were abl submio t e t their results, althougt hno always for the full range of radionuclides. The most frequently measured sample SW-N-2 which were already partially published in preceding elements were 239+240pu an(j 13?cs (83% and 75% respectively), whereas the reports, were brought up-to-date by the inclusion of supplementary elements measure lease th d t often were 90sr, 238pu an(j 241^ (50% each). results and correction of a few misprints brought to our attention by the Results of this intercalibration were evaluated and communicated to the laboratories concerned. participant Novemben i s r 1983e reporTh . t appearee th Annes n a di x4 Report fro Technicaa m l Committee Meeting, Stockholm, 22-26 August 1983 Following past practic date e thos Tablen th ear i a e5 selectes2- d e "Studoth n f Radioactivo y e Material Baltie th n ci s Sea" issuen i d from individual reports with minor alterations comprising mainle th y December 1983 (2). removal of excessive digits, standardizing activity units and matching the activities to reference dates. The errors associated with individual y 198I nMa watea 3 se anothef ro samplet se r s collecteswa r fo d . values, however, were modified to a greater extent to make the data more intercalibration purposes. These samples, coded SW-B-1, were taken from comparable with one another. Thus a concept of overall uncertainty the surface of the Baltic Sea during the cruise of R/V "Gauss" and were rather than statistical counting error was adopted, in which both the sent to the laboratories concerned in June and July 1983 for 90sr, 137g counting erro1 sigm t a r probabla e th leve d lan e systematico t erro e du r s instrument calibration were taken into account by combining them in and transuranic measurements. In contrast to SW-N-2, SW-B-1 resembled quadrature. Whe mentioo n participant'a s mad n wa i e s e reporth f o t very closel n averaga y e sampl Baltif o e watera se cs n termit i , f o s concentratio f radionuclideo n d salinityan s , which enablee th d magnitude of systematic error, this was arbitrarily estimated at +5%, participant e theius o rt s original analytical procedures without which accordin r observationou o t g valu e th es i smos t frequently quoted alteration. in intercalibration exercises. It is evident that such treatment enlarges the uncertainty margin of the results, depending to some extent In the course of September 1983 all participants received a seaweed relative th n o e proportion kindo tw f errordoet so e i th st f ,bu so however makestimatios it e n more realistic. Whil mosr efo t environmental sample (AG-B-1) driewhica homogenized s an dhwa d brown alga Fucus vesiculosus collecte Augusn i d t 1982 frosouthwese th m t Baltic neae th r measurements random errors tend to be dominant, in some cases (such Swedish nuclear plant at Barseback. This material was expected to have a AG-B-e th d 6°C n an 1oi K samplea4° s accurace )resulte th th f s yo i s fairly high conten f 60co possibltd oan y other gamma emitting likel depeno t y d almost entirel amoune th f systematin o tyo co t erro e rdu instrument calibration. If this error is neglected the situation may radionuclides addition ,i norma e th o t ln rang f radioélémento e s measured arise that seemingly precise data lack coherence with one another within in previous intercalibration samples. the quoted uncertainty limits resulte Th . Tabln si whice3 h were intentionally left unchanged from the originals received from the At the CRM in Stockholm in August 1983 the participants were advised to proceed wite intercalibratioth h n measuremento t s a y n sucwa i s a h participants can be instructive in this respect. make the results available for evaluation by the end of March 1984. Practice showed, however, that the suggested deadline was difficult to 3. Discussion meet for certain laboratories. 'The situation as it stood in mid-May 1984 was described in the "Progress Report on Intercalibration" (3), a copy of 3.1 Identification of outlying data whic s sen eaco hwa t h participan e samth te month .missine th Mos f o tg data arrived shortly afterwards, finally yieldin vera g y satisfactory e principath Onf o e l objective e intercalibratioth f so n overall percentage of positive responses (94%). exercises was to check if the data produced within the Baltic Group are mutually consistent and can be regarded as belonging to the same The samples use n thesi d e intercalibration exercise e listesar n i d population. Several criteria have been proposerejectioe th r fo df no Table 1. They consist of samples specifically collected for the Baltic suspect values, none of which are fully satisfactory because of Programme (SW-B-1) as well as those which have either become reference various assumptions which must be made "a priori". To partially material (SD-N-1/1 e bein n ar simultaneousl ru gr ) o widen i y r overcome this problem we have recently adopted a nonparametric intercalibration programmmes differena e t lattea Th .e rar t stagf o e procedure develope modified Vegliy an b d ) Pszonicky (4 ab d . al t ie development, but the amount of data available so far enables some useful (5), which requires verpriow fe y r assumption bees ha n d founsan o t d comparisons with the data sets obtained within the Baltic group. be applicable to small (although not less than five) sets of data. Using this method we have tested all the data in Tables 2-5 and identifie possible th d e outlier asterisksy sb . Their numbers differ 2. Data Treatment depending on the radionuclide and the type of sample. Not surprisingly, the least number of outliers were found in the groups All data submitted by the participants over the whole study period of of radionuclides measured entirely or predominantly by gamma 1981-84 have been reviewed and rechecked before being compiled in spectrometry. For instance, the percentages of outliers in Tables 2-5. Analytical result lesr sfo s frequently measured nuclides measurements were 8%, 20%, 0% and 0% for samples SD-N-1/1, SW-N-2, were withheld if they were insufficient in number to produce any useful SW-B-1 and AG-B-1 respectively, which means that all or nearly all 111 intercomparisons date sedimenr Th .fo a t sample SD-N-1/ watea se rd 1an reported values were good. The results for other gamma emitters in 178

Table 1. Characteristics of intercalibration samples analyzed by laboratories participating in the Co-ordinated Research Programme "Radioactive Material Baltice th n i s" 1981-84.

Number of laboratories Principal „ Sample , . „ . . D.itc of Period of nuclldcs No. Cod„ Te Samplv e Origi° n collectio, , n uiterca. l tbratio. .. n. receiving the returning the sample results analyzed 60„ 90. 137„ 1 SD-N-1/1 Fine-grained sediment 1981 1981/84 12 s C 12 , Sr , Co from Scheldt estuary 238 239+240 (North Sea) PuD , PuD , 241 Am

90. 137 238 2 SW-N-2 Surfac watea se e r from 1981 1982/83 12 12 Sr, Cs, Pun , the North Sea (S = 35 %,) 239+240 241

90 137„ 238„ 3 SW-B-1 Surface sea water from 1983 1983/84 12 10 0 Sr, Cs, Pu, the Baltic Sea (S = 37.,) 239+240 241 Pu, Am

4 AC-B-1 Brown algae, Fucus vesiculosus 1982 1983/84 12 11 5V 6°Co. «Zn.

9°Sr, •''Cs, '"Cs137C ,

239+2400„pu>

Am Table 2. Results reporte e SD-N-1/th n o d 1 sediment e samplinterca1ibratioth n i e n exercis f radionuclido e e measurements by laboratories participating in the Co-ordinated Research Programme "Radioactive Material e Balticth n I s " 1981-84.

Radionuclide concentrations in mBq.g dry sample. Reference date 1 Jan. 1982

Lab. No. 90. 238„ 239*240„ 241 6°Co Sr 13?Cs Pu Pu Am

1 10.7 + 0.4 13 .3 + 0.6 0.1 0.0+ 9 2 0.53± °-03 0.5 0.0+ 7 3

2 11.0 + 1.1 0.61 * 0.03 11.8 + 0.9 *0.15 + 0.02 0.5+ 60.03 0.44 + 0.04

3 12.0 + 2 .7 <0.7 13.5 ± 0.7 0.1 0.0+ 9 3 0.58+ 0.07 - 4 11.4 + 8 5 1 .It *3.35 1. 3+ .5 + 3.7 a) *1.11 i °-19 _ *22 .2 + 2.2'b)

5 2 8. ^ 1 .6 1.26 + 0.31 11.1 + 1 .5 *3.26 ± °-82 -

6 11.5 t 2.6 1.48 + 1.70 12.6 + 1 .0 a) _ _ _ 13 ,u Ï 1 .5 b)

7 0 + 4 7. .6 14.0 + 0.8 0.2 0.0+ 0 3 *0.72 ± °-05 *0.30 + 0.06

8 13.1 + 7 .9 13 .3 + 1 .9 0.18 + 0.02 0.6+ 20.06 -

9 0 11.+ 8 .7 13 .7 + 0.7 *0.15 + 0.02 0.5± 1°-04 0.5 0.0+ 0 4 10 8.6 + 0.9 - - - - -

11 10.4 8^ .2 12 . 1 ± 1 .9 - - - 12 0.3 0.0+ 5 5 13 2 0.1 0.0+ 9 1 0.59 02 0.4 0.0+ 8 2 - - ± °-

Overall average 10.7 * 1.9 1.41 + 1.17 13 .8 •*- 2.7 0.1 0.08+ 2 0.94± °-89 0.4 0.1* 6 0 (18%) (837.) (207.) (117.) (947.) (227.)

Average after 10.7 + 1.9 0.92 * 0.53 13.1 + 1 .1 0.19 * 0.01 0.5± °7-04 0.50 + 0.05 rejectiof o n (187.) ( 587.) (97.) (47.) (77.) (117.) outliers

Notes ) 1 error: s Include both rando d systematian m c errors 2) asterisks mark the values which fell outside the accepted range 3) values marked uith a) and b) "ere obtained by beta counting and gamma spectromctry respectively

179 180

Tabl . 3 e Results reporte e SW-N-th a wate n se 2o d r e intercalibratiosamplth n i e . Result<, in s reporte e SW-B- th a wate n se o 1d r e intercalibratiosamplth n i e n e

exercise of radionuclide measurement Tab s by laboratories participating exercis f radionuclido e e measurement y laboratorieb s s participating in the Co-ordinated Research Programme " Radioactive Materials in e Co-ordinateith n d Research Programme "Radioactive Materiale th n i s the Baltic" 1981-84. Baltic" 1981-84.

Radionuclide concentrations in mBq.dm . Reference dat 1 Jane . 1982 Radionuclide concentrations in mBq dm . Reference date 1 Jan. 1984

. No Lab. 90Sr 137 238 239+240pu 241 Lab No. „ 90 137„ 239+240_ 241 CS Pu Ara u P s C Sr Am

135 9 109 + 7 1 28.9 + 0.3 171+1 33+5 ± 1 -25.8 + 1.3 16.0 +1.1 3.0+0.63 0. * 6 0. 120+20 2 + 0 12 2 + 9 2 2 * 5 3 159 + 5 2 '27+3 14.9 + 1 .4 5.0 + 2.0 2.1 + 1.2 1 + 6 2 3 165+1 29+7 1 + 0 11 100 +_ 10 3 7 0. + 6 4. 0 1. + 9 19.14.0. 2 9+ < 1 4 25.2 + 2.1 154 + 3 ^440 + 240 - 4 3 1. 9 + 16.19.0. 4 4+ - 5 *390 +28 280 + 60 - 5 6 1. + 18.6 - 6 21." + 0.6 7 15 + 7 0 *197 + 0 "410 + 150 - 6 9 0. + 17.13.7+0.3 8 - 7 180 + 20 110 +_ 50 34 ± 8 7 _ - 8 - 150+40 - 8 _ - 9 0 22+2 6 95 + IB 4 1 + 3 9 9 17.3+1.7 6.5+1.7 3.0 - 0.7 10 170-20 - - 10 16.0 + 2.6 - 11 26.7 + 4.1 156 + 8 - - 11 2 3. 5 + 14.17.2. 8 + 0 - 12 4 _ - 2 3 0 +1 0 16 0 1 + 0 12 100 + 10 12 2 1. + 6 2. 4 1. _ + 15.3 3 0. + 8 0.

204 + 128 Overall 4 6 + 26.9 5 3 + 2. 3 67 + 0 19 105 -. 10 Overall average 21.1+4.2 6 1. _ + 15.7+1. 3 4. 5 1 1. + 6 1. ave ge " (107.) (38%) (109%) (637.) (97.) (207.) (97.) (367.) (707.)

Average after 26.3 + 2.6 161+7 33+2 130+280 1 + 5 10 Average6 afte1. + r 3 4. 0 1. 5 + 18.15.1. 4 7+ 1.6 + 1.1 rejection of rejection of (47.) (7%) (227.) (97.) (67.) (97.) (367.) outliers outliers (707.)

-3 Notes ) 1 Plutoniu: d americiuan m m concentration e expressear s n pBq.di d m Notes) 1 Plutoniu: d americiuan m m concentration e m expressed ar s q pB n i d ) 2 Errors quote e laboratorie e thosth ar dy b e s 3) Outlying values are marked with an asterisk ) 2 Errors comprise bote countinth h g erro d incorcalioratioan r n error Table 5. Results reported on the AC-B-1 seaweed sample In the IntercalibratIon exercise of radionucllde measurement y laboratorieb s s participatin e Co-ordinateth n i g d Research Programme "Radioactive Material e Balticth n i s" 1981-84,

Radionuclide concentration mBq.y n samplei sdr g . Reference date 1 January 1984. Lab. No. 90. 134 7 239+240„ 241 4°K 54Mn 60Co 65Zn Sr Cs 13 ~Cs 238Pu Pu Ara

1 780+40 20.2+1.4 1400+70 37.9+2.9 11.5+0.7 3.2+0.7 16.7+1.3 7.5+^2 70+8 24+7 2 - 19.3+1.1 1403+70 48.7+2.8 2.4+0.4 17.U1.0 3+2 3 3U 70+5 3 - 20+5 1376+69 52+10 <5 21+6 <5 66+8 4 80U57 25.2+2.3 1372+77 - 9.8+1.0 21.0+1.) 5a - *97+3 26.1+2.3 b) 5 835+51 21.3+2.7 1365+80 24+4 3.5+1.3 16.8+2.6 *72+9 *155+17 6 ------7 767+45 25.6+4.3 1360+91 *97+ll <14 21.8+3.6 - - 8 - 14+3 1340+70 7 + 6 1 - 11+4 - *95+14

9 832+57 19+1 1390+74 36+2 3.4+0.4 15.9±1.3 - 52+9 13+3 10 *670+43 17+2 *1270+65 36+4 - 14+2 - - 11 868+79 22+6 1320+70 52 + 17 - 20+6 - -

12 - - - - 10.5+0.8 15.9±1.2 2.6+1.1 59+18 5.2+1.9

X 793+64 20.4+3.5 1360+41 44.4+23.2 10.6+0.9 3.1+0.5 18.1+4.0 21.3+33.9 83+33 18.3+11.5 (87.) (177.) (37.) (527.) (87.) (167.) (227.) (1597.) (407.) (637.)

*X 814+38 20.4+3.5 1376+21 37.8+13.1 10.6+0.9 3.1+0.5 18.1+4.0 4.4+2.7 63+8 18.3+11.5 (57.) (in) (27.) (297.) (87.) (167.) (227.) (62ï) (127.) (637.)

Notes: 1) errors include both random and systematic errors 2) X is the arithmetical mean of all results reported 3) *X is the arithmetical mean after removing outliers (marked with an asterisk) 4) plutonium and americium concentrations are expressed in pBq.g

181 seaweee th d18 sampl2 e AG-B-1 were equally good, wit houtlierf o onl % 7 y s The number of 90gr results available for evaluation was rather on average mosn I .t case magnitude sth departurf eo outlyine th f eo g modest, particularly for the seaweed and sediment samples. In the data from the mean concentrations calculated from the good values was latter group, which comprised six results (one of them from Monaco not tremendousl e totath l f y o n facnumbei hig t td ou hf an onl ro o tw y Laboratory), two values had to be excluded leaving the remaining four with a high variation coefficient of 58%. Only three strontium 64 gamma measurements may be causes for concern (i.e. 65zn in AG-B-1 by Lab. No. 7 and 137Cs in SW-N-2 by Lab. No. 5). results were available for the AG-B-1 sample which although very close together, are of little informative value to those who did not measur themselvest ei seawates a r fa rs A .sample e concernesar e th d The result transuranicn so s were, however ,littla e less situation looks better, but the appearance of two outliers among six satisfactory. The proportion of outliers in 239+240pu data ranged reported values for the SW-B-1 sample should be regarded as a warning from nil for sea water SW-B-1 to as much as 30% and 38% for sea water signal. SW-N- d seawee2an d AG-B-1 f thehighee o o factoa ar ml tw y Al . rb f ro or three compared wit average th h e values calculated froe th m e resultTh f testinso outlierr fo g e summarizesar Tabln i d . e6 accepted individual results. Ther fewee ear r outlier range th en si of 24lAm data but that is due to the fact that 24lAm values are normally less frequently reported numbee Th .valuef o r s availabls ei 2 Evaluatio3. intercalibratiof no n data often insufficien r applyintfo y rejectioan g n criterione th n o t ,bu other hand it must be recognized that the laboratories which have It can be seen from Tables 2-5 that after rejecting outliers the already gained experienc transuraniun ei m element measuremente sar comparabilit datf yo a improves considerably e coefficientTh . f so generally capable of producing results of high quality. The variation becom worse e th morr lowe o factoa t n i e3 y case rb f ro s proportion of such laboratories is at present rather low (four or e th r fa w sucho plutonius k ha as AG-B-e th w no n 1 i mn sampleca e On . inferree b f eleven o n fivt ca ou eds ) a frointercalibratioe th m n individual data are from what we accept as a reference value. The results and some effort toward raising it would be welcome. simplest and most straightforward answer to this question is to show the magnitud departurf eo singlf o e e values froe averagth m e value calculate datf o at dwhicse froe hth m passe e tesr outliersth dfo t .

Table 6. Proportion of outlying results in the dat

Sample 40,, 54., 60„ 65, 90„ 134„ 137. 1 24 239*242380 „ Code K Mn Co Zn Sr Cs Cs Pu Pu Am

SD-N-1/1 0/11 - 1/4 - 1/12 2/6 3/8 1/4

SW-N-2 - - - - 0/6 - 2/9 1/5 3/9 0/5

SW-B-1 - - - - 2/6 - 0/9 0/4

AG-B-1 1/7 0/10 1/10 1/9 - - 0/11 3/7

Notes : 1) numerator and denominator indicate the number of outliers and the total number of results considered

2) dash indicates no or insufficient data available for testing The results of this calculation are shown in Tables 7 and 8. They Precision of 90gr measurements in sediment sample SD-N-1/1 is indicate that for sea water the precision of measurements of 90Sr far from being satisfactory e valueTh . s reporte participante th y b d s and 137c s generallsi y satisfactorye th r fo lest ,bu o s varied by one order of magnitude and the resulting average value has transuranics. The difficulties in measuring very low levels of a good dea uncertaintyf o l neeA .improvo t d precisioe eth '^Sf no r plutoniu d americiuman reflectee ar m muca y hb d larger scattef o r measurement n sedimensi t sample obvious si f suce si b ho t date ar a results for SW-B-1 compared with the SW-N-2 sample. used for inventory studies. s transurania r Afa s c measurement concernee sar magnitude th d e Determinatio f radionuclideno n solii s d samples seem preseno t s t f scatteo r seem depeno t s d largelexperience th analyse n o yth f eo t no major difficulties in most cases. Although successful gamma and the quality of instrumentation with which laboratories are measurements depend largel concentrationn o y f radionuclideso n si equipped t shoulI . e realizedb d , however, that activity measurements samples e participantth , s were abl deteco t e d measurtan e activities l levelg~ q sanB t will alway subjece sb higa o t h degref o e as low as a few mBq/g with satisfactory precision using intact uncertainty. Considering all the difficulties associated with such samples. Compariso 137cf no s values measure gammy b d a spectrometry analyses, variation coefficient regardee b n ca s da % largs 50 sa s ea with those obtaine mory b d e laborious chemical procedure d betsan a acceptable. counting showed that thero significann s ei t differenc valuee th n ei s themselveassociatee th n i r so d errors.

Table 7. Departure of Individual radionuclidr measurements from the accepted average values (in 7.).

SW-N-2 SW-B-1 Lab. No. 238„ 1 239*24024 „ 90 137_ 1 239+24024 „ a Ar 9°Sr u P 137Cs u P P Sr Cs Pu Am

1 10 6 0 44 *40 2 -30 -63

2 10 -4 6 -8 14 *47 -5 16 31

3 -1 2 -12 -15 -5 4 -5 7 < -38

It -4 -4 *238 5 4 -

5 *142 *115 18 -

6 -17 -2 *476 *215 -6 -13 -

7 - 3 38 5 - -

8 - 15 - -

9 *40 -27 -11 10 51 88

10 5 - 2 -

11 2 -3 - -3 -11 -

12 5 - 8 - -1 3 - -3 -39 -50

183 Noteé valueth : s that fell outsid e acceptancth e e limit e marken asterisa ar s y b d k 184

Tabl . 8 e Departur f Individuao e l radlonuclidc measurements froe accepteth m d average valuen (I s

SD-N-1/1 AG-B-1 Lab. No. 90 137„ 238„ 1 24 239„ 40„ 54, 60„ 65 90„ 134 137 238 239 241 m A u P u P C os C C Sr s C Cs r S P un Z Po uC n AM m K

1 0 - 2 0 -7 14 -4-12083 -8 70 11 31

29 6 31 1 -3 42 -3 -10 6 - *-2 13 -2 - 2- -1 9 22 2 5 -

3 14 <-24 30 2 - -2 0 38 - <61 16 <14 5

4 10 *262 18 a) - *95 -2 24 0 - -8 - 16 a) - *54 *69 b) 44 b) 5 -24 37 -15 - *472 3 4 -1 -37 - 13 -7 *1536 *146

6 7 61 -4 a) - 2 b) 7 -31 - 7 - 5 0 2 *26 2 1 *4- 35 *150 5 - 2 7 -6

8 28 2-59- -31 -3 -58 - - -39 - *51

9 10 5 *-29 -2 1 7 -11-1 - 0 2 2-71--1 0 1 - 5

10 -20 _ *_18 -17 *-8 -5 - - -23 - -

11 1 8 - - - 7 8 -4 38 - - 10 - -

12 2 -7 - 6 - -62 1 -4 -1 2 -1 0 - 4 1 - -4 -

Note: the values that fell outside the acceptance limits are marked by an asterisk Table 9. Concentrations of less frequently reported radionuclides 3 Compariso3. n with other intercallbration data in the intercalibration samples.

The accuracy of analytical results obtained on the SD-N-1/1 Nuclide Lab . No . Activity e checkesamplb n ca ed directl y comparinb y g them witreference th h e Nuclide Lab .. No Activity values established for this sample through worldwide inter- calibration. These are the following: SD-N-1/1 mBq.g SW-N-2 raBq.dtr,"

2 435 + 22 3H 1 1900 + 260 Nuclide 60 90Sr 137 238Pu 239+240Pu A Co Cs °K 4 1 8 + 3 53 2 5 7 3 73 3 5 377 + 70 Md mBq.g-1 11.£ 0.72 14.0 0.18 0.56 0.49 6 520 7 20 99„ 9 5.1 t 0.2 7 422 7 19 Te - 10 3 0. + 6 377. 0 + 52 1 134 3 27 """ 9 S L Confidence 10.8-12.6 0.35-1.48 13.0-14.8 0.15-0.19 0.54-0.58 0.44-0.52 0 (16%7 + )3 44 Av = . limits 2 + 8 10 11 6.5 7 1.0 ( o= 0.05) 54 9 0.7 + 0.4 Mn 3.6 7 1.4 10 4 9 31.2268. 5 + KD3 ~~ This comparison indicates that except for three results for 60Co 21°Po 6 94 + 8 (Lab. Nos. 5, 7 and 10) and one 24lAm result (Lab. 1) all the data 9 2 2 + 5 15 SW-B-l which passed the rejection test are good, i.e., they fall within the 12 131 + 7 adopted confidence limits. In addition, two 238pu values which were 6 0 63090 0+ H 3 earlier considere outliers a d welt sfi l (Labw no ) .9 Nosd an .2 226 2 114 + 8 withi n thue range concludeca e th nb s t I . d tharesulte th t s obtained i\ a 4 1 1 7 07 Baltie bth y c countrie sedimene th n so t sample SD-N-1/ e fre1ar e from 226. 12 2.3 + 0.2 any significant systematic error and can be deemed accurate. 6 2 + 8 6 Ra — 7 63 7 7 9 107 7 1 Although the worldwide intercalibration exercises on samples AG-B-1 raBq g" finishedt ye SW-N- t AG-B-d no 2an ,e sufficiena 1ar t numbef ro 12 107 7 7 results are already available for most radionuclides to make the 58 2 Co 2 <1.5 comparison usefulabsence th n establishef I eo . d reference data 228 32 + 3 Ra 9 4 2+ 6 3 < 5 compariso respective th f o n e group measurementf so eacr sfo h element 4 1 < 7 seems appropriate e questioTh . answeo date t n th a whethes t ri no r o r 2 27 + 2 9 1.2 + 0.2 sets from the Baltic countries differ significantly from those 228Th 11 <7.8 acquired from other laboratories participating in worldwide A 31 + 9 6 4 297 99 Intercalibrations appln nonparametrica r e thi Fo th ye .sw c 1 2 14.T0. e 7+ Wilcoxon-Mann-Whitney test, whic s distributioi h n o freetw o t , 7 38 7 4 9 9 5 11.0. 47 independent sample sets. The test results on the SW-N-2 sample have 1 *1 37 12 5 11.1. 17 shown that thero statisticalln s ei y significant difference th t ea 12 2 29+ nuclidee th f o significanc sl al excep r fo t 1 90sre0. e leveTh = . t lc Av. =31+4 (147.) average strontium concentration is higher in the Baltic group compared to the remaining group of results. Considering the higher 5 5 + 6 2 232Th number of samples in the Baltic group and their lower dispersion, it In 7 2 + 8 2 can be safely assumed that they are closer to the true value. 9 2 1+ 2 12 2 297 Only gamma emitters were AG-B-e testeth n 1i d e samplth s ea

numbe f dato r othe fo a r radionuclide eithen i sw lo ro to grou s pwa 0-10 238U 2 6 3 + 6 9 for suc a htrial e tesTh .t demonstrate l thesdal thaer fo nuclidet s 5 64 7 6 there is no significant difference between the averages and there is 9 16 7 1 no reason to believe that the data do not belong to the same 12 2 297 185 population. List of Institutions . 4 Othe186 r Data Participating in Intercalibration Exercises withi Framewore th nBaltie th P f cCR ko Several participants reported result r othesfo r radionucliden si 1981-84 additions to those listed in Tables 2-5. These were however not numerous enougmeaningfua usee b n i do t h l evaluatio purpose th r thif nfo eo s report. Mos f theso t e data will certainl utilizee yb worldwide th n i d e Institution Investigator intercalibratio latea t na r date, when more similar measurements become available. Thos somf o eee b whicinteres y analyste hma th o t e sar Ris0 National Laboratory Aarkro. A g liste Tabln i d . 9 e Roskilde

Finland Institute of Radiation A. Salo Protection, Helsinki T. Taipale REFERENCES Sinkk. K o J. Ojala R. Saxen 1. Evaluation of Results of the Intercalibration Exercise of T. Tuomainen Radionuclide Measurements on the Sediment SD-N-1 and the Flans for the Future Intercalibration (June 1982) : ReporIn . Consultantf o t s German Democratic National Board of Nuclear F. Moldenhawer "Stude th Radioactivf n yo o e Material Baltie th n csi Sea" y (3-Ma 6 Republic Safet Radiatiod yan n Thiel. J e 1983) Kautsk. ,H P.Od .yan Agnedal (eds.). ,pp Anne6 , x3 Protection, Berlin D. Weiss

. Intercalibratioe 2 Reporth f o t Radionuclidf no e Measurementa Se n so Germany, Federal German Hydrographie H. Kautsky Water Sample Framewore SW-H- th IAEe n th 2i A f Co-ordinateko d Republic of Institute, Hamburg H.F. Eicke Research Programme, "Study of Radioactive Materials in the Baltic P. Bergheim Sea". In: Report from a Technical Committee Meeting, Stockholm, M. Domian 22-26 August 1983 on the "Study of Radioactive Materials in the Goronc. I y Baltic Sea". , pp Anne8 , x4 Norway Institut Energr fo e y G.C. Christensen 3. Progress Report on the Intercalibration of Radionuclide Measurements Technology, Kjeller . SaetyA r n Sampleo Marinf o s e Origi Participanty nb e IAEA'th f so Co-ordinated Research Programme, "Stud Radioactivf o y e Materialn si Poland Central Laboratorr fo y Baransk. A i the Baltic Sea", 31.20.04. pp 1984y 8 ,Ma , Radiological Protection J. Tomczak Warsaw 4. Veglia, A., A Nonparametric Statistical Method for the Determination oConfidenca f f Resulto t eSe sIntervaMeaa e obtaineth f no r fo ln i d Sweden Studsvik Energiteknik AB P.O. Agnedal Laboratora y Intercomparison, IAEA/RL/84, Augus. pp t 7 19811 , Nykoping

5. Pszonicki, L., A.N. Hanna and 0. Suschny, Report on Intercomparison National Institution of R. Böge V-9 of the Determination of Trace Elements in Cotton Cellulose, Radiation Protection J. Suomela IAEA/RL/97, March 1983, 23 pp. Stockholm M. Elbe

6. Natrella, M.G., Experimental Statistics, National Bureau of Standards Radiation Physics Department E. Holm Handboo U.S, .91 k Govt. Printing Office, Washington, U.C., August Lund University, Lund 1963. The National Swedish Environment M. Hotter Protection Board, Drottningholm Neuman. G n

USSR Khlopin Radium Institute I.M. Ivanova Leningrad

Monaco International Laboratory of S. Ballestra Marine Radioactivity R. Bojanowski IAEA, Monaco D. Vas LIS MEETINGF TO PARTICIPANTD SAN S 10. Mr.J. Kovacs International Atomic Energy Agency (Scientific Secretary) Wagramerstrasse 5 P.O.Box 1OO, A-1400 Vienna, Austria I. Technical Committee on the "Co-operative Programme on the Study of Radioactive Materials in the Baltic Sea" (11-14 February 1980, IAEA, Headquarters, Vienna, Austria).

1. Mr.A. Aarkrog Riso National Laboratory II. First Research Coordination Meeting on the "Study of Radioactive DK-4000 Roskilde Material Baltie th n i sc Sea" (5-9 July 1982, IAEA Headquarters, Denmark Vienna, Austria).

2. Ms. A. Salo Institute of Radiation Protection 1. Mr.A. Aarkrog Riso National Laboratory, F-00101 Helsink P.O.Bo, 10 i 8 26 x DK-4000 Roskilde, Finland Denmark

3. Mr.A. Voipio Finnish Institute of ilarine 2. Ms.A, Salo Institute of Radiation Protection, (Chairman) Research P.O.Box 268, F-00101 Helsinki, Asiakkaankat A P.O.Bo u3 3 3 x Finland SF-0093I, Helsink Finlan, i93 d 3. Mr.F, Moldenhawer National Boar f Nucleado r Safety 4. Mr.F. Moldenhawer National Boar r Nucleafo d r and Radiation Protectioe th f no Safet d Radiatioan y n Protection GDR, Waldow-Allee 117, of the GDR, Waldow-Allee 117 DDR-115 Berlin BerlinH GD , GDR 5. Mr.H. Kautsky Deutsches Hydrographisches 4. Mr.H. Kautsky Deutsches Hydrographisches Institut Institut, Postfach 220 Postfach 220 D-2000 Hambur, 4 g D-2000 Hamburg 4 FRG FRG . 5 Mr.G.C. Christensen Institut r Energefo y Technology, 6. Ms.K. Gaarder Institut r Atomiefo c Energy Box 40, N-2007 Kjellor IM-2007 Kjeller, P.O.Box 40 Norway Norway . 6 Mr.A. Baranski Central Laboratory for . 7 Mr.Z. Jaworowski Central Laboratory for Radiological Protection, Radiological Protection Konwaliowa 7 Warsaw 03-194 Poland Konvraliowa 7 . 7 Mr.P.O. Agnedal Studsuik Energiteknik AB Poland S-611 82 Nyköping 8. Mr. Per-Olof Agnedal Studsi/ik Energiteknik AB Sweden S-611 82 Nyköping Sweden . 8 Mr.R. Böge National Institut f Radiatioo e n Protection, S-104 01 Stockholm (Chairman) 9. Mr.R. Böge National Institute of Sweden Radiation Protection S-104 01 Stockholm . 9 Mr.E. Holm Radiation Physics Department, Sweden Lund University, Lasarettet, S-22 15 Lun8 d Sweden 187 10 Ms M Nottor The National Swedish Environment A Baransk r M i9 Central Laboratory for Protection Board, Research Radiological Protection laboratory, S-l/ Drottningholm01 1 , Konwaljowa 7 Warsaw 03-194 Poland M IvanovL s M 1a1 Khlopin Rwdium Institute, Roentgenst 1 19/07r ? Leningrad 10 Mr P 0 Agnedal Studsvik EnergitekniB fl k UGGR S-611 82 Nykoping Sweden J Kovac r M s 2 1 International Atomic Energy Agency, Wagramerstrasse 5, 11 Mr R Böge National Institute of Radiation (Sciemific 3eore:a-y) P 0 Box 100, fl-1400 Vienna, (Chairman) Protection Austria Box 60204 S-10 1 Stockhol0 4 m Sweden

12 Mr E Holm Radiation Physics DpparLment Lund University I abdrettot, S-27 5 Lun8 1 d Sweden III Technical Committee on the Study of Radioactive Materials in the Baltic Sea 13 Ms M Notter The National Swedish Environment (22-26 August 1983, Stockholm, Sweden) Protection Board, S-1l 7Oi Drottingholm A Aarkro r M g 1 Riso National Laboratory Sweden DK-4000 Roskilde, Denmark M IvanovL s M a 4 1 Khlopin Radium Institute, Roentgenstr 1 2 Ms A Salo Institut f Radiatioo e n Protection 197022 Leningrad E Jlu r M s 3 P 0 Box 268 USSR SF-00101 Helsinki Finland 15 Mr R Bojanowski International Laborator Marinf o y e Radioactivity F Moldenhauie r M 4 r National Board of Nuclear Safety Océanographie Museum D Weis r M s 5 and Radiation Protection Monaco-Ville Waldoui-Allee 117 Principalit Monacf o y o DDR-115 Berlin GDR V Aleiruko r M 6 1 v International Atomic Energy Agency (Scientific Secretary) Wagramerstrasse 5 Mr H Kautsky Deutsches Hydrographisches P O Box 100 Institut, Postfac0 27 h A-1400 Vienna, D-2000 Hamburg 4 Austria FRG

J Kovac r M s Hungarian National Atomic Energy Commission 1374 Budapest 5, Pf 565 IV Final Research Co-ordination Meetine Studth f Radioactivo n y o g e Hungary Septembe8 2 Material 4 e Balti(2 th a rn Se i cs1984 , Helsinki, Finland)

Mr G C Christensen Institute for Energy Technology, Mr A Aarkrog Riso National Laboratory Box 40, N-2007 Kjellor 9 4 x Bo 0 P Norway DK-4000 Roskilde Denmark 2 Ms A Salo Finnish Centre for Radiation and M IvanovL s M 1a3 Khlopin Radium Institute 3 Mr E Jlus Nuclea8 r26 x SafetyBo 0 P , Roentgenstr 1 SF-00101 Hplsmki 10 197072 Leningrad Finland USSR

4 Mr A Voipio '"iT'ish Inbt.tut f iXnno e e F Khoklou D s M a 4 1 State Committee for Utiliration of Research Atomic Energy Asia'ticaankat F.u.BoA 3 u 3 3 x Moscow 3F-C093I, Helsinki 93, 'nla'd USSR D WQIS r M S 5 National Board of Nuclear Safety R Bojanowsk r M 5 1 i International Laboratory of and Radiation Protection 16 Mr E Holm Marine Radioactivity Waldow-Allee 117 Océanographie Muspum DDR-1557 Berlin Monaco-Ville GDR Principalit f Monaco y o

H Kautskr M y 6 Deutsches Hydrographisches 17 Mr H Veiner Baltic Marine Environment Institut, Postfach 220 Protection Commission D-2000 Hambur4 g Etelaesplanad3 4 C 22 i FRG SF-00130 Helsink3 i Finland C Christense G Mr 7 n Institu r Energfo t y Technology P 0 Box 40 E Aleiniko V r M u8 1 International Atomic Energy PJ-2007 Kjeller (Scientific Secretary) Agency Norway Wagramerstrass5 e 0 10 x Bo 0 P 8 Mr Z Jaworowski Central Laboratorr fo y A-1400 Vienna Radiological Protection Austria Konwaliowa 7 Warsaw 03-194 Poland

9 Mr R Böge National Institu f Radiatioo e n (Chairman) Protection P 0 Box G0204 S-104 01 Stockholm Sweden

10 Mr P 0 Agnedal Studsvik EnergitekniB A k S-611 8? Wykoping Sweden

M Noties M 11 r e NutiondTh l Swedish Environment Protection Board S-17011 Drottingholm

12 Mr Ch Samuelsion Lund University Lasarettet S-22185 Lund Sweden 189