Geological Survey of Finland Current Research 2001-2002

Geological Survey of Finland, Special Paper 36

edited by Sini Autio

Geological Survey of Finland Espoo 2003 Autio, Sini (ed.) 2003. Geological Survey of Finland, Current Research 2001-2002. Geological Survey of Finland, Special Paper 36, 97 pages, 34 figures and 14 tables. The publication contains 10 articles outlining the current research at the Geological Survey of Finland (GTK). The articles are divided into 3 categories. At the end of the publication there is a list of publications by GTK staff in 2001 and 2002. An article in industrial mineral potential in Finland presents the high rate of the occurrence of the deposits. A scetch map shows the most promising exploration areas. The origin of the Petäiskoski carbonate veins at Juuka, eastern Finland has been studied to be associated with Svecofennian orogeny. Combined isotopic data indicate a hydrothermal process for the veins. Comparision on mechanical sieve size analyses and digital size analyses of Kemi chromite shows good correlation so, that size analysis of the ore using image manipulation can be used to predict ore breakage and mineral liberations can be obtained at certain grinds. Estimation of ferric iron, crystal water and calculation of chemical formulae for altered ilmenite from electron microprobe analyses, based on stoichiometric criteria. Silvery greyish nuggets from Ivalojoki placers, Finnish Lapland are interpreted as amalgamated gold nuggets resulting from historical gold recovery operations that utilized mercury. The store and long-term accumulation of iron, phosphorus and nitrogen in Finnish lake sediments are presented. The results of the Barents Ecogeochemistry project show, that local basic geology has a strong influence in element distribution in stream waters and in certain mosses. The inverse relationship between acute myocardial infarction (AMI) and total hardness of ground water is reconfirmed. Heavy metal enrichment factors for different analytical methods are studied and the results are compared. A case study on an ice-marginal deposit by airborne electromagnetic measurements is presented.

Key words (GeoRef Thesaurus, AGI): Geological Survey of Finland, current research, programs, bibliography, Finland

Sini Autio Geological Survey of Finland P.O. Box 96 FIN-02151 ESPOO, FINLAND

E-mail: [email protected]

ISBN 951-690-861-6 ISSN 0782-8535

Vammalan Kirjapaino Oy 2003 Geological Survey of Finland, Current Research 2001-2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 2003.

CONTENTS

Preface ...... 4

Mineral exploration and economic geology

Industrial mineral potential in Finland, Olli Sarapää, Timo Ahtola, Jukka Reinikainen and Hannu Seppänen ...... 5

The Petäiskoski carbonate veins at Juuka, eastern Finland, Matti Tyni, Kauko Puustinen, Juha Karhu and Matti Vaasjoki ...... 13

Direct comparison on mechanical and digital size analyses of Kemi chromite, Finland Tegist Chernet and Jukka Marmo ...... 17

Estimation of ferric iron, crystal water and calculation of chemical formulae for altered ilmenite from electron microprobe analyses, based on stoichiometric criteria, Tegist Chernet and Lassi Pakkanen...... 23

Mercury-rich coating on some gold nuggets from Ivalojoki placers, northern Finland, Kari A. Kinnunen ...... 29

Environmental studies and geochemical applications

Iron, phosphorus and nitrogen in Finnish lake sediments: their store and long-term accumulation, Hannu Pajunen and Jari Mäkinen...... 35

Barents Ecogeochemistry - a large geochemical baseline study of heavy metals and other elements in surficial deposits, NW-Russia and Finland, R. Salminen, I. Bogatyrev, V. Chekushin, S. P. Glavatskikh, V. Gregorauskiene, L. Selenok, M. Tenhola and O. Tomilina ...... 45

Geochemistry of local ground water in relation to the incidence of chronic diseases, Anne Kousa and Maria Nikkarinen ...... 53

Heavy metal enrichment factors for different analytical methods, Timo Tarvainen and Philipp Schmidt-Thomé ...... 61

Geophysical applications

Survey of a buried ice-marginal deposit by airborne EM measurements – A case from Kyrönjoki valley plain in southern Ostrobothnia, Finland, P.Lintinen, I. Suppala, H. Vanhala and M. Eklund ...... 67

Publications

Papers published by Geological Survey of Finland staff in 2001-2002 ...... 77 Geological Survey of Finland, Special Paper 36 MattiSini Autio Tyni, Kauko(ed.) Puustinen, Juha Karhu and Matti Vaasjoki

PREFACE

The Geological Survey of Finland - GTK - performs its prime task by producing information to create conditions for sustainable raw materials supply and land use. GTK secures the mineral raw materials of the country with special reference to the constructing industry by indicating occurrences of industrial minerals and natural stones, as well as sand and gravel resources. The present Special Paper, for example, outlines the industrial-mineral potential of Finland and presents new geophysical methods for locating hiddenRaimo sand-gravel Matikainen deposits. Increasing attention is paid to environmental studies with specialDirector reference General to geochemistry. GTK has been pioneer in regional geochemical studies and now plays a major role in genuine international cooperation in this field. An excellent example is given in the paper outlining results of the Barents Ecogeochemistry project, which is a large environmental baseline study of Northwest Europe extending from Finland to the Urals. Geochemistry of lake sediments in Finland and the Baltic Soil Survey project are presented. Geomedical applications of regional geochemical data explore new frontiers of geoscience by looking for the cause of chronic diseases in the geochemical features of the bedrock. This new Special Paper demonstrates that our research serves the society. Geoscience is changing by diversification and new applications, and GTK follows this trend being an active factor in service of society. Our publication record demonstrates that, besides massive data collection, GTK aims at innovative and high-level research.

Professor Raimo Matikainen Director General

4 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 5– 12 , 2003.

INDUSTRIAL MINERAL POTENTIAL IN FINLAND

by Olli Sarapää, Timo Ahtola, Jukka Reinikainen and Hannu Seppänen

Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): industrial minerals, mineral exploration, potential deposits, titanium ores, ilmenite, marble deposits, resources, Kairineva, Kuovila, Hakala, Finland

Introduction pegmatites.

During the last five years the Geological Survey of Industrial mineral potential in Finland Finland (GTK) has investigated industrial minerals, targeting in particular carbonate rocks in SW-Finland Finland has a high potential for the occurrence of and ilmenite in western Finland. In 2001, the report of industrial mineral deposits. This is indicated by sixteen four industrial mineral deposits (Sarapää et al. 1999a, marble, ten industrial mineral and six industrial rock 2001): Hyypiämäki calcite, Iso-Sorro calcite-dolo- deposits that are currently in production. During last mite, Illo calcite deposit and the Peräneva ilmenite five years, GTK has located and studied twenty deposit were submitted to the Ministry of Trade and industrial mineral deposits in southern Finland by Industry (KTM). Already in 2000, KTM sold the claim mapping and drilling. Eleven of them, nine marble and rights of the Järvenkylä calcite deposit to Nordkalk two ilmenite deposits are economically interesting and Co. and in 2002 Omya Oy acquired the rights of the six of them have been sold to domestic and interna- Hyypiämäki and Nordkalk Co those of the Iso-Sorro tional industrial mineral enterprises (Table 1). deposit. The Norrlammala calcite marble deposit at The industrial mineral potential map of Finland Kemiö, owned by Omya Oy, is at present under shows the most promising exploration areas for indus- evaluation for quarrying as an open-pit mine. trial minerals (Fig. 2). They include paper pigment By the end of 2002, the three economically interest- minerals, rare elements and fertilizer minerals (apa- ing industrial mineral deposits of Kairineva ilmenite, tite, dolomite). High quality calcite marble deposits Kuovila calcite-wollastonite and Hakala calcite were are found to occur adjacent to metavolcanic rocks in reported to the Ministry of Trade and Industry. The Finland and they are generally intensively folded and Peräneva and Kairineva ilmenite deposits were sold to metamorphosed to high-grade (Reinikainen 2001). In the Kalvinit Oy. GTK’s drilling program in 2002 western Finland there are small ilmenite-apatite-gabbro covered the Mäntsälä (Kalkkisaari), Salmijärvi and and ilmenite-gabbro bodies, for example at Koivu- Nummi-Pusula deposits for calcite and wollastonite saarenneva, that contain a lot of magmatic ilmenite and the Iso-Kisko deposit for ilmenite (Fig. 1). A and ilmeno-magnetite is rare. (Kärkkäinen 1999). newly defined exploration project, “The studies of Therefore they seem to be good raw material for

Industrial minerals in south and west Finland” begins TiO2-pigment production (Kärkkäinen at al. 1997). in 2003. Apart from the paper pigments minerals, it The rare elements in granitic pegmatites are seen as covers the rare elements (Ta, Be, Nb, Li) in granitic several zones in Finland (Alviola et al. 1989, Alviola et

5 Geological Survey of Finland, Special Paper 36 Olli Sarapää, Timo Ahtola, Jukka Reinikainen and Hannu Seppänen

Fig. 1. Location of the studied marble deposits and marble mines in southwest Finland on a geological map. al. 2001, Mäkitie et al. 2001). The potential for kaolin at present owned by Kalvinit Oy. and talc deposits (Pekkala & Niemelä 1997, Niemelä The Kairineva deposit was located by systematic 2001) is the highest in mid-eastern (Sarapää 1996, ground geophysics (gravity high, magnetic high, and 1997, 1999, Sarapää et al. 1996) and northern Finland reverse electromagnetic anomaly) and by drilling. It is (Pekkala & Sarapää 1989, Lintinen 2000) and possible a magmatic titanium ore deposit in Svecofennian in mid-west Finland as well. The latter is based on the mafic intrusion. Layered mafic intrusions (1881 Ma) new interpretation of the low-altitude geophysics and with ilmenite ores and magmatic stratigraphy were ground gravimetric measurements. emplaced into granitoids at the contact zone of the Central Finland Granitoid Complex (Kärkkäinen 1999, Kairineva ilmenite deposit in mid-west Kärkkäinen & Sarapää 2002). The Kairineva deposit Finland is a vertical and folded sheet that is composed of strongly disseminated and massive oxide ore bodies GTK discovered and explored the Kairineva ilmenite within the gabbro. The length of deposit is 400 metres deposit during 2000-2001. The aim of the study was to and it is 50 metres wide. The total indicated resources are 5.4 Mt with the average grade of 20wt% ilmenite find raw material for the domestic TiO2-pigment industry. The Ministry of Trade and Industry released and 9% magnetite. The estimate extends down to 75 in 2002 an International Tender Notice to awaken metres from the surface. Based on the gravity studies companies’ interest for further exploration of the the ilmenite rich units continue at least to the depth of Kairineva deposit. The deposit is located at Halsua 170 m, and accordingly the inferred resources are 10 three kilometres southwest of the Peräneva deposit million tons. Based on a gravity estimate the inferred and five kilometres southwest of the Koivusaarenneva resources of the Kairineva deposit are 40 Mt. deposit (Fig. 3). Claim rights of those two deposits are Ilmenite and magnetite at Kairineva occur as indi-

6 Geological Survey of Finland, Special Paper 36 Industrial mineral potential in Finland

Fig. 2. Map of industrial mineral potential in Finland.

vidual grains (Fig. 4), but ilmeno-magnetite grains are Koivusaarenneva and Peräneva, which means that rare. Magnesium and chromium contents in ilmenite ilmenite concentrate of commercial quality can be are very low, as well as vanadium and niobium (Table produced by using traditional beneficiation methods. 2). Magnetite contains 0.86% vanadium, which is The Kälviä-Halsua area seems to have an excellent higher than that of the magnetite of the Otanmäki Ti- potential for gabbro-hosted ilmenite deposits of high Fe-V-ore. The mineralogy and structure of the quality ilmenite. The demand of ilmenite concentrate Kairineva ilmenite ore is similar to that of in Finland is growing because Kemira Pigments Co.

7 Geological Survey of Finland, Special Paper 36 Olli Sarapää, Timo Ahtola, Jukka Reinikainen and Hannu Seppänen

Table 1. Mineral resources of the studied marble deposits in southern Finland.

Deposit Resources/ Ore content ISO-Brightness Current stage Owner depth <20 µm

Norrlammala Under evaluation Omya Oy Calcite marble 7.1 Mt/75 m 78.2% calcite 91.5-92.1% for open-pit mine

Genböle GTK Calcite marble 5.3Mt/100m 87.1% calcite 90.0-91.7%

Illo Open for tender GTK Calcite marble 5.8Mt/80m 77.4% calcite 89.5-95% 9.4Mt/120m -"- 12.9Mt/160m -"-

Järvenkylä Calcite marble 1.9 Mt/75 m 80.3% calcite 91.2-94.7% Nordkalk Co. 3.2Mt/125m 82.4% calcite 7.7Mt/300m -“-

Kalkkimäki Open for tender GTK Calcite marble 2.0Mt/75m 81.6% calcite 91.1-92.9% in 2003 Calc-dolo marble 3.7Mt /75m 70.1% carbonate 88.2-90.4% Woll-calc marble 2.0Mt/75m 14.7% wollastonite 57.5% calcite

Iso-Sorro Nordkalk Co. Calcite marble 2 Mt/ 75 m 70% calcite 91.3-92.1% Dolomite marble 6 Mt/100 m 55% dolomite, 30% calcite

Hyypiämäki Calcite marble 17Mt/100 m 76% calcite 90.4-94.2 % Feasibility studies Omya Oy or 7.2 Mt 86.7 % calcite

Kuovila Open for tender GTK Calcite marble 39Mt/125 m 75% calcite 90.4-95.9% in 2003 or 20.2 Mt 81.8 % calcite Woll-calc marble 9 Mt/125 m 54% calcite, 15% wollastonite

Hakala Open for tender GTK Calcite marble 1.3 Mt/125 m 84% Calcite 94.5-94.8% in 2003

Fig. 3. The ilmenite deposits (black) of the Kälviä-Halsua area on the gravity and ground magnetic map.

8 Geological Survey of Finland, Special Paper 36 Industrial mineral potential in Finland

Fig. 4. Ilmenite from the Kairineva deposit, DH 503, 15.10 m, on polished slab (left) and microphotograph (right), in which oxide minerals are grey and silicate minerals black, scale bar 0.5 mm.

Table 2. Chemical composition of the Kairineva Kuovila calcite-wollastonite marble deposit ilmenite by microprobe analysis.

N Minimum Maximum Mean GTK explored the Kuovila calcite-wollastonite marble deposit in the years 1999-2002 for its suitability TiO 24 48.36 50.46 49.45 2 as a raw material for paper pigment. The deposit has FeOtot 24 46.11 48.39 47.14 MnO 24 .73 .88 .80 been quarried as a small scale open-pit mine in the MgO 24 .02 .20 .08 Cr 24 .00 .02 .01 early 1900’s. The Kuovila deposit is located in south- V 24 .14 .23 .18 western Finland within the 1.9 Ga Uusimaa Belt, which is composed of high-grade metamorphic felsic and mafic volcanic rocks, mica gneisses and granites. Exploration included geological mapping, magnetic and gravimetric ground surveys and the drilling of 52 has a plan to increase the capacity of the Pori TiO2- holes, altogether 5398 metres. The Kuovila deposit, plant from the present 130.000 TPA to 150.000 TPA. bordered by felsic and mafic volcanic rocks, which is

Fig. 5. The Kuovila calcite-wollastonite deposit in the Pohja district of southwestern Finland.

9 Geological Survey of Finland, Special Paper 36 Olli Sarapää, Timo Ahtola, Jukka Reinikainen and Hannu Seppänen composed of two lenses, which are 20-150 m wide GCC products (Table 1). Preliminary laboratory scale and about 1850 m long (Fig. 5). The deposit is covered benefication tests of the wollastonite-calcite marble by a 3-15m thick sandy till layer. The indicated produce a concentrate with about 74% wollastonite. resources of the Kuovila deposit estimated to the depth of 50 m to 125 m are 39 Mt calcite marble with Hakala calcite marble deposit 75% calcite and 9 Mt wollastonite-calcite marble with 54% calcite and 15% (10-60 %)wollastonite. The Hakala calcite marble deposit, a few hundred The Kuovila deposit comprises alternating, 10-45 m metres from the Järvenkylä deposit, is situated 35 km thick layers of calcite and calcite-wollastonite rock, southeast of the coastal city of Turku and twenty which are separated by 3-10 m thick felsic and mafic kilometers west of the city of Salo. The Hakala deposit volcanic rock layers. Within the deposit there are consists of four almost vertical calcite marble layers occasionally layers of diopside-garnet rock and gran- (Fig. 6). Total length of the deposit is about 500 ite. Calcite marble is typically coarse-grained, light metres. There is granite, granite pegmatite and skarn gray or white in colour with thin silicate interlayers. intercalations between the calcite marble layers. The Calcite content of the calcite marble ranges from 60 country rocks consist of granites, granite pegmatites to 95% and calcite in the marble is low in magnesium, and granodiorites. The indicated mineral resources iron and manganese. Thin silicate interbeds are com- estimate of the Hakala deposit to the depth of 125 m posed of quartz, feldspars, diopside and phlogopite. is 1.3 Mt with 84% CaCO3. The resource estimate is The wollastonite-calcite rock occurs in the border based on geological mapping and on 25 drill holes, zone of the deposit and also as individual layers. It is altogether 2780 metres. composed of alternating beds of calcite, quartz, The calcite marble of the Hakala deposit is coarse wollastonite, diopside and garnet. Laboratory scale grained and generally white or light gray in colour. benefication tests from the core samples were car- Mineralogically it is very pure and contains over 90% ried out at GTK and they produced concentrates calcite. Accessory minerals are diopside, quartz, containing over 99% calcite. After fine-grinding, the tremolite, wollastonite and sphene. No dolomite or ISO-brightness of minus 30 microns fraction of the graphite has been detected in the deposit. Calcite calcite concentrates is 90.4-95.9% and yellowness marble is chemically pure, 55% of the analysed sam-

0.3-1.8%, which correspond with the commercial ples contain over 90% CaCO3. Magnesium and iron

Fig. 6. A block diagram of the Hakala calcite marble deposit. The length of the deposit is about 500 metres.

10 Geological Survey of Finland, Special Paper 36 Industrial mineral potential in Finland

Lintinen, P. 2000. Kaoliinitutkimukset Sodankylän Suola- contents are low, generally MgO < 0.4%, Fe2O3 < 0.2%. Beneficiation tests of the calcite marbles give kaarkossa 1998-1999. Geological Survey of Finland, unpublished report M19/3732/2000/1/82 9 p., 7 app. 94-95% ISO-brightness values. Because the deposit Mäkitie, H., Kärkkäinen, N., Lahti, S. I.. & Alviola, R. has potential for underground mining, more detailed 2001. Compositional variation of granitic pegmatites in drilling is recommended to verify the continuation of relation to regional metamorphism in the Seinäjoki region, the deposit in deeper levels. western Finland. In: Mäkitie, H. (ed.) Svecofennian granitic pegmatites (1.86-1.79 Ga) and quartz monzonite (1.87 Ga), and their metamorphic environment in the Seinäjoki region, Conclusion western Finland. Geological Survey of Finland. Special Paper 30, 31-59. This paper presents briefly the essential results of Niemelä, M. 2001. Talc-magnesite deposits in Finland. In: Radvanec, M., Gondim, A. C. & Németh, Z. (eds.) IGCP most recent studies on marble (Reinikainen 1997, 443: magnesite and talc: geological and environmental corre- Reinikainen et al. 1999, Sarapää et al. 1999b, 2001) lations. Mineralia Slovaca 33 (6), 561-566. and ilmenite deposits (Kärkkäinen & Sarapää 2002, Pekkala, Y. 1998. Finland: paper pigments lead growth. Kärkkäinen 1999) in southwestern and western Fin- Industrial Minerals 374, 57-61. Pekkala, Y. 1999. Industrial minerals - consumption and land. They have potential to be further studied and perspectives in Finland. In: Shchiptsov, V. V., Skamnitskaya, developed by domestic and international industrial L. S. & Danilevskaya, L. A. (eds.) Industrial minerals: mineral companies operating in Finland (Pekkala 1998, deposits & new developments in Fennoscandia: proceed- 1999, 2001, Laurén 1999, 2001, 2002). A conclusive ings of the international conference, Petrozavodsk 1999. Petrozavodsk: Karelian Research Center. Institute of Geol- table of industrial mineral resources and their techni- ogy, 11-13. cal properties is also included. Apart from these, a Pekkala, Y. 2001. The potential of industrial minerals in map of industrial mineral potential is presented and it Fennoscandia. In: 3rd Fennoscandian Exploration and Min- gives an overview of industrial minerals sector in ing, Rovaniemi, December 3-4, 2001: final programme and event documentation. [S.l.]: European Union, European Finland (see also Pekkala & Reinikainen 1999, Pekkala Regional Development, 7 p. & Seppänen 2002). A comprehensive list of the Pekkala, Y. & Sarapää, O. 1989. Kaolin exploration in relevant papers of industrial minerals in Finland is also Finland. In: Autio, S. (ed.) Geological Survey of Finland. Current Research 1988. Geological Survey of Finland. Spe- added herein. cial Paper 10, 113-118. Pekkala, Y. & Niemelä, M. 1997. Vuolukivi - elämää tulikiven REFERENCES lämmössä. Summary: Soapstone - life in the heat of fire- stone. Vuoriteollisuus 55 (1), 27-32. Alviola, R. 1989. Rare element pegmatites in Finland. In: Pekkala, Y. & Reinikainen, J. P. 1999. Paperin mineraaliset Lahti, S. I. (ed.) Symposium Precambrian granitoids. raaka-aineet - käyttö ja kehitysnäkymät Suomessa. Sum- Petrogenesis, geochemistry and metallogeny, August 14- mary: Mineral raw materials in paper - consumption, and 17, 1989, Helsinki, Finland. Excursion C 1: Late orogenic perspectives in Finland. Vuoriteollisuus 57 (2), 52-56. and synorogenic Svecofennian granitoids and associated Pekkala, Y., & Seppänen, H. 2002. Perspectives on the pegmatites of southern Finland. Geological Survey of Fin- Finnish industrial mineral industry. In: Scott, P. W. & land. Guide 26, 11-15. Bristow, C. M. (eds.) Industrial Minerals and Extractive Alviola, R., Mänttäri, I., Mäkitie, H., & Vaasjoki, M. 2001. Industry Geology. 36th forum of the Geology of Industrial Svecofennian rare-element granitic pegmatites of the Minerals and 11th Extractive Industry Geology Congress, Ostrobothnia region, western Finland: their metamorphic Bath, England, 7th-12th May, 2000, Geological Society of environment and time of intrusion. In: Mäkitie, H. (ed.) London, 129-132. Svecofennian granitic pegmatites (1.86-1.79 Ga) and quartz Reinikainen, J. P., 1997. Carbonate rock units in the monzonite (1.87 Ga), and their metamorphic environment Svecofennian Uusimaa Belt, SW Finland. In: Autio, S. (ed.) in the Seinäjoki region, western Finland. Geological Survey Geological Survey of Finland, Current Research 1995-1996. of Finland. Special Paper 30, 9-29. Geological Survey of Finland. Special Paper 23, 37-41. Kärkkäinen, N. 1999. Titanium ore potential of small mafic Reinikainen, J. P. 2001. Petrogenesis of Paleoproterozoic intrusions based on two examples in western Finland. marbles in the Svecofennian Domain, Finland. Geological Houghton, MI: Michigan Technological University. 193 p. Survey of Finland, Report of Investigations154. 84 p., 1 Kärkkäinen, N., Sarapää, O., Huuskonen, M., Koistinen, app., 2 app. maps. E.& Lehtimäki, J. 1997. Ilmenite exploration in western Reinikainen, J. P., Ahtola, T. & Seppänen, H. 1999. Finland, and the mineral resources of the Kälviä deposit. In: Paleoproterozoic sedimentary carbonate rocks in the Autio, S. (ed.) Geological Survey of Finland, Current Re- Uusimaa Belt, southwestern Finland, Svecofennian Do- search 1995-1996. Geological Survey of Finland. Special main. In: Shchiptsov, V. V., Skamnitskaya, L. S. & Paper 23, 15-24. Danilevskaya, L. A. (eds.) Industrial minerals: deposits & Kärkkäinen, N. & Sarapää, O. 2002. Kälviän-Halsuan new developments in Fennoscandia: proceedings of the ilmeniittiesiintymät. Vuoriteollisuus 60 (4), 33-38. international conference, Petrozavodsk 1999. Petrozavodsk: Laurén, L. 1999. Industrial minerals maintain growth despite Karelian Research Center. Institute of Geology, 45. some setbacks. Kemia 26 (6), 489-491. Sarapää, O. 1996. Proterozoic primary kaolin deposits at Laurén, L. 2001. Solid performance by industrial minerals. Virtasalmi, southeastern Finland. Espoo: Geological Survey Kemia 28 (6), 480-481. of Finland. 152 p., 6 app. Laurén, L. 2002. Nordkalk diversifies output from its lime- Sarapää, O. 1997. Genesis and properties of Virtasalmi stone deposits. Vuoriteollisuus 60 (4), 14-15. kaolin deposits, SE Finland. In: Papunen, H. (ed.) Mineral

11 Geological Survey of Finland, Special Paper 36 Olli Sarapää, Timo Ahtola, Jukka Reinikainen and Hannu Seppänen

deposits: research and exploration - where do they meet? from calcite and ilmenite exploration in Finland. In: Autio, Proceedings of the Fourth Biennial SGA Meeting, Turku/ S. (ed.) Geological Survey of Finland, Current Research Finland/11-13 August 1997. Rotterdam: A. A. Balkema, 1997-1998. Geological Survey of Finland. Special Paper 27, 747-749. 25-34. Sarapää, O. 1999. Genesis of Virtasalmi kaolin deposits, SE Sarapää, O., Lohva, J., Lehtimäki, J., Kärkkäinen, N. & Finland. In: Shchiptsov, V. V., Skamnitskaya, L. S. & Jokinen, T. 1999b. Geophysical exploration of pigment Danilevskaya, L. A. (eds.) Industrial minerals: deposits & mineral deposits (kaolin, calcite, ilmenite) in Finland. In: new developments in Fennoscandia: proceedings of the EAGE 61st conference and technical exhibition, Helsinki, international conference, Petrozavodsk 1999. Petrozavodsk: Finland, 7-11 June 1999: extended abstracts book. Vol. 2: Karelian Research Center. Institute of Geology, 73-74. Poster presentations. Houten: European Association of Sarapää, O., Kuivasaari, T., Niemelä, M., Pekkala, Y. & Geoscientists & Engineers, 4 p. Reinikainen, J. 1996. Kaolin deposits in the Virtasalmi Sarapää, O., Reinikainen, J. P., Seppänen, H., area, Southeastern Finland; Geology, technical properties Kärkkäinen, N. & Ahtola, T. 2001. Industrial minerals and possible uses. In: Sarapää, O. Proterozoic primary exploration in southwestern and western Finland. In: Autio, kaolin deposits at Virtasalmi, southeastern Finland. Espoo: S. (ed.) Geological Survey of Finland, Current Research Geological Survey of Finland, p. 43-83. 1999-2000. Geological Survey of Finland. Special Paper 31, Sarapää, O., Kärkkäinen, N., Reinikainen, J. P., Ahtola, 31-40. T., Appelqvist, H. & Seppänen, H. 1999a. New results

12 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 13– 16 , 2003.

THE PETÄISKOSKI CARBONATE VEINS AT JUUKA, EASTERN FINLAND

by Matti Tyni1), Kauko Puustinen2), Juha Karhu3) and Matti Vaasjoki2)

1)Malmikaivos Oy, present address: Korvenkuja 7, FIN-62310 VOLTTI, FINLAND 2)Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND 3)Department of Geology, FIN-00014 University of Helsinki, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): carbonate rocks, veins, geochemistry, chemical composition, isotopes, Archean,Petäiskoski, Finland

Introduction the Juuka church, at a place where a forestry track crosses Petäisjoki (Fig. 1). An ash sample was col- Malmikaivos Oy observed, in the course of mineral lected from the campfire site of the bridging party, and exploration in 1988, that the first kimberlites it had it exhibited clearly anomalous contents of Ba. Also the found seemed to lay along a line extending towards heavy mineral fractions of soil samples from the NNE from Tuusniemi. A roughly corresponding line immediate surroundings displayed clearly elevated could be observed as a lineament on satellite photo- REE levels. Up to 50 cm large, red, galena-bearing graphs, which gave rise to interest in the northern carbonate boulders were found in the forest, and some extension of the kimberlite line. The area had already outcrops contained similar, but very narrow and sharp- earlier been of prospective interest, as Outokumpu Oy edged veins. As the find was not a kimberlite, the had in the 1950s several exploration claims along company soon abandoned the investigation. How- Petäisjoki northwards from Keskimmäinen Jokilampi ever, the region is still generally of prospective inter- up to the latitude of Petäiskoski. Among other things, est. Especially the boggy area north of the rapids could a barite-bearing target close to the Panjavaara farm, be investigated by till sampling. Some rock samples which lies c. 1.8 km SE of Petäiskoski had been collected from the vicinity of Petäiskoski and sus- investigated. Both lead isotopic measurements (Kouvo pected of being magmatic in origin have formed the 1958, Kouvo & Kulp 1961) and mineralogical studies material for this study. (Papunen 1967) were carried out on the target, but it has not been possible to find the exact location later Locality description on. In addition, the mineral catalogue for Finland (Laitakari 1967) lists (oral communication by Viluksela, Petäiskoski lies within an Archean granite-gneiss Vuorelainen & Huhma 1961) a bastnaesite- and area. In addition to the felsic gneisses, there occurs galena-bearing target on the western boundary of the also a narrow amphibolite belt, which appears on the Juuka parish. According to the map name, the location aeromagnetic map as a c. 1.5 km long, N-S striking could be 4 - 5 km NE of Panjavaara and Petäiskoski. anomaly. One target of Malmikaivos Oy lay close to the According to the regional geochemical mapping, a boundary of the Rautavaara parish c. 25 km WNW of Ba-La till anomaly stretches for c. 5 km NE from

13 Geological Survey of Finland, Special Paper 36 Matti Tyni, Kauko Puustinen, Juha Karhu and Matti Vaasjoki

Fig. 1. Location of the Petäiskoski area at Juuka in eastern Finland.

Panjavaara (Geological Survey of Finland 1990). Isotopic studies Around Petäiskoski, some sampling sites also exhibit elevated contents of Pb and Th. This is in accordance Because the composition of the Petäiskoski car- with the aerogeophysical ~-radiation map, which shows bonate vein resembles that of carbonatites, its oxygen a clear U anomaly at Petäiskoski, a weak extension of and carbon isotopic compositions were investigated. which continues for 1.5 km SE (Geological Survey of Also a bastnaesite sample from Panjavaara was Finland 1991). In contrast, no radiation anomaly exists analysed, and results for both samples are reported in at Panjavaara. Table 2. The carbon isotopic compositions of the samples are almost identical within experimental un- Petrography, mineralogy and chemical com- certainty, but are markedly more negative than the position average mantle value of –5 ‰. According to Deines (1989) 91 % of undisturbed carbonatites fall within the Macroscopically, the rock is coarse-grained and composition range from –2 ‰ to –8 ‰. Thus the partially breccia-like. The dominating colour is an carbon isotopic data does not support a carbonatitic intense brick red with paler patches and dark green origin of the Petäiskoski vein, although a mantle origin amphibole schlieren. The main minerals are calcite (0 cannot be completely ruled out. - 2 % Sr), bastnaesite (0 - 20 % Sr) and barite. The oxygen isotopic compositions of the Petäiskoski Strontianite, galena, alkali amphibole and quartz occur and Panjavaara samples differ greatly from each as accessory minerals. other. One possible reason could be differences in The chemical composition of one sample from the crystallization temperatures and reactions with exter- Petäiskoski occurrence is shown in Table 1, from nal fluids. According to this interpretation, the which the anomalously high levels of Sr, Ba and REE Petäiskoski calcite would represent a much later and are evident. more altered phase than the Panjavaara bastnaesite. The lead isotopic compositions of samples G20-

14 Geological Survey of Finland, Special Paper 36 The Petäiskoski carbonate veins at Juuka, eastern Finland

Table 1. Chemical composition of the carbonate rock at Petäiskoski.

(%) (ppm) (ppm)

SiO2 4.71 Co 1 La 35 500 TiO2 0.02 Cu 40 Ce 47 900 Al2O3 0.08 Ga 8 Pr 4 340 Fe2O3 1.47 Nb 1 Nd 11 100 MnO 0.27 Ni 22 Sm 651 MgO 0.63 Pb 855 Eu 115 CaO 36.10 Sb 1 Gd 384 SrO 2.28 Sc 4 Tb 40 BaO 3.87 Sn 10 Dy 38

Na2O 0.28 Ta 0 Ho 4 K2O 0.07 T h 83 Er 8 P 2O 5 0.43 U 2 Tm 1 CO2 33.38 V 11 Yb 5 SO3 2.26 Zn 40 Lu 1 Cl 0.03 Zr 4 Y 123 REE-Ox 12.03

Total 97.91

Table 2. Carbon andoxygen isotopic analyses. Table 3. Lead isotopic data ongalenas

Locality Nro Mineral d13Cd180 Sample Locality 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb (PDB) (SMOW) G20 Panjavaara 15.590 15.299 35.182 Petäiskoski C-490 Calcite -15.50 18.39 G500 Petäiskoski 15.596 15.290 35.171 Panjavaara C-235 Bastnaesite -16.38 9.98 Data normalized to the accepted values of SRM 981.

Fig. 2. Lead isotopic composition of the Petäiskoski and Panjavaara galenas in relation to other data from Finland.

15 Geological Survey of Finland, Special Paper 36 Matti Tyni, Kauko Puustinen, Juha Karhu and Matti Vaasjoki

Panjavaara and G500-Petäiskoski are presented in composition is also unique for the Karelian domain, Table 3, which demonstrates that the two samples are and thus the combined isotopic data are possibly almost identical within experimental error. Figure 2 indicative of a hydrothermal process closely associ- shows the results in relation to other galena data from ated with the Svecofennian orogeny. Finland. The striking feature is that the Petäiskoski and Panjavaara leads have isotopic compositions similar to the Svecofennian orogenic leads rather than the REFERENCES Archean or Karelian signatures typical of their geological environment (cf. Vaasjoki 1981). This is the Deines, P. 1989. Stable isotope variations in carbonatites. In: first time such a lead isotopic composition has been Bell, K. (ed.) Carbonatites: Genesis and evolution. London: Unwin Hyman, 301-359. recorded from the Karelian domain. At their face Geological Survey of Finland 1990. Map sheet 4312. value, the lead isotopic results seem to suggest a Geochemical maps 1 : 100 000, till. closer relationship to the Svecofennian orogeny than Geological Survey of Finland 1991. Map sheet 4312. would be assumed from the geographic location. Aerogeophysical maps 1 : 20 000. Kouvo, O. 1958. Radioactive age of some Finnish Precambrian minerals. Geological Survey of Finland, Bulletin 182. 70 p. Conclusion Kouvo, O. & Kulp, J. L. 1961. Isotopic composition of Finnish galenas. Annales of the New York Academy of The mineralogy and geochemistry of the Petäiskoski Sciences 91, 476-491. Laitakari, A. 1967. Suomen mineraalien hakemisto - Index of carbonate veins are unique for their geological envi- Finnish minerals with bibliography. Geological Survey of ronment and are suggestive of a carbonatitic origin. Finland, Bulletin 230. 842 p. However, the carbon isotopic results seem to rule out Papunen, H. 1967. On the barytes of Finland. Comptes a pure mantle source, while the oxygen isotope data Rendus de la Société Géologique de Finlande 39, 45-69. Vaasjoki, M. 1981. The lead isotopic composition of some indicate a large difference in crystallization conditions Finnish galenas. Geological Survey of Finland. Bulletin 316. for calcite and bastnaesite. The galena lead isotopic 25 p.

16 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 17– 21 , 2003.

DIRECT COMPARISON ON MECHANICAL AND DIGITAL SIZE ANALYSES OF KEMI CHROMITE, FINLAND

by Tegist Chernet and Jukka Marmo

Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): chromite ores, crushing, chromite, grain size, size distribution, sieving, image analysis, Elijärvi, Finland

Introduction The direct comparison of sieve and image analyses is considered to be possible because of the simple General crystal shape and morphology of chromite. The crystal habits of chromite include octahedrons, often with Chromite ore samples from the Länsiviia open pit of dodecahedral faces modifying the edges of the octa- the Elijärvi Mine, Kemi, Finland, were taken for grain/ hedron to the point of rounding the crystal. Here, well- particle size determination of the chromite in the ore. formed crystals are common and chromite is usually The samples were selected from a relatively less found as massive or granular aggregates and dissemi- fractured area. Seven to ten cm long pieces of chromite nated. Minerals forming acicular, bladed, fibrous, ore samples were treated by electric shock crusher at platy, prismatic, tabular, pseudomorphic crystals may the Forschungs - Zentrum, Karlsruhe, GmbH, Ger- need correction factors (Higgins 2000), if comparing many. The objective of this approach is to get liberated sieve and image analysis is to be possible at all. chromite grains in order to analyse the size distribution of chromite in the ore using sieve and image analysis. Application of electric shock crusher Polished sections were also prepared directly from the ore samples for size analyses by image processing. Compared to all other crushing (e.g., gyratory, roll, The study comprises three steps: impact, etc.) and grinding (conventional tumbling mills) - sieve analyses of chromite from crushed ore, techniques, where the breakage forces are applied by - image analyses of chromite from crushed ore, and compression or impact, the electric shock crusher - image analyses of chromite in the unbroken ore. separates materials along loose ends such as grain The aim was to investigate the correlation between boundaries and fractures. The advantage of this method sieve and image analysis on the one hand, and the is to liberate chromite grains along the natural grain correlation of the image size analyses of unliberated boundaries and existing deep fractures without unnec- chromite in the rock and liberated chromite in the essary breakage of particles. After crushing, chromite crushed ore on the other hand. The ultimate goal, of grains/particles are expected to show a similar grain/ course, was to find a better control in predicting particle size as in the rock. mineral liberations at certain grinds. The principle of operation is well described by

17 Geological Survey of Finland, Special Paper 36 Tegist Chernet and Jukka Marmo

Bluhm et al. (2000) and Sjomkin, et al. (1995). The Table 2. Heavy liquid separation of each sieve fraction process is disintegration of solid material through less than 400 microns. pulsed electric discharges. The material immersed in Particle size Heavy Light Heavy Light water is subjected to high voltage pulses up to several (microns) (wt%) (wt%) (cum wt%) (cum wt%) hundreds of kilovolts. Water has excellent breakage >400, if any 400-315 15.65 18.82 84.35 81.18 strength when the pulse voltage rises quickly, and 315-250 20.84 15.74 63.51 65.43 these bring about the concentration of electric field in 250-180 30.11 19.16 33.40 46.27 the solids. The electrical energy in the material then 180-90 27.69 23.75 5.65 22.52 90-63 4.62 9.72 1.03 12.80 creates very high pressure, which leads to the frag- 63-45 0.86 6.02 0.17 6.78 mentation of the material along grain boundaries and <45 0.17 6.78 0.00 0.00 existing fractures. As a result, composite materials and minerals can be decomposed in to separate and a separate frequency plot is shown in Figure 1. components. Sieve fractions between 800-400 microns (21% of the sample) contain only about 1-3% free chromite par- Particle size analyses of chromite in the ticles and as a result were not treated by heavy liquid. crushed ore (Sieve analysis) In this fraction almost every grain of silicate/carbonate contains chromite crystals as inclusions. In terms Mechanical sieving and sieve size analyses of the cumulative distribution, about 85% of chromite particles are less than 400 microns (Fig 1). Due to fine The electric shock treatment gave unexpectedly particle adhesion, repeated heavy liquid separation good results. Most of the chromite grains were liber- was needed for fractions less than 63 microns. There- ated and show perfect crystal shape/structure. Grains fore, the results for <63 microns are approximate. with deep fracturing broke along the fractures, which In the fraction 400 to 250 microns, almost all still show the actual particle size of chromite in the ore. chromite grains have perfect crystal shape without As a result of mechanical wet sieving in to 11 being broken. Broken pieces and flakes of chromite narrow fractions, 99% of the crushed ore is less than particles started to appear in the fractions bellow 250 800 microns (Table 1). Observing all the fractions, microns, and increase gradually along with decreas- chromite appeared to be considerably liberated in the ing grain size, especially in the fraction 90-63microns. fractions less than 400 microns, above which fine- Most of these liberated particles, however, appear the grained chromite (<45 microns) is embedded in coarse- same as in the rock. grained silicates and carbonates.

Particle size analyses of chromite in the Table 1. Wet mechanical sieve fractions. concentrate and in the ore (Image analysis)

Sieve size Wt (%) Cum. (microns) wt% Image analysis and principle >800 0.88 99.12 800-500 11.02 88.10 Image analysis is a technique for characterizing, 500-400 8.73 79.37 400-315 13.15 66.21 classifying and comparing images by using numerical 315-250 15.11 51.10 values for properties of features in images (Lastra R., 250-180 20.97 30.14 180-90 21.05 9.08 et al. 1998). Performing image analysis includes im- 90-63 5.01 4.07 age acquisition, image processing (e.g., enhancement, 63-45 2.12 1.96 segmentation and binary image processing), image 45-32 0.56 1.39 <32 1.39 0.00 analysis (measurements, quantitative data), and evaluation or representation of the results. In this study, the acquired images are processed and individual measurements are done for each feature in the images Heavy liquid separation and sieve size analy- (object specific), which includes area, length, width ses of chromite concentrate and sphericity of each feature. Several images were taken from petrographic mi- Liberated chromite was separated from the rest of croscope as colour images using a colour video cam- the gangues, which consists of silicates and carbon- era and frame grabber. Using KS-400 version 3 image ates using heavy liquid. The result is shown in Table 2, analysis software, a segmentation routine is per-

18 Geological Survey of Finland, Special Paper 36 Direct comparison on mechanical and digital size analyses of Kemi chromite, Finland

100 10 0

80 80

60 60

40 40 Cum wt% Cum wt%

20 20

0 0 0 0100 100 200 200 300300 400400 500500 ParticleParticle sizesize (microns)

Fig. 1. Frequency and cumulative particle size distribution of heavy liquid separated chromite concentrate.

Fig 2. Image of chromite ore overlapped with honeycomb structure for grain boundary reconstruction. formed manually to segment images of chromite analysed from the given fractions. Measurement data grains/particles into separate binary images. It is is given in Table 3. performed by detecting and setting the lower and upper gray levels for chromite. When chromite occurs Table 3. Particle/grain size distribution of chromite in masses or clustered where grain boundaries and grains/particles according to image analyses (selected sieve fractions 160-250 microns). deep fractures are poorly delineated, a grain boundary reconstruction technique was used to produce dis- Particle size No. of grains No. of grains (microns) measured in % crete grains (Fig. 2). <45 11 0.11 45-63 137 1.4 Chromite concentrate 63-90 213 2.18 90-180 4679 47.94 180-250 4184 42.86 Polished sections were made from size fractions 250-315 471 4.83 160-250 microns of the chromite concentrates. This 315-400 57 0.58 fraction constitutes 36% of the heavy fractions (<400 >400 9 0.09 microns). The selection of this fraction is on the basis total 9761 of best liberation, and silicates here are rare. Particle sizes of discrete grains/particles of chromite were analysed from the reconstructed images. The area and maximum and minimum ferets of each particle were measured. About 10,000 separate features were

19 Geological Survey of Finland, Special Paper 36 Tegist Chernet and Jukka Marmo

Chromite in the unbroken ore lation. Although not enough work has yet been done on the Particle/grain size of chromite was also analysed liberated chromite particles/grains to fully compare directly from the ore (from the Länsiviia open pit). The image analyses results of the liberated chromite and analyses include all sizes in the ore. Very fine-grained chromite from unbroken ore, basic conclusions can be chromites (<50 microns), however, are scrapped for drawn from about 4500 features analysed. As shown the reason of comparison to that of the concentrate. in Table 2 and Figure 1, over 57 wt% of the heavy Most of these fines are embedded in the coarse- fraction (chromite concentrate, all < 400microns) is grained gangue minerals within the fraction 400-800 between 90-250 microns. Considering the image analy- microns, which is not included in the chromite concen- ses result (Table 5), 56wt% of chromite particles/ trate (<400 microns). About 4500 grains/particles are grains analysed in the ore are between 90-250 mi- measured and the results are tabulated in Tables 4 crons. Keeping in mind the fact that the present size of and 5. most chromite in the ore is similar to that of chromite in the crushed ore, image size analysis of chromite in

Table 4. Particle/grain size distribution of the chromite the ore yields similar size distribution as if it were done from the unbroken ore using image analyses (calculated by sieve. from ferets average). Furthermore, it was studied which of the feature analyses would match best with the sieve analysis. Particle size No. of No. of Weight Weight Both area diameter and feret average of chromite (microns) grains grains (%) (gm) (%) grains/particles in the ore are measured and plotted. <63 0 0.00 0.00000 0.00 Ferets, which imply maximum and minimum length of 63-90 33 0.74 0.00011 0.01 90-180 1238 27.86 0.01882 2.12 particles, are measured by the software and the 180-250 1159 26.08 0.05925 6.68 average is calculated using excel. As shown in Figure 250-315 771 17.35 0.08766 9.88 315-400 647 14.56 0.14570 16.42 3, the sieve analysis frequency distribution of chromite 400-500 325 7.31 0.15841 17.85 concentrate almost overlaps the plot of ferets average 500-800 239 5.38 0.28012 31.56 >800 32 0.72 0.13745 15.49 represented by number of grains percent rather than calculated as weight percent. On the other hand, area diameter calculated as weight percent almost overlaps Table 5. Particle/grain size distribution of the chromite to that of sieve analysis rather than area diameter from the unbroken ore using image analyses (calculated from area diameter). calculated as number percent (Fig. 4). As a result, the percent of the number of particles calculated from ferets average and the weight percent calculated from Particle size No. of No. of Weight Weight (microns) grains grains (%) (gm) (%) area diameter correlate more closely to that of sieve analysis represented by weight percent. <45 200 4.47 0.00003 0.09 45-63 459 10.26 0.00015 0.46 63-90 986 22.05 0.00093 2.86 Conclusions 90-180 2185 48.86 0.00996 30.67 180-250 453 10.13 0.00821 25.27 250-315 115 2.57 0.00493 15.19 Chromite grains were almost completely liberated in 315-400 54 1.21 0.00450 13.84 400-500 17 0.38 0.00294 9.05 grain sizes below 400 microns. In order to compare >500 3 0.07 0.00084 2.59 sieve size and image size of chromite particles, chromite in the concentrate should appear in size similarly as in the ore. Disintegrating chromite using high intensity Comparison electrical pulses turned out to be the only way to liberate chromite along existing boundaries. Simple According to image analyses results of the selected microscope observation indicated chromite in the origi- sieve fraction (160-250), about 90.8% of the grains/ nal rock (ore) and chromite as a product of electric particles fall between 90-250 microns (see Table 3). shock crusher to be correlated. The size analysis result About 10,000 features analysis is considerable for shows considerable correlation between mechanical making comparison. Although the quality of the im- sieve size analyses and digital size analyses. Moreo- ages, orientation and shape factors affect the similar- ver, image size analyses of chromite in the ore were ity, the result generally shows good correlation be- found to be correlated to that of the sieve analysis of tween mechanical sieve size analyses and digital size chromite concentrate. The ferets average represented analyses. Further data manipulations and estimating by number percent and the area diameter represented the sampling error might lead to an even better corre- as weight percent are more closely correlated to the

20 Geological Survey of Finland, Special Paper 36 Direct comparison on mechanical and digital size analyses of Kemi chromite, Finland

35,00 35,00 chromite conc., sieve analysis (wt%) 30,00 chromite conc., sieve analysis (wt%) 30,00 25,00 25,00 chromitechromite inin the the ore, ore, feret feret av. av. (wt% (wt%)) 20,0020,00

15,0015,00 chromite in the ore, ferets av. (no%)

wt%, no of grains % 10,0010,00 chromite in the ore, ferets av. (no%) wt%, no of grains %

5,005,00

0,000,00 0 200 200 400 400 600 600 800 800 1000 1000 1200 1200 particle size size (micron) (micron)

Fig 3. Comparison of image analysis results of chromite calculated from ferets average to that of chromite concentrate sieved.

60.00 60,00 50.00 50,00 chrom ite in the ore, area diam eter (no% ) chromite in the ore, area diameter (no%) 40.0040,00 % 30.0030,00 chromchromite ite conc., conc. ,sieve sieve analysis analysis (w(wt t%%) ) w eight w eight weight % 20.0020,00 chromitechrom itein thein the ore, ore,area area diameter diam eter (wt%) 10.0010,00

0.000,00 0 100 200 200 300 300 400 400 500 500 600 600 700 700 800 800 900 900 particlparticlee sisizeze (micron)

Fig 4. Comparison of image analysis results of chromite calculated from area diameter to that of chromite concentrate sieved sieve analysis. REFERENCES In addition, this study indicates that size analysis of Bluhm, H., Frey, W., Giese, H., Hoppé, P., Schultheiss, C. the ore using image manipulation can be used to & Strässner, R. 2000. Application of pulsed HV dis- predict ore breakage and mineral liberations can be charges to material fragmenation and recycling. IEEE Trans- obtained at certain grinds, as in the experience at the actions on Dielectrics and Electrical Insulation 7, 625-636. Higgins, M. D. 2000. Measurement of crystal size distribu- Kemi mine. tions. American Mineralogist 85, 1105-1116. Lastra R., Petruk W. & Wilson J. 1998. Image analysis techniques and applications to mineral processing. In Mod- ern Approaches to Ore and Environmental Mineralogy, Mineralogical Association of Canada 27, 327-366. Sjomkin, B., Ussov, A. & Kurets, V. 1995. The principles of electric impulse destruction of materials. Akademi Nauk Rossija (in Russian). No pagination.

21 Geological Survey of Finland, Special Paper 36 Matti Tyni, Kauko Puustinen, Juha Karhu and Matti Vaasjoki

22 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 23– 28 , 2003.

ESTIMATION OF FERRIC IRON, CRYSTAL WATER AND CALCULATION OF CHEMICAL FORMULAE FOR ALTERED ILMENITE FROM ELECTRON MICRO- PROBE ANALYSES, BASED ON STOICHIOMETRIC CRITERIA

by Tegist Chernet and Lassi Pakkanen

Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): ilmenite, alteration, pseudorutile, electron probe data, ferric iron, stoichiometry, formula

Introduction the parent minerals, ilmenite and pseudorutile respectively, until the structure breaks down completely. Overview Chaudhuri and Newesely (1990), Mücke and Chaudhuri (1991) and Chernet (1999) also discussed In sand deposits, ilmenite exhibits various degrees the continuous transformation of ilmenite to leucoxene. of alteration due to oxidation and preferential leaching The alteration starts with a continuous removal of of iron. However, only three mineral phases: ilmenite, Fe+2, and the electrostatic charge is balanced by pseudorutile and rutile have been well identified with oxidizing the remaining iron and/or addition of H+. ideal composition of 47.35% FeO + 52.65% TiO2, Ferrous iron is totally oxidized at the formation of

39.98% Fe2O3 + 60.02% TiO2 and over 95% TiO2, pseudorutile. Further removal of ferric iron is com- respectively. The theoretical chemical formulae are pensated for by the addition of OH- into the mineral

FeTiO3 for ilmenite, Fe2Ti3O9 for pseudorutile and lattice. Along with the advance of the alteration, the

TiO2 for rutile. Due to alteration, the chemistry of water content increases until the breakdown of a these individual phases shows deviations from their pseudorutile structure, which appears at the compo- ideal compositions, which is also reflected in their sition of about 77-79% TiO2 and 9-12% Fe2O3 optical properties. The alteration product, which devi- (Chernet 1999). Leucoxene is the incomplete break- ates substantially from the ideal ilmenite composition down of pseudorutile, and consists principally of fine but not completely altered to pseudorutile, is identified grained, usually fibrous-like crystalline rutile. These as pseudoilmenite in Chaudhuri and Newesely (1990) referred conditions are taken into consideration to and as leached ilmenite in Chernet (1999). Continuous draw an assumption for correcting the analyses and transition from ilmenite to pseudorutile are also well recalculating ferric iron, lattice water content and the described recently (Kao & Yang 1999). Further chemical formula at a given composition of altered alteration of pseudorutile to leucoxene often shows an ilmenite. intermediate product identified as leached pseudorutile Reduction is one of the important steps in the TiO2 (Chernet 1999). Leached ilmenite and leached pigment production in the sulphate process if ferric pseudorutile are intermediate phases and they do not iron is present. Ilmenite raw material might be up- have their own characteristic peaks in the X-ray graded by reduction in order to remove accessory diffraction pattern. They show the same structure as minerals by magnetic separation (Balderson et al.

23 Geological Survey of Finland, Special Paper 36 Tegist Chernet and Lassi Pakkanen

2002). As a result, determination of ferric iron has not to a mineral. However, this may not always be only scientific but also economic significance. Al- sufficient. Chemical analyses show which elements though the samples studied are from Australian com- are present, and how much of each, but not how they mercial sand ilmenite concentrate, determination of are combined in the structure of the mineral. For ferric iron and chemical formulae is applicable for the altered ilmenite, this last uncertainty could be exempli- above-mentioned phases from any hard rock or black fied by the role of water and oxidation state of iron in sand deposits. the analysis. In the method described below, the following as- Objective sumptions are taken into consideration: 1) As alteration starts with a continuous removal As a result of continuous alteration, there is no of Fe+2, for the formation of leached ilmenite definite expression for the intermediate phases in (pseudoilmenite) the electrostatic charge is assumed terms of chemical composition, structure and formu- to be balanced only by oxidizing the remaining iron. lae except for ilmenite, pseudorutile and rutile. (oxidation) Carmichael (1967), Droop (1987) and Deer et al. 2) Total iron is oxidized at the formation of (1992) have shown how to determine ferric iron from pseudorutile. Removal of iron is a continuous process electron microprobe analyses, which cannot distin- and at the formation of pseudorutile phases, the guish between the two oxidation states. These formu- removal of ferric iron is assumed to be compensated lae are well applicable to some silicates and oxides by the addition of OH ions into the mineral lattice. This (e.g. ilmenite and rutile), which have a definite number is according to Grey and Watts (1994), Mücke and of anions and yield good analytical calculations. For Chaudhuri (1991) and Chernet (1999), who regarded the altered phases, however, erratic analysis totals pseudorutile phase as an oxyhydroxide mineral. (leach- and the presence of water in the crystal lattice further ing and hydrolization) complicate the calculation of chemical compositions 3) Upon the formation of leucoxene, OH is re- and the determination of chemical formulae. leased to a large extent due to the breakdown of the This paper presents a simple mathematical flow- pseudorutile structure into rutile and water.

sheet to estimate wt% of FeO, Fe2O3 and H2O from (dehydrolization) the given electron microprobe analysis data, using All methods are hypothetical and are not necessar- stoichiometric criteria. The flow-sheet further presents ily warranted and all may give only approximate the chemical formula representation of the phase at a results. given chemical composition. In order to determine this flow sheet, however, the basic ideas are referred to Analyses data and stoichiometric consideration from Droop (1987) and Deer et al. (1992). Electron microprobe analyses have been done to Microscopic descriptions of altered ilmenite confirm the complete range of alteration products of Microscopic descriptions of altered ilmenite ilmenite observed under the microscope, and to study The ore microscopy observations of ilmenite and its the chemical composition of each phase (Table 2). alterationThe ore microscopy products along observations with their of ilmenite characteristic and its Moreover, the data is used to calculate Fe2+ and Fe3+ alterationfeatures are products listed in along Table with 1. Figurestheir characteristic for typical content, and the respective chemical formulae of features are listed in Table 1. Figures for typical features of each phase can be referred to in Chernet stable and intermediate phases. The operating condi- features of each phase can be referred to in Chernet (1997, 1999). tions were: accelerating voltage 15-20 kV, probe (1997, 1999). current 20-40 nA, and beam diameter 1-10 µm. The ferric iron and the chemical formulae for Microprobe analyses and calculation of ilmenite and rutile can be determined using Droop’s formulae (1987) formulae, or after the estimation of the two irons, the Deer et al (1991) method can be used to represent the formulae.

Assumptions Trivalent iron, H2O and the chemical formulae for the intermediate products (leached ilmenite, pseudo- A characteristic chemical composition can be ex- rutile, leached pseudorutile) can be derived as follow: pressed by a formula that shows the elements present 1. Determination of molecular proportions

in the mineral and the proportion in which they are e.g., SiO2 (mol. prop.) = SiO2 (wt%)/ SiO2 (mol. wt) combined. Its chemical analysis provides the basic 2. Determination of mole % on the basis of Ti = 3

evidence for assigning the correct chemical formula e.g. Si (mole %) = 3 * (SiO2 / TiO2) (mol. prop.)

24 Geological Survey of Finland, Special Paper 36 Estimation of ferric iron, crystal water and calculation of chemical formulae for altered ilmenite... ilmenite ilmenite, ilmenite, ilmenite ect,with Mn ect than in ilmenite lections, microfractures lections, microfractures ong anisotropic effect, with Mn rich ellowish brown colour impression, internal ellowish colour impression, internal reflections less anisotropic effect and relatively less anisotropic effect fine rutile crystals and other leached products ellow, white microfractures, aggregates of fine rutile crystals ellow, white reflections,microfractures, aggregates of none eff strong colour, anisotropic none str colour, none against grey impression colour lections y brown, ong brightness yellow, orange, strong brightness, twinning, internal reflection ong brightness without reflections y brown, reflections red brown brown, tint) to light pinkish brown) colournone grey bright to distinct, none pinkish against brown grey impression to colour grayish brown pleochroism to light brown grey)none colour (as in the air medium) none anisotropism effect is less than ilmenite none against blue impression colour nonenone with brightness distinct brown, orange by covered internal internal ref brown, abundant: y none by covered internal brown, abundant: y poor light blue grey) without colour brown, red, blood red ellowish grey blue grey, bright pinkish tint brown with pinkish colour rich ilmenite, no pleochroism and relatively blue (Fe poor) light blue grey) without colour brown, red, blood red grey, dull grey grey, grey, dull grey brown, orange brown and other leached products oil light grey, faint strong (light grey to strong brightness yellow, orange, strong brightness, twinning, internal reflection oil pinkish brown strong (pinkish brown strong brightness without oil yellowish grey oil brown grey very slight (brown grey distinct brightness without oil grey none by masked internal brown, orange internal ref oil blue grey, bright none none, very weak, weak rare: red brown, against blue impression colour Table 1. Ore microscopy description of ilmenite and its alteration products. phaseIlmenite medium air colour with brown pleochroism to (brown slight light str anisotropism internal reflections characteristic features Primaryrutile air bluish grey, light to grey (light slight str when Fe Leachedilmenite air brown grey Secondaryrutile air y grey dull ref less eff anisotropic Pseudorutile air pseudorutile brownish grey colour brown Leached air grey

25 Geological Survey of Finland, Special Paper 36 Tegist Chernet and Lassi Pakkanen

Table 2. Microprobe analyses of ilmenite and its alteration products.

Ilmenite

SiO2 TiO2 Al2O3 Cr2O3 V2O3 FeO MgO MnO CaO ZnO NiO Nb2O3 Ta2O5 SnO Total 0.02 49.70 0.01 0.15 0.27 47.24 0.20 0.36 0.00 0.00 0.01 0.13 0.00 0.02 98.10 0.00 49.56 0.00 0.02 0.01 46.20 0.04 2.33 0.00 0.02 0.00 0.42 0.00 0.04 98.63 0.02 50.04 0.06 0.00 0.00 47.46 0.06 0.73 0.03 0.03 0.02 0.06 0.12 0.08 98.71

Leached ilmenite

SiO2 TiO2 Al2O3 Cr2O3 V2O3 FeO MgO MnO CaO ZnO NiO Nb2O3 Ta2O 5 SnO Total 0.07 55.70 0.59 0.05 0.11 33.37 0.04 4.97 0.03 0.11 0.00 0.09 0.08 0.01 95.20 0.01 55.56 0.05 0.03 0.00 37.96 0.07 1.82 0.01 0.10 0.00 0.03 0.00 0.03 95.66 0.13 58.30 0.62 0.21 0.30 35.40 0.13 1.45 0.03 0.03 0.00 0.09 0.00 0.02 96.71

Pseudorutile

SiO2 TiO2 Al2O3 Cr2O3 V2O3 FeO MgO MnO CaO ZnO NiO Nb2O3 Ta2O 5 SnO Total 0.12 66.04 0.52 0.06 0.08 24.21 0.08 1.33 0.04 0.04 0.03 0.09 0.00 0.02 92.67 0.19 64.62 0.52 0.13 0.00 25.62 0.12 1.58 0.05 0.04 0.02 0.09 0.00 0.00 92.98 0.15 62.16 1.04 0.08 0.15 28.28 0.04 1.21 0.04 0.02 0.02 0.45 0.04 0.03 93.71

Leached pseudorutile

SiO2 TiO2 Al2O3 Cr2O3 V2O3 FeO MgO MnO CaO ZnO NiO Nb2O3 Ta2O 5 SnO Total 0.26 70.67 2.46 0.13 0.16 15.79 0.07 0.11 0.08 0.05 0.03 0.07 0.08 0.00 89.96 0.23 72.02 0.96 0.12 0.31 13.95 0.00 0.32 0.04 0.00 0.03 0.08 0.12 0.01 88.18 0.91 74.57 2.43 0.20 0.35 10.32 0.01 0.14 0.07 0.00 0.00 0.09 0.00 0.01 89.08

For leached ilmenite on the basis of Ti=3

Equations to determine Fe3+ for leached ilmenite

E.g., Si=0.005, Al=0.02, ….., Fe=2.00, Mg=0.004, Mn=0.3, Nb=0.0015 (mole %)

2+ 3+ +4 3+ 2+ 4+ 2- Fex + Fey +Si0.005 +Al0.02 +Mg0.00 +…+ Ti3 +O9 = 0

2x + 3y = 5.28 (1) x + y = 2.00 (2)

from equation (1) and (2) Fe2+=0.72, Fe3+=1.28 2+ 3 Fe Ti 0 leached ilmenite: (Fe 0.72Fe 1.28 Mn0.3 …)Ti309 = 2.33 3 9

For pseudorutile on the basis of Ti=3

Equations to determine (O2- +OH1- ) for pseudorutile

E.g., Si=0.01, Al=0.02, …., Fe=Fe3+=1.36, Mg=0.01, Mn=0.07, Nb=0.001(mole %)

4+ 3+ 3+ 2+ 2+ 4+ 4+ 2- 1- Si0.01 +Al0.03 +…+Fe1.28 +Mg0.01 +Mn0.07 +Nb0.001 +Ti3 +(Ox +OHy )9 = 0

2x + y = 16.34 (3) x + y = 9 (4)

from equation (3) and (4) O = 7.34, OH = 1.66 3+ Fe Ti O (OH) pseudorutile: (Fe 1.36Si0.01Al0.02….Mg0.07Mn0.05…)Ti3O7.34(OH)1.66 = 1.5 3 7.34 1.66

26 Geological Survey of Finland, Special Paper 36 Estimation of ferric iron, crystal water and calculation of chemical formulae for altered ilmenite...

For leached pseudorutile on the basis of Ti=3

Equations to determine (O2- +OH1- ) for pseudorutile

E.g., Si=0.01, Al=0.08,.., Fe3+=0.83, Mg=0.01, Mn=0.01, Ca=0.01, Nb=0.001 (mole %) 4+ 3+ 3+ 2+ 2+ 4+ 2- 1- Si0.01 +Al0.08 +…+Fe0.83 +Mg0.01 + Mn0.01 +…+Ti3 +(Ox +OHy )= 0

2x + y = 14.83 (3) x + y = 9 (4)

from equation (3) and (4) O = 5.83, OH = 3.15 3+ Fe Ti O (OH) leached pseudorutile: (Fe 0.83Si0.01Al0.08…Mg0.01Mn0.01…)Ti3O5.83(OH)3.15 = 0.94 3 5.83 3.15

Table 3. Corrected microprobe analyses of ilmenite and its alteration products.

Ilmenite

SiO2 TiO2 Al2O3 Cr2O3 V2O3 FeO Fe2O3 MgO MnO CaO ZnO NiO Nb2O3 Ta2O5 SnO Total 0.02 49.70 0.01 0.15 0.27 37.07 11.30 0.20 0.36 0.00 0.00 0.01 0.13 0.00 0.02 99.23 0.00 49.56 0.00 0.02 0.01 34.39 13.12 0.04 2.33 0.00 0.02 0.00 0.42 0.00 0.04 99.95 0.02 50.04 0.06 0.00 0.00 37.64 10.91 0.06 0.73 0.03 0.03 0.02 0.06 0.12 0.08 99.80

Leached ilmenite

SiO2 TiO2 Al2O3 Cr2O3 V2O3 FeO Fe2O3 MgO MnO CaO ZnO NiO Nb2O3 Ta2O5 SnO Total 0.07 55.70 0.59 0.05 0.11 12.04 23.70 0.04 4.97 0.03 0.11 0.00 0.09 0.08 0.01 97.57 0.01 55.56 0.05 0.03 0.00 18.13 22.04 0.07 1.82 0.01 0.10 0.00 0.03 0.00 0.03 97.87 0.13 58.30 0.62 0.21 0.30 7.51 31.00 0.13 1.45 0.03 0.03 0.00 0.09 0.00 0.02 99.81

Pseudorutile

SiO2 TiO2 Al2O3 Cr2O3 V2O3 Fe2O3 MgO MnO CaO ZnO NiO Nb2O3 Ta2O5 SnO H2O Total 0.12 66.04 0.52 0.06 0.08 26.91 0.08 1.33 0.04 0.04 0.03 0.09 0.00 0.02 4.13 99.49 0.19 64.62 0.52 0.13 0.00 28.47 0.12 1.58 0.05 0.04 0.02 0.09 0.00 0.00 3.10 98.93 0.15 62.16 1.04 0.08 0.15 31.43 0.04 1.21 0.04 0.02 0.02 0.45 0.04 0.03 1.39 98.24

Leached pseudorutile

SiO2 TiO2 Al2O3 Cr2O3 V2O3 Fe2O3 MgO MnO CaO ZnO NiO Nb2O3 Ta2O5 SnO H2O Total 0.26 70.67 2.46 0.13 0.16 17.55 0.07 0.11 0.08 0.05 0.03 0.07 0.08 0.00 8.37 100.08 0.23 72.02 0.96 0.12 0.31 15.50 0.00 0.32 0.04 0.00 0.03 0.08 0.12 0.01 9.83 99.56 0.91 74.57 2.43 0.20 0.35 11.46 0.01 0.14 0.07 0.00 0.00 0.09 0.00 0.01 11.13 101.36

Summary the formation of pseudrutile. Pseudorutile consists of

Fe2O3 and H2O, until the formation of rutile. The Microprobe analyses show a wide range of chemi- structure of pseudorutile breaks down upon the for- cal composition with erratic and low analysis totals for mation of rutile and dehydrolization resulted in the altered ilmenite. There is neither definite expression removal of water from the system. At this point, the of chemical composition nor ideal chemical formulae above formula could not be applicable. for altered ilmenite as in the parent minerals. At a given chemical composition of altered ilmenite, REFERENCES however, wt% estimation of FeO, Fe2O3 and H2O, correction of electron microprobe analyses data, and Balderson, G & Potivin, J.C. 2002. Beneficiation of an chemical formula can be determined. The basis of this ilmenite feedstock for the sulphate TiO2 pigment process estimation is the determination of molecular propor- by reduction roasting. 15th Industrial Minerals International tions of compounds and mole percent of the corre- Congress, 50-55. sponding elements on the bases of titanium rather than Carmichael I. S. E 1967. The Iron-Titanium oxides of salic Volcanic rocks and their associated ferromagnesian sili- oxygen. Ilmenite consists of both FeO and Fe2O3, until cates. Contribution to mineralogy and petrology 14, 36-64.

27 Geological Survey of Finland, Special Paper 36 Tegist Chernet and Lassi Pakkanen

Chaudhuri J.N.B.& Newesely, H. 1990. Transformation of Longmans, 678-681, 578-579. Droop, G.T.R. 1987. A general equation for estimating Fe3+ ilmenite FeTiO3 to leucoxene TiO2 under the influence of weathering reactions. Indian Journal of Technology 28, 13- concentrations is ferromagnesian silicates and oxides from 23. microprobe analyses, using stoichiometric criteria. Minera- Chernet, T. 1997. Mineralogical study on Australian sand logical Magazine 51 (3), No. 361, 431-435. ilmenite concentrate, Australia. Extended abstract, Mineral Grey, I.E. & Watts, J.A. 1994. Mineralogical nomenclature: deposit: Research and exploration - where do they meet? pseudorutile revalidated and neotype given. Mineralogical Proceedings of the 4th biennial SGA meeting, Turku, Fin- magazine 58, 597-600. land. Rotterdam: A.A. Balkema, 709-712. Kao, Li-Shun &Yang, Houng-Yi 1999. TEM study of the Chernet, T. 1999. Applied mineralogical studies on Austral- continuous transition from ilmenite to pseudorutile by ian sand ilmenite concentrate with special reference to their vacancy-ordering and Fe-oxidation. Geological Society of behaviour in sulphate route pigment extraction process. America, 31(7), 170. International Journal of Minerals Engineering 12 (5), 485- Mücke A.& Chaudhuri, J.N.B 1991. The continuous altera- 495. tion of ilmenite through pseudorutile to leucoxene. Ore Deer, W. A., Howie, R.A. & Zussman, J. 1992. An introduc- geology reviews 6, 25-44. tion to the rock forming minerals. 2nd edition, Harlow:

28 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 29– 33 , 2003.

MERCURY-RICH COATING ON SOME GOLD NUGGETS FROM IVALOJOKI PLACERS, NORTHERN FINLAND

by Kari A. Kinnunen

Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): gold ores, placers, gold, nuggets, mercury, panning, amalgamation, Ivalojoki, Finland

Introduction posed of gold with a thin gold-mercury coating. They are interpreted as amalgamated gold nuggets resulting Silvery greyish nuggets were sent to GTK from from historical gold recovery operations that utilized Ivalojoki as possible platinum nuggets. Laboratory mercury. The amalgam nuggets are described and the determinations showed that the nuggets are com- environmental implications of the find are discussed.

Fig. 1. Known localities of amalgamated gold nuggets in the Ivalojoki placer area: 1 Ruikanmutka, 2 Kolmosenkoski and 3 the junction of Sotajoki. Map of the claims 1880’s, according to G. Svedelius (Fig. 7 in Sarlin 1902). The length of the bar depicts the gold content of the gravel at individual claims.

29 Geological Survey of Finland, Special Paper 36 Kari A. Kinnunen

Gold prospectors were interviewed for similar finds. mosenkoski to Grönholmankoski (river length about 6 Amalgamated nuggets showed to be rare, because km) by the Jansson diving team, only the mentioned only three river bottom localities revealed mercury two places are noted. All observations are from the indications from Ivalojoki. Similarly, no positive mer- bottom sediments of the river, none is known from the cury anomalies were seen in the geochemical maps shore sediments. Thus the total number of known sites from the Ivalojoki area (Reimann et al. 1998). in the Ivalojoki river area is only three (Fig. 1). These localities with mercury contamination were Localities all exploited for the most part in 1870-1880 (Sarlin 1902). According to Sarlin (1902, p. 16), mercury was These nuggets were found in summer 2002 by Mr. occasionally used in the recovery of the finest gold. Kalle Kupi from the claim of Mr. Sastos Rapelli and Two of the old claims, Ruikanmutka and Kol- Jouni Lönngvist. The nuggets were gathered with mosenkoski, also yielded comparatively high gold suction dredging from the bottom of the Ivalojoki river amounts, typically over 10 kg Au per claim, compared bed in Ruikanmutka, Ivalojoki area (Fig. 1). The to the typical 1 kg Au per claim in the river area concession name of this claim is Legenda and code (Sigzelius 1987, p. 45). 7123/1 (map sheet 3813 09). The nuggets occurred at a depth of half a metre from the sediment and water Mercury-rich coating interface. According to Mr. Kupi, the nuggets from deeper sediment layers were devoid of the greyish Two flaky gold nuggets (length about 4 mm) show- coating. ing greyish coating from Ruikanmutka (Fig. 2) were Only two other localities of similar mercury con- analysed with SEM EDS by Bo Johanson at GTK, tamination are known from the Ivalojoki placer area Espoo. The average composition of the coating was (Per Olov Jansson, personal communication 2002). 60 wt. % Au and 40 % Hg. This is a mean of three One locality is near the southern shore of Kol- analyses from different points, which showed varia- mosenkoski about 2 km downstream from the histori- tion from 1 to 2 wt.% in both elements. This result cal gold station of Kultala. The other is near the corresponds to Au-amalgam. confluence of the Sotajoki river with the Ivalojoki The exposed gold area in these larger nuggets did river. In this place, metallic mercury was seen in at a not show any detectable Ag, Cu or Hg. Likewise, the depth of half a metre in the river bottom. It is notewor- Au-amalgam coatings did not show traces of Ag or thy that although hundreds of crevasses and depres- Cu. The contents of these elements are thus less than sions have been prospected in the area from Kol- 0.1 wt.%, which is the detection limit of the SEM-EDS

Fig. 2. Partly amalgamated gold nuggets from Ruikanmutka claim no. 20, according to G. Svedelius and matching the claim 7123/1 today (locality 1 in Fig. 1). The nuggets are of plate morphology with dimensions 4.0 x 2.9 x 0.3 mm (on left) and 4.3 x 2.2 x 0.4 mm (on right). Photo: Kari A. Kinnunen.

30 Geological Survey of Finland, Special Paper 36 Mercury-rich coating on some gold nuggets from Ivalojoki placers, northern Finland

Fig. 3. Totally amalgamated smaller gold nuggets from Ruikanmutka (locality 1 in Fig. 1). The length of the nuggets ranges from 0.6 to 2.4 mm. Photo: Kari A. Kinnunen.

instrumentation used. It should be noted that, although from the Ivalojoki area show typically various natural naturally occurring gold containing traces of mercury surface coatings and modifications. Limonitic coat- without significant Ag contents are known, so high ings and leached outer layers are the most common mercury contents (up to 40 wt. % Hg) are obtained types. They result from natural processes in soil and only experimentally (Basu et al. 1981). In Finland, sediments. very high Hg contents, up to 14 wt. %, are known only High purity gold coating is common on the more from electrum occurring as inclusions in arsenopyrite argentiferous nuggets in Ivalojoki placers (Saarnisto of the Rauhala Zn-Cu-Pb sulphide deposit in western & Tamminen 1987). It is understood to form, when Finland (see Kojonen et al. 1988), but this electrum silver and copper are leached away from the outer- contains high amounts of Ag (over 40 wt. %) in Au. most parts, and while gold is recrystallized as micro- Therefore, the chemical composition of the Au-amal- scopic crystallites on the surface (Groen et al. 1990). gam coating on some Ivalojoki gold nuggets shows its Limonite coatings are dark brown and usually pre- man-made origin. served only in cavities. They resemble laterite in Larger nuggets (length up to 4 mm) are only to some chemical composition (Saarnisto & Tamminen 1987): extent coated. The area of the mercury coating on 43-55 % SiO2, 34-39 % Al2O3, 5-20 % Fe2O3, 2-7 % 2 individual nuggets ranges up to 1.4 x 3.2 mm . The TiO2 with some Mn and K. Other representative smaller nuggets are completely coated (Fig. 3). These natural coatings are clayish layers and detrital mineral nuggets range in diameter from 0.6 to 2.4 mm. They grains (usually quartz, feldspars, garnet and are of flake and plate morphology. amphiboles) filling many cavities. The thickness of the coating varies from a very thin coating of only a few micrometers up to about 30 Discussion micrometers. The colour of the coating ranges from light grey N7 to medium light grey N6 (in Munsell). The use of mercury in old time gold mining relied on its low price compared to gold. One gram of gold cost Natural coatings as much as one kilogram of mercury. Because of its low price a lot of mercury was discarded. Amalgama- The gold nuggets without an amalgamated layer tion was performed in the pan itself in the final stages

31 Geological Survey of Finland, Special Paper 36 Kari A. Kinnunen

of panning (McCracken 1983, p. 38-51). Mercury noted from several larger nuggets studied at GTK. was poured into the copper pan in order to improve the The Hg content inside the larger gold nuggets from the recovery of the fine-grained gold (Boericke 1936). In Ivalojoki placer area stays around 0.1 wt. % (anal. Bo California in 1870’s, a mercury layer was also used in Johanson in Kinnunen et al. 1997). In Tankavaara sluice box cavities (Veiga & Meech 1995). This placer gold the Hg content is lower around 0.03 wt. % procedure was based on the fact that the specific (Kinnunen et al. 1998). However, in the Lemmenjoki gravity of mercury is between gold and other heavy placer gold higher Hg contents of up to around 0.8 wt. minerals. Gold, platinum and amalgamated gold sank % have been reported (Kinnunen et al. 1996). In while the other heavy minerals floated away. The southern Finland in Svecofennian domain the Hg method utilized both density separation and amalga- contents are notably higher: in electrum from the mation at the same time. In the pan and sluice Isovesi mineralization 1.3 wt.% Hg and in the Järvenpää methods, the frequent natural limonitic or clayish mineralization 1.2-2.9 wt.% Hg (Luukkonen 1994). coating of the nuggets made the amalgamation proc- However, the number of analysed grains is still limited. ess somewhat ineffective. It may be tentatively concluded that the natural mer- Eetu Savolainen described in 1959 historical gold cury content of native gold in the Ivalojoki area stays working methods to new gold washers in GTK (Per below the average mercury contents in Finnish bed- Olov Jansson, personal communication 2002). Ac- rock gold mineralizations in general. cording to Savolainen, boxes (1 x 1 m) with sheet of Mercury interaction with polluted river water has copper covered with a thin layer of mercury were been tested in laboratory experiments using simulated positioned after the normal sluice boxes in order to gold placers (Miller et al. 2002). It was found that trap the finest gold. Sarlin (1902, p. 16) states that mercury coatings can be formed without actual Hg mercury was sometimes used in the Ivalojoki river in contact on gold grains from polluted river water. sluice boxes in order to recover the more fine grained However, the Hg contents reach only 0.5 wt. % at a gold. Stigzelius (1987) wrote that mercury was used maximum on the surface of the gold nuggets. This in the processing of the bedrock gold at the Kerkelä observations shows that the mercury coated nuggets mine in the year 1902. described in this study from the Ivalojoki placer were However, there seems to be no clearly reported formed in direct contact with mercury. cases in the literature of amalgamation in placer mining in Lapland (cf. Eerola & Eerola 1995). This, together with the rarity of the finds of polluted gold REFERENCES grains, suggest that amalgamation was not in routine Basu, K., Bortnykov, N., Mookherjee, A., Mozgova, N. & use in Ivalojoki compared to, for example, North and Tsepin, A.I. 1981. Rare minerals from Rajpura-Dariba, South America (see Veiga & Meech 1995). The Rajasthan, India II: Intermetallic compound Ag 74.2 Au 16.4

Lemmenjoki and Tankavaara gold fields were oper- Hg 9.4. Neues Jahrbuch für Mineralogie, Abhandlungen 141, ated much later and amalgamation was not popular 217-223. Boericke, W. F. 1936. Prospecting and operating small gold any more since its health risks were by then well- placers. Second edition. New York: Wiley. 145 p. known. Eerola, T. T., Eerola, E.C. & Evelyse, C. 1995. Kullankaivuun Further signs of old prospecting methods have been aiheuttamat ongelmat Lapissa ja Amazoniassa. Summary: detected from nuggets in Lapland. Vuorelainen and Problems occasioned by gold washing in Lapland and Amazonia. Geologi 47 (6), 84-88. Törnroos (1986) noticed that some spherical platinum Groen, J.C., Craig, J.R. & Rimstidt, J.D. 1990. Gold-rich rich nuggets resulted from the roasting in drying of the rim formation on electrum grains in placers. Canadian Min- final concentrate on a steel pan bottom over a flame. eralogist 28, 207-228. It is probable that some gold tellurides and other easily Kinnunen, K. A., Johanson, B., Terho, M. & Puranen, R. 1996. Lemmenjoen alueen Puskuojalta elokuussa 1995 combustible minerals may have similarly transformed löytyneen Iivari-kultahipun (125,95 g) morfologia ja to native gold. However, proof of their existence is pintarakenne, kemiallinen ja mineraloginen koostumus sekä lacking. petrofysikaaliset ominaisuudet. Geological Survey of Fin- Two other points should be discussed in this con- land, archive report, M19/3812/96/1, 18 p. Kinnunen, K. A., Johanson, B., Terho, M. & Puranen, R. nection. The first is the natural background level of 1997. Nondestructive analysis of morhphology, chemical mercury in native gold. The second is the interaction composition and physical properties of large gold nuggets of mercury with placer gold in polluted river water (cf. from Finnish Lapland. Geological Survey of Finland, Special Miller et al. 2002). Paper 23, 29-35. Kinnunen, K. A., Johanson, B, Puranen, R. & Kivekäs, L. The surface chemistry in larger Finnish nuggets is 1998. Tankavaaran Kultamuseon turistihuuhtomolta usually very pure gold and this rim has not been found löydetyn Mopoksi kutsutun kultahipun (38,0 g) mineralogia, to contain any SEM-EDS detectable mercury, as kemiallinen koostumus ja petrofysikaaliset ominaisuudet.

32 Geological Survey of Finland, Special Paper 36 Mercury-rich coating on some gold nuggets from Ivalojoki placers, northern Finland

Geological Survey of Finland, archive report, M16/3742/98/ T. & Volden, T. 1998. Environmental geochemical atlas of 1, 9 p. the central Barents region. Trondheim: Geological Survey of Kojonen, K., Johanson, B. & Törnroos, R. 1988. Ore Norway. 745 p. mineralogy of the Rauhala Zn-Cu-Pb sulphide deposit. Saarnisto, M. & Tamminen, E. 1987. Placer gold in Finnish Geological Survey of Finland, Special Paper 11, 19-42. Lapland. Geological Survey of Finland, Special Paper 3, 181- Luukkonen, A. 1994. Main geological features, metallogeny 194. ?? and hydrothermal alteration phenomena of certain gold and Sarlin, E. 1902. Kultalöydöistä Suomen Lapissa. Suomen gold-tin-tungsten prospects in southern Finland. Geological teollisuushallituksen tiedonantoja 32. 1902. P. 1-30. Survey of Finland, Bulletin 377. 153 p. Stigzelius, H. 1987. Kultakuume. Lapin Kullan Historia. 2. McCracken, D. 1983. Advanced dredging techniques. Volume edition. Helsinki: Suomen Matkailuliitto. 257 p. 2 – Part 2. Los Angeles: Bridge Publications. 164 p. Veiga, M. M. & Meech, J. A. 1994. A brief history of Miller, J. W., Callahan, J. E. & Craig, J. R. 2002. Mercury amalgamation practices in the Americas. In: Brazilian Sym- interactions in simulated gold placer. Applied Geochemistry posium on Ore process and Hydrometallurgy, Rio de Ja- 17, 21-28. neiro, Sept. 3-6, 1995, 581-594. Also: Y. & Törnroos, R. 1986. Man-made Pt-PtAs2 V., Boyd, R., Caritat, P. de, Dutter, R., Finne, T. E., Vuorelainen,spherules after Y. &sperrylite Törnroos, from R. alluvial1986. Man-made deposits in Pt-PtAs2 Finnish Halleraker, J. H., Jæger, Ø., Kashulina, G., Lehto, O., spherulesLapland. Theafter Canadian sperrylite Mineralogist from alluvial 24 deposits (3), 523-528. in Finnish Niskavaara, H., Pavlov, V. A., Räisänen, M. L., Strand, Lapland. The Canadian Mineralogist 24 (3), 523-528.

33 34 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 35– 44 , 2003.

IRON, PHOSPHORUS AND NITROGEN IN FINNISH LAKE SEDIMENTS: THEIR STORE AND LONG-TERM ACCUMULATION

by Hannu Pajunen and Jari Mäkinen

Geological Survey of Finland, P. O. Box 1237, FIN-70211 KUOPIO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): lakes, lake sediments, iron, phosphorus, nitrogen, depositon, concentration, Holocene, Finland

Introduction is carrying out a project that studies the role of lake sediments as a store and sink for carbon. The aim of Lakes are deposition basins for matter transported this study is to estimate the iron, phosphorus and from a drainage basin, precipitated within the lake or nitrogen stores and related accumulation rates and to produced by a lake ecosystem. Lake sediments may give background information on their concentrations. be considered as a permanent sink for many elements, This paper includes results from 81 lakes (Fig. 1). although there is chemical interaction between water and sediment near the sediment surface (e.g. Koyama Methods and data 1990, Thomson et al. 1995, Zhang et al. 1999). The oldest lakes in Finland were formed immediately after In those lakes with a approximate area of about 2 deglaciation and are 12 000 to 10 000 years old. Most km2 or more, acoustic sounding data were collected to of the lakes were isolated from the ancient Baltic Sea estimate the sediment quantity. In smaller lakes this between 10 000 and 6 000 BP as the result of shore- estimation was based on coring and on-site survey. line displacement (cf. Saarnisto 2000). Usually the larger lakes consist of several basins in Finnish lake sediments have been used as archives which sedimentation conditions may differ. Therefore for past environmental changes. There are several the number of cores collected for laboratory analyses paleolimnological studies in which individual lakes vary. Four cores were collected from Lake Inarijärvi, have been thoroughly investigated and models created three from Lakes Pielinen, Oulujärvi and Kallavesi, to describe lake development. The focus of interest two from Lakes Puulavesi, Höytiäinen and Kiantajärvi has been on the sedimentation of iron, carbon, nitrogen and one from every other lake. Altogether 93 cores and phosphorus. Several digestion methods have been were collected. used to study the binding of elements in different The cores were opened and their stratigraphy sediment phases (e.g. Itkonen & Salonen 1994, Itkonen described using the Troels-Smith method. The cores & Olander 1997, Kauppila & Salonen 1997 and Kauppila were divided into 2015 samples, usually 20 cm in et al. 2002). Because of scattered data it has been length. Due to the extent of stratigraphical horizons, difficult to give reliable estimates for the stores and there are exceptional sample lengths locally. Usually related accumulation rates at either a national scale, or the cores extend from the sediment surface to the in a still wider context. glacial sediments and cover the entire lake history. At present, the Geological Survey of Finland (GTK) The level of lake onset was determined using both

35 Geological Survey of Finland, Special Paper 36 Hannu Pajunen and Jari Mäkinen

stratigraphical description and the results of loss on ignition and carbon content analyses. Samples origi- nating from the pre-isolation period were excluded. Each sample was analysed for its water content and loss on ignition, and its density calculated. Iron and phosphorus concentrations were analysed using in- ductively coupled plasma atomic emission spectrometry (ICP-AES), which was carried out after microwave- assisted nitric acid digestion. The efficiency of the leachate is at least the same as in hot aqua regia. The leaching method used in ICP-AES analysis dissolves all salts, iron hydroxides and part of the mineral phases, of which the more significant are sulphides, clay minerals, trioctahedral micas and apatite. The most significant insoluble minerals are quartz, feldspar, muscovite, pyroxenes, amphiboles and magnetite (Räisänen et al. 1992). For clay or silt fractions, the iron concentrations represent about 58 % of the total iron amount. If lake sediment contains abundant iron hydroxides or sulphides, the analysed iron concentration covers even 70 % of the total amount of iron (Räisänen, pers. comm.). Where clay or silt sediment is in question, the analysed phosphorus is a total concentration. The estimate has been made by comparing the XRF- and ICP- analyses of till fines (n = 619) (Tarvainen 1995). In a geochemical mapping project covering 10 Euro- pean countries surrounding the Baltic Sea, it has been found that usually only 4 % of the total phosphorous was extractable by ammonium acetate from top agricultural soils and less than 2 % from subsoils (Reimann et al. 2000, Reimann & Tarvainen, pers. comm.). Thus, the proportion of phosphorus taking part in biological processes is small, only a few percent. Fig. 1. Studied lake basins; their size and location. Location codes: HH -high altitude headwater lake, HD -high altitude drainage lake, Nitrogen concentration was determined with a LECO LH -low altitude headwater lake and LD -low altitude drainage CHN-600 elemental analyser and the results indicate lake. total nitrogen. Pajunen et al. (2000) describe the methods used in more detail. The average stores and accumulation rates for the In each lake the sediment volume and the average total data and for the groups described below were density were used to calculate the store of total dry calculated from the corresponding lake values by matter. The store of each element was obtained from weighting them with the sediment volume. that of total dry matter by using its average concentra- Several dated levels are required to study long-term tion. To obtain comparable results, the stores were variations in the accumulation rates. Two cores from divided by the lake areas and the results given as Lakes Pielinen and Ontojärvi were dated by the kilograms per square metre (relative store). paleomagnetic method while the radiocarbon method The average long-term accumulation rate was cal- was applied to two cores, one from Lake Puulavesi culated by dividing the relative store by the age of the and the other from Lake Mäkijärvi. The usefulness of lake (cal. BP). Lake emergence occurred when the the former method depends on the presence of mag- basin was deglaciated or isolated. The timing of this netic mineral particles whereas the latter is better event was established from the post-glacial history of suited to small lakes. These methods are described the area. Evidence for this has been presented by e.g. by Äikää et al. (1992), Saarinen (1999) and Saarnisto (2000). In this paper long-term accumula- Pajunen et al. (2000). All ages are given in calendar tion rates are given as grams per square metre per years before present (1950). Variations in accumula- year. tion rates indicate variations at the survey site and in

36 Geological Survey of Finland, Special Paper 36 Iron, phosphorus and nitrogen in Finnish lake sediments... its near vicinity. Because the cores were collected low altitude headwater group. from the area of maximum deposition, these rates are A further aim was to compare lake size to the much higher than the relative rates calculated for the geochemical properties of the sediment. The study whole lake. included factor analysis of the material using the sur- Lake size is one of the most important factors face area and the average concentrations of iron, affecting sedimentation conditions. In this study, the phosphorus and nitrogen as variables. The factor analy- lakes were classified into the following five size sis was made using the SPSS software (version 9.0.1) classes: (1) >100 km2, (2) from 100 to 10 km2, (3) from and rotation was carried out with the varimax method. 10 to 1 km 2, (4) from 1 to 0.1 km2 and (5) <0.1 km2 (c.f. Before factor analysis, a logarithmic transformation Raatikainen & Kuusisto 1990). The lake sizes vary was made of the surface area variable of the lakes in from 1090 km2 to 0.03 km2, and average 78 km2. The order to obtain a normalised distribution of it. number of lakes by size class is 17, 14, 22, 20 and 8 respectively. Results The lakes studied were classified into two groups Stores according to their altitude relative to the level of highest post-glacial shoreline minus 30 m. Those lakes The store of iron soluble in nitric acid varies consid- located above this level were classified as high altitude erably from lake to lake (Table 1). The data includes lakes (H) and those below it as low altitude lakes (L). one lake, Lake Pyhäjärvi (Lapinjärvi), where the In this study, the number of high altitude lakes is 40 and relative store is exceptionally high, 97 kg m-2. All other that of low altitude lakes 41. The aim of this division lakes have stores smaller than 50 kg m-2 while the was to separate lakes of clay-dominated areas from smallest stores do not exceed 0.5 kg m-2. The average those of till-dominated areas. However, this division is iron store expressed as a weighted average is 20 kg approximate: small clay areas might occur within the m-2. Large relative stores occur in the southern and drainage basins of the high altitude lakes, especially in eastern parts of the country (Fig. 2). However, the sheltered locations, while, in the drainage basins of the areal distribution of the relative store is not very clear. low altitude lakes, clay areas may be absent. For the size classes >100 km2, 100 - 10 km2, 10 - 1 km2, The lakes were further divided according to their 1 - 0.1 km2 and <0.1 km2, the average iron stores are location within the drainage system. If the area of a 19 kg m-2, 30 kg m-2, 16 kg m-2, 12 kg m-2 and 6.7 kg lake exceeded the total lake area within its drainage m-2 respectively. The largest relative store occurs in basin, it was classified as a headwater lake (H) In this the second size class and, beginning with this, the case the lake itself was not included in the drainage results indicate decreasing store with decreasing size basin. Other lakes were classified as drainage lakes class. At a low altitude the location within a drainage (D). This division was made using statistics on Finnish system does not affect iron store. Of lakes at high drainage basins (Ekholm 1993) and large scale topo- altitude, drainage lakes have larger stores (26 kg m-2) graphic maps. In this data the number of headwater than headwater lakes (13 kg m-2). lakes is 46 and that of drainage lakes 35. The average phosphorus store is 0.45 kg m-2. Lake Using these two divisions the lakes studied were averages vary from 2.2 to 0.023 kg m-2 indicating a divided into the following groups: high altitude hundred-fold difference between the largest and small- headwater lakes (HH), high altitude drainage lakes est store (Table 1). For phosphorus, the largest rela- (HD), low altitude headwater lakes (LH) and low tive store also occurs in the sediment bed of Lake altitude drainage lakes (LD). The number of lakes in Pyhäjärvi (Lapinjärvi) while large stores, around 1.5 each group is 24, 16, 22 and 19 respectively. Most of kg m-2, have also been calculated for Lakes Ruuhilampi the high altitude headwater lakes are situated in the and Postilampi. Large relative stores may occur eastern and northern parts of the country (Fig. 1). throughout Finland (Fig. 3). For the size classes >100 They are usually small, half of them smaller than 1 km2, 100 - 10 km2, 10 - 1 km2, 1 - 0.1 km2 and <0.1 km2, km2. Nevertheless this group does include three large the average phosphorus stores are 0.43 kg m-2, 0.73 lakes: Inarijärvi, Yli-Kitka and Koitere. The high kg m-2, 0.52 kg m-2, 0.58 kg m-2 and 0.26 kg m-2 altitude drainage lakes occur in the same area and respectively. For iron, maximum stores and minimum comprise only two lakes, Kiantajärvi and Ontojärvi, stores occur in the same lake size classes: however the which each slightly exceed 100 km2 in area. The low trend for phosphorous is not as clear. Drainage lakes, altitude headwater and low altitude drainage lakes especially those at high altitude, have larger stores occur in the southern and central parts. Both groups than headwater lakes. include six lakes larger than 100; however lakes in the The average nitrogen store varies from lake to lake low altitude drainage group are larger than those of the but follows a narrower range than the store of iron or

37 Geological Survey of Finland, Special Paper 36 Hannu Pajunen and Jari Mäkinen -1 a -2 g m 0.120.14 0.87 0.56 rate % -2 nitrogen. -1 a -2 0.048 0.20 2.6 0.24 1.0 0.039 0.24 0.63 0.063 0.38 0.028 0.17 0.74 0.068 0.42 0.033 0.21 0.64 0.068 0.43 rateg m % kg m -2 phorus Nitrogen 0.90 0.092 0.14 4.7 0.48 0.75 0.410.620.67 0.0350.28 0.065 0.062 0.18 0.047 0.20 0.300.95 1.7 0.084 1.5 1.7 1.9 0.15 0.15 0.15 0.16 0.10 0.31 0.73 0.46 0.79 6.30.98 0.56 0.68 0.540.46 0.057 0.044 0.15 0.21 1.6 1.7 0.17 0.16 0.43 0.78 0.530.056 0.18 1.7 0.18 0.59 -1 a -2 0.70 4.1 0.25 0.027 0.16 0.86 0.091 0.53 0.60 4.6 0.10 0.0096 0.0731.3 0.12 0.89 rate % kg m g m -2 storekg m lation content store lation content store lation content code Relative Accumu- Average Relative Accumu- Average Relative Accumu- Average district 2 87.8 LD 2.30.22 4.6 0.088 0.0084 0.18 0.26 0.025 0.52 65.1 LH 19 2.0 4.7 0.29 0.031 0.074 2.2 0.23 0.55 44.3LD42.9 7.8 HD 33 0.80 3.2 6.4 0.20 21 0.46 0.020 0.16 0.044 0.57 0.29 1.5 0.059 0.47 0.15 0.97 20.419.9 LD18.2 LD LH 131.34.0 40 0.44 22 0.15 0.0430.131.5 3.7 2.2 0.46 14 7.8 0.71 0.54 0.066 0.054 0.25 0.19 2.1 2.1 0.20 0.21 0.73 0.74 15.512.9 LD5.88 LD4.07 494.01 HD LH 97 HH2.60 24 172.15 8.0 LH2.04 5.2 LD1.73LD HD 4.5 11 0.221.52 2.33.6 28 4.4 0.74 1.8 4.4 44 HH 6.32.2 0.021 1.1 0.45 13 2.30.63 3.5 0.55 0.058 0.39 2.5 0.0335.7 4.7 0.25 2.2 0.73 0.12 0.18 0.86 1.2 4.9 2.8 0.26 8.3 0.15 1.1 0.099 0.077 3.5 0.22 1.2 3.0 0.32 5.7 4.0 0.026 1.0 0.15 0.11 0.65 0.020 0.11 0.132.1 2.8 0.64 0.430.36 0.20 0.25 0.064 0.12 0.21 0.37 0.29 5.1 0.99 0.16 8.30.72 1.0 0.57 3.2 0.088 0.55 0.82 1.1 0.97 0.32 0.77 1090 HH 8.30.74 6.9 0.12 0.010 0.097 0.58 0.051 0.48 km ämäen 21.0 HH 14 1.2 5.2 0.53 emäki 37.8 LH 35 5.5 3.8 tjärvi 9.73HH 7.8 0.68 4.3 0.27 0.023 0.15 1.3 0.12 0.73 tijärvi nnonkoski 153LH 25 2.6 7.9 almi uopioinen appajärvi 142 LH 17 2.8 5.0 aala mlk Pusula 9.10. Nilakka Koitere11. Pyhäjärvi12. Kivijärvi13. Kiantajärvi14. Tervo Viinijärvi Ilomantsi Eura16. Ka Suomussalmi Keurusselkä 17. Ontojärvi Liperi 15318. 164 Vuohijärvi Mänttä 16819. Lestijärvi Kuhmo 154 HD HH LD Valkeala 148 LH Les 23. 118 Muuratjärvi 2 7 2 824. 104 Pieksänjärvi 131.4 LH LH Muurame 1 2 HD Pieks 1 5 31.7 32 5.5 26 2.5 2.4 LH 1.9 0.390.041 6.7 1.5 0.17 1 2 1 3.4 2 2.4 3.3 1.3 9.30.39 1 1 0.30 15 0.38 0.047 0.034 0.081 0.22 2.3 1.2 0.37 0.11 0.63 0.71 20. Kukkia L 15. Lappajärvi L 21. Kostonjärvi22. Sääksjärvi Taivalkoski Kok 7. Suvasvesi8. Yli-Kitka Heinävesi Kuusamo 276 LD 240 HH 6.0 1 1 0.64 1.1 5.2 0.22 8.2 0.35 0.0230.19 0.60 0.033 0.25 0.064 1.2 0.52 4.5. Kallavesi6. Puulavesi Höytiäinen Leppävirta Hirvensalmi Kontiolahti 517 325 291 LD LD LH 11 12 14 1.1 1.1 1.37.925. Karijärvi 0.30 7.1 5.3 J 0.31 3. Oulujärvi Vaala 865 LD 2 4 2.6 6.7 26. Pihlajavesi 27. Kolkonjärvi28. Keyritty Rantasalmi29. Keuruu Nerkoonjärvi 18.8 Iis Rautavaara HH 1.8 0.71 2.5 0.064 0.0061 0.089 0.630.060 0.87 30. 30. Ätäskö31. Pyhäjärvi32. Nurmijärvi 33. Kuonanjärvi 34. Kitee Kevätön Lapinjärvi 35. Rau Uuranjärvi Kerimäki 36. Hossanjärvi 37. Pintamojärvi 38. Multia Siilinjärvi Kätkänjärvi Pudasjärvi 13.0 Suomussalmi39. Ylä-Siikajärvi40. Sääjärvi 3.94 Lehtimäki 3.41 Nilsiä41. HH Vahermanjärvi Nummi- HD LH42. Havanganjärvi43. 14 Haukijärvi Janakkala Virrat 2.32 8.0 6.5 Maaninka LH 1.3 4 0 0.78 3.0 2.4 4.1 0.21 0.12 6.4 0.018 0.012 0.044 0.037 3.5 3.7 0.31 0.36 0.74 1.1 Table 1. Location of lakes and their Lake relative name stores, long-term accumulation rates and concentrations for iron, phosphorus and Outlet Area1.2. Inarijärvi Location Pielinen Iron Inari Eno 871 LD 232.1 Phos 5.8 0.50 0.046 0.131.1 0.099 0.27

38 Geological Survey of Finland, Special Paper 36 Iron, phosphorus and nitrogen in Finnish lake sediments... -1 a -2 g m rate % -2 -1 a -2 rateg m % kg m -2 phorus Nitrogen 0.46 0.0730.071 1.8 0.29 0.28 0.20 0.036 0.047 4.0 0.73 0.96 0.930.089 0.134.0 0.380.57 -1 a -2 0.11 1.30.068 0.0068 0.078 1.2 0.12 1.4 0.17 1.2 0.0230.0020 0.014 2.3 0.20 1.4 rate % kg m g m -2 storekg m lation content store lation content store lation content code Relative Accumu- Average Relative Accumu- Average Relative Accumu- Average district 2 0.040.03LH HH 31 0.37 4.2 3.3 0.033 1.5 0.48 0.16 0.042 0.20 0.0038 4.9 0.055 0.84 0.51 0.076 0.65 1.1 1.40 HD 10 0.86 6.30.41 0.0330.24 2.2 0.18 1.3 1.13HD1.03HH 9.30.98 32 0.850.54 HH0.47 LH 3.0 HH 15 4.6 11 29 5.5 0.66 0.20 1.4 0.49 3.1 0.060 0.019 3.5 0.332.6 0.070 4.3 4.1 0.72 0.24 0.38 0.85 1.7 0.069 1.3 0.035 0.092 0.16 0.17 0.30 0.12 0.60 4.0 2.0 4.3 0.39 0.18 0.47 0.94 1.6 0.61 1.24 HD 131.32.0 0.56 0.056 0.086 4.30.430.66 0.28 LH0.260.25 HH 5.50.21 LH HH 12 3.8 0.56 11 1.1 0.69 3.2 0.99 0.11 4.4 1.5 3.0 0.29 0.24 0.011 1.1 0.026 0.062 0.044 0.10 1.5 0.11 0.095 3.1 0.30 3.8 0.16 4.4 0.56 0.34 0.89 0.40 1.2 1.4 1.2 0.170.15 LD0.150.12 HD0.12 HD 15 LD0.08 HH 19 2.70.06 HH 200.06 3.2 HD0.04 1.6 2.1 HH 1.7 0.26 1.5 HH 1.8 0.28 2.0 1.7 17 0.20 4.9 1.2 1.2 0.13 1.6 2.4 0.18 1.5 0.11 1.8 0.34 0.54 1.4 1.6 0.12 1.30.11 0.15 0.011 0.14 0.035 0.054 0.029 8.4 0.136.5 0.050 0.011 0.014 0.41 0.14 0.0030 0.065 0.17 3.6 0.076 0.131.5 0.67 5.30.50 0.036 5.0 2.8 0.012 2.9 2.0 0.35 0.72 1.4 0.14 0.070 0.50 0.24 0.30 1.6 2.18 0.18 2.1 1.3 0.60 1.4 2.1 0.19 1.1 km iemen iemen almi nkoski ämäen majärvi majärvi imäki upovaara uunupyy 1.32 LD 18 3.3 4.3 uokolahti nontekiö 0.12 HD 4.0 0.37 2.2 0.060 0.0056 0.033 1.4 0.13 0.77 uonenjoki aala 0.33 LH 27 2.6 3.9 mlk mlk mlk kunta Mustalampi 81. PostilampiAverage Nilsiä 20 2.1 7.2 0.45 0.047 0.16 1.5 0.16 0.53 80. Teerilampi Kuhmo Table 1. (cont.) Lake name Outlet 44. Vuontisjärvi Area45. Kinnasjärvi Enontekiö Location 1.43HH Tu Iron 12 1.2 4.4 1.2 Phos 0.12 0.47 2.3 0.23 0.86 46. Tvärasjön Kr 47. Saarijärvi48. Pyhäluoma49. Tervajärvi Saarijärvi50. Pieks Kalliojärvi 51. Muntsurinjärvi Lieksa52. Kylmäjärvi 1.25 Luumäki 53. Sulkuejärvi Juuka 54. Iso-Lyly 55. Suomussalmi HD Puntasjärvi 1.05 1.1556. Kihniö Kypärijärvi57. Kuru Vehmasjärvi HH58. Kaavi Joukkaisjärvi 1 LH 059. Vihti Ylimmäinen S 1.03 Inari 9.30.84 Sammallampi 8.7 0.57 J LH 0.430.0390.14 2.1 0.98 HD 0.35 3.0 4.8 0.76 3.4 HH 0.19 3.1 1.9 0.53 2.5 0.35 0.31 0.69 0.37 2.2 0.033 1.5 0.31 0.032 0.49 0.11 0.11 0.034 3.1 0.045 2.9 0.14 0.22 0.29 1.7 2.7 0.25 0.92 0.19 0.25 0.82 1.2 0.79 69. Ruuhilampi Virtas 70. Tutulampi71. Keskijärvi72. Piilampi73. Lampi Taivalkoski 13060274. Haukilampi Luhanka E 75. Iso Leppäjärvi76. R Tammalampi Kuru77. Ristiina Vittikkolampi Toh 78. Rovan Tuomaslampi 79. Alinen Toh 0.07 HH Töysä 0.49 0.04 LD 0.045 4.7 0.58 0.47 0.11 1.4 0.0098 0.530.052 0.131.5 0.16 0.14 4.4 1.8 0.431.3 60. Paukajärvi61. Vihteljärvi62. Rytijärvi Virrat 63. Mikkeli Kankaanpää Pieni-Montonen 64. Koijärvi65. Rovan 0.32 Kalijärv 0.27 0.3266. Mäkijärvi LD67. Ker Hanhijärvi HD Pedersören LH Kuopio 2 Jämsä 8 6.1 1.1 0.57 4.5 1.6 4.4 0.61 0.057 0.16 3.8 0.36 0.99 68. 68. Talvijärvi Kuusamo 0.17 HH 0.51 0.047 0.26 0.15 0.014 0.074 4.30.40 2.2

39 Geological Survey of Finland, Special Paper 36 Hannu Pajunen and Jari Mäkinen

Fig. 2. Relative iron store. Fig. 3. Relative phosphorus store. phosphorus (Table 1). The average nitrogen store is Long-term accumulation 1.5 kg m-2 and relative stores vary by lake from 8.3 to 0.26 kg m-2. The largest relative stores are in Lakes The stores described above have formed after Sääjärvi, Hanhijärvi, Sääksjärvi and the smallest in either deglaciation or isolation of the basin. The length Lakes Vuohijärvi, Kukkia and Inarijärvi. Small stores of this period varies and covers the last 12 200 years occur especially in the large lakes of eastern Finland in the oldest lake and the last 5 500 years in the (Fig. 4). For the size classes >100 km2, 100 - 10 km2, youngest. 10 - 1 km2, 1 - 0.1 km2 and <0.1 km2, the average stores The long-term accumulation rate for iron varies are 1.3 kg m-2, 3.3 kg m-2, 3.9 kg m-2, 3.6 kg m-2 and considerably from lake to lake resulting in an average 2.3 kg m-2 respectively. The largest relative store rate of 2.1 g m-2 a-1 (Table 1). For the size classes >100 occurs in the size class 10 - 1 km2 and therefore km2, 100 - 10 km2, 10 - 1 km2, 1 - 0.1 km2 and <0.1 km2, diminishes with both increasing and decreasing size the average accumulation rates are 1.9 g m-2 a-1, 3.7 g class. When considering lake location, the low altitude m-2 a-1, 1.8 g m-2 a-1, 1.3 g m-2 a-1 and 0.67 g m-2 a-1 headwater lakes have the largest average store (2.0 respectively. Accumulation rates indicate a decreas- kg m-2) and the high altitude headwater lakes the ing trend except in the largest size class. Headwater lowest (1.1 kg m-2). lakes at low altitude have considerably higher average rates (2.6 g m-2 a-1) than those at high altitude (1.1 g m-2 a-1). Accumulation rates for phosphorus are low com-

40 Geological Survey of Finland, Special Paper 36 Iron, phosphorus and nitrogen in Finnish lake sediments...

uniform data. When considering lake location, the most noticeable difference occurs within the group of headwater lakes. In these, the average rate for low altitude lakes is nearly three times higher than that of high altitude lakes.

Variations in accumulation rates

Data from four lakes studied in more detail indicate continuous accumulation (Fig. 5). Since lake onset, accumulation rates have varied but each lake appears to have its own history. The core from Lake Pielinen indicates the stable conditions of a large lake. Concen- trations of iron, phosphorus and nitrogen vary within a narrow range and the accumulation rate for total dry matter has been quite high but constant, between 110 and 160 g m-2 a-1. Accumulation of the elements studied has continued for 8 000 years at around their average level (Fig. 5). Small variations suggest fluctuations in the deposition rate (mm a-1); however, these variations most probably relate to dating inaccu- racies. In the core from Lake Ontojärvi, accumulation rates for the elements studied are lower than in the previous core and do not indicate any increasing or decreasing tendency. Higher rates in the lowest section indicate intensive deposition of mineral matter during the early phase of lake development. The core from Lake Puulavesi originates from Vuojaselkä basin, which is separated by a shallow strait from the main basins. Therefore the deposition conditions at this sampling site differ from those in a large basin. The profiles for Lake Puulavesi indicate Fig. 4. Relative nitrogen store. constant accumulation rates for iron and phosphorus but decreasing rates for nitrogen (Fig. 5). In the basal pared to those of iron (Table 1). The average long- section the accumulation rate for total dry matter has term rate for phosphorus is 0.047 g m-2 a-1. For the size been twice as high as in the section above. Intensive classes >100 km2, 100 - 10 km2, 10 - 1 km2, 1 - 0.1 km2 accumulation is seen only in the profile for iron. and <0.1 km2, the average accumulation rates are Lake Mäkijärvi is a small high altitude headwaterbody 0.043 g m-2 a-1, 0.086 g m-2 a-1, 0.051 g m-2 a-1, 0.057 g in hilly till landscape. The profiles indicate decreasing m-2 a-1 and 0.027 g m-2 a-1 respectively. Headwater accumulation rates for each element studied. During lakes at high altitude have low accumulation rates and the early phase of lake development, deposition of differ evidently from lakes in other locations. mineral matter washed down from the drainage basin The average long-term accumulation rate for nitro- has been intensive. After this stabilization phase, gen is 0.16 g m-2 a-1 (Table 1). For the size classes stable deposition conditions have prevailed. >100 km2, 100 - 10 km2, 10 - 1 km2, 1 - 0.1 km2 and <0.1 km2, the average accumulation rates are 0.14 g Factor analysis m-2 a-1, 0.40 g m-2 a-1, 0.38 g m-2 a-1, 0.36 g m-2 a-1 and 0.22 g m-2 a-1 respectively. The average rates in the The results of factor analysis are presented in Table largest and smallest lakes are lower than in those lakes 2. The first factor has positive loadings for lake of medium size. Both the maximum (0.98 g m-2 a-1) and surface area and iron but negative loading for nitrogen. minimum (0.025 g m-2 a-1) rates occur in the size class The second factor has positive loadings for phospho- 100 - 10 km2. Within the other size classes, the rus and iron. maximum range is about sevenfold indicating more

41 Geological Survey of Finland, Special Paper 36 Hannu Pajunen and Jari Mäkinen

Fig. 5. Long-term variations in iron, phosphorus and nitrogen accumulation rates established in cores from Lakes Pielinen, Ontojärvi, Puulavesi and Mäkijärvi.

Table 2. Factor loadings of the variables. Loadings under tonnes and that of nitrogen about 82 million tonnes. 0.4 are ignored. Due to the method used, the iron store is about 58 - 70 Factor 1 Factor 2 % of the total store whereas the stores of phosphorus and nitrogen indicate almost total stores. The store of Surface area 0.88 Fe_% 0.56 0.65 carbon calculated using the same method, but using a P % 0.94 smaller database (31 lakes), is about 780 million tonnes N %-0.90 -0.90 (Pajunen 2000). Thus, the store of phosphorus is about 2 % and that of nitrogen about 10 % of the carbon store. Discussion In Finnish lake water the average weight ratio between phosphorus and nitrogen is 1:25 measured Usually, large relative stores correspond to high from epilimnion (Särkkä 1996). The present data accumulation rates and small stores to low accumula- indicate that the corresponding ratio in the sediment tion rates. The difference between stores and rates is bed is much higher, about 1:5. This is partly due to most remarkable when comparing data from the expiration of nitrogen. In this study phosphorus is oldest and youngest lakes. For example, if we assume mainly minerogenic and may not correspond to that of equal accumulation rates, those lakes that were iso- Särkkä (1996). For these elements, the path from lated from the ancient Baltic Ice Lake have much epilimnion to stabilized sediment bed is long and larger relative stores than lakes isolated from the complicated but ultimately phosphorus appears to be Litorina Sea. enriched in the sediment bed. From the present data, it is possible to calculate the The amount of iron accumulated annually has been store and long-term accumulation rate of each ele- about 70 000 tonnes, that of phosphorus about 1800 ment in a national context. These calculations were tonnes and that of nitrogen about 8 800 tonnes. The made according to size classes using the average data amount of phosphorus corresponds to about 40 %, and obtained in this study and the total lake area given by the amount of nitrogen to about 10 %, of the total Raatikainen and Kuusisto (1990). According to the discharge of Finnish rivers into the Baltic Sea in 1991 size classes used in this study (>100 km2, 100 - 10 km2, (Environment Statistics 1994). 10 - 1 km2, 1 - 0.1 km2 and <0.1 km2), the Finnish lake In the data, the negative correlation between lake area is 14 128 km2, 7 227 km2, 5 703 km2, 3 934 km2 size and nitrogen concentration is noteworthy (Factor and 1 671 km2 respectively. 1, Table 2). Same kind of correlation exists between In Finnish lake sediments, the store of iron is about carbon concentration and lake size (Kortelainen 1993, 660 million tonnes, that of phosphorus about 17 million Kortelainen & Pajunen 2000). Thus small lakes are

42 Geological Survey of Finland, Special Paper 36 Iron, phosphorus and nitrogen in Finnish lake sediments... subject to the intensive deposition of humic sub- REFERENCES stances. Contrary to this, to the deposition of iron Äikää, O., Mäntynen, P. & Kankainen, T. 1992. High- appears to be more intensive in large lakes. The performance 14C gas-proportional counting system apply- second factor indicates that the sedimentation of iron ing pulse-shape discrimination. Radiocarbon 34, 414 - 419. and phosphorus is closely connected (cf. Håkanson & Ekholm, M. 1993. Suomen vesistöalueet. Abstract: Drainage Jansson 1983, Jensen et al. 1992). The highest iron basins in Finland. National Board of Waters and Environ- ment, Publications of the Water and Environment Admin- and phosphorus concentrations occur in high altitude istration - series A 126. 163 p. lakes. Thus the factor 2 has a certain regional signifi- Environment statistics 1994. Official Statistics of Finland, cance. Helsinki. 216 p. When environmental factors are considered, the Håkanson, L. & Jansson, M. 1983. Principles of lake sedimentology. Berlin: Springer. 316 p. effect of the concentration and mobility of elements is Itkonen, A. & Salonen, V-P. 1994. The response of sedimen- significant. Thus, in high altitude areas, lake sediments tation in three varved lacustrine sequences to air tempera- containing large iron, phosphorus and nitrogen con- ture, precipitation and human impact. Journal of centrations are, from an environmental viewpoint, Paleolimnology 11, 323-332. Itkonen, A. & Olander, H. 1997. The origin of the hyper- more sensitive to risk than clay-dominated lake trophic state of a shallow boreal shield lake. Boreal Environ- sediments in low altitude areas. ment Research 2, 183-198. Jensen, H.S., Kristensen, P., Jeppesen, E. & Skytthe, A. 1992. Iron: phosphorus ratio in surface sediment as an Conclusions indicator of phosphate release from aerobic sediments in shallow lakes. Hydrobiologia 253, 47-59. The average store of iron, phosphorus and nitrogen Kauppila, T. & Salonen, V-P. 1997. The effect of Holocene is 20 kg m-2, 0.45 kg m-2 and 1.5 kg m-2 respectively. treeline fluctuations on the sediment chemistry of Lake Kilpisjärvi, Finland. Journal of Paleolimnology 18, 145- Since lake emergence, which occurred from 12 200 163. to 5 500 years ago, the average long-term accumula- Kauppila, T., Moisio, T. & Salonen, V-P. 2002. Diatome- tion rate for iron, phosphorus and nitrogen has been 2.1 inferren increase in limnetic phosphorus concentration and g m-2 a-1, 0.047 g m-2 a-1 and 0.16 g m-2 a-1 respectively. the associated changes in sedimentary phosphorus fraction in Valkjärvi, a lake in Kärkölä, Finland. Boreal Environment The average concentrations of iron, phosphorus and Research 7, 27-40. nitrogen are 7.2 %, 0.16 % and 0.53 % respectively. Kortelainen, P. 1993. Content of total organic carbon in In Finnish lake sediments the store of iron is about 660 Finnish lakes and its relationship to catchment characteris- million tonnes, that of phosphorus about 17 million tics. Canadian Journal of Fisheries and Aquatic Sciences 50, 1477-1483. tonnes and that of nitrogen about 82 million tonnes. The Kortelainen, P. & Pajunen, H. 2000. Carbon store in Finnish amount of iron accumulated annually is about 70 000 lake sediments: a preliminary estimate. Geological Survey tonnes, that of phosphorus about 1800 tonnes and that of Finland, Special Paper 29, 83-92. of nitrogen about 8 800 tonnes. Koyama, T. 1990. Gases in lakes, their production mechanism and degassing (CH4 and H2) the earth. In: Durrance, E. M., Nitrogen, together with humic substances, is depos- Galimov, E. M., Hinkee, M. E., Reimer, G. M. & Augusthitis, ited most intensively in small lakes whereas the depo- S. S. (eds.) Geochemistry of gaseous elements and com- sition of iron is more intensive in large lakes. The pounds. Athen: Theophrastus Publications, 271-335. largest iron and phosphorus concentrations occur in Pajunen, H. (ed.) 2000a. Carbon in Finnish lake sediments. Geological Survey of Finland, Special Paper 29, 92 p. high altitude lakes. Pajunen, H. 2000b. Lake sediments: their carbon store and related accumulation rates. In: Pajunen, H. (ed.) Carbon in Finnish lake sediments. Geological Survey of Finland, Spe- Acknowledgements cial Paper 29, 39 - 69. Pajunen, H., Hämäläinen, L., Kankainen, T., Korpijaakko, M., Kortelainen, P., Lehto, O., Saarinen, T., Saarnisto, The cores were collected by several sampling M., Vuorenmaa, J. & Väänänen, T. 2000. Methods. In: teams led by Jorma Ikonen, Hannu Pelkonen and Pajunen, H. (ed.) Carbon in Finnish lake sediments. Geologi- Seppo Putkinen. Jorma Ikonen opened the cores and cal Survey of Finland, Special Paper 29, 7 - 17. Räisänen, M.L., Tenhola, M. & Mäkinen, J. 1992. Rela- prepared them for laboratory analyses. The physical tionship between mineralogy and the physico-chemical and chemical analyses were carried out in the properties of till in central Finland. Bulletin of the Geologi- Geolaboratory, GTK. Radio carbon dating and cal Society of Finland 64, 35-58. paleomagnetic dating were made by workgroups led Raatikainen, M. & Kuusisto, E. 1990. Suomen järvien lukumäärä ja pinta-ala. Abstract: The number and surface by Tuovi Kankainen and Timo Saarinen respectively. area of the lakes in Finland. Terra 102, 97 - 110. Useful comments were given by Tommi Kauppila, Reimann, C., Siewers, U., Tarvainen, T., Bityukova, L., Esa Kukkonen, Marja-Liisa Räisänen and Kimmo Eriksson, J., Gilucis, A., Gregorauskiene, V., Lukashev, Virtanen. We are very grateful to all of them for their V., Matinian, N.N. & Pasieczna, A. 2000. Baltic Soil Survey: Total concentrations of major and selected trace contribution to this paper. elements in arable soils from ten countries around the Baltic

43 Geological Survey of Finland, Special Paper 36 Hannu Pajunen and Jari Mäkinen

Sea. The Science of the Total Environment 257 (2-3), 155- Tarvainen, T. 1995. The geochemical correlation between 170. coarse and fine fractions of till in southern Finland. Journal Saarinen, T. 1999. Palaeomagnetic dating of Late Holocene of Geochemical Exploration 54, 187-198. sediments in Fennoscandia. Quaternary Science Reviews Thomson, J., Higgs, N. C., Wilson, T. R. S., Croudace, J. 18, 889 - 897. W., DcLange, G. L. & Van Santvoort, P. J. M. 1995. Saarnisto, M. 2000. Shoreline displacement and emergence of Redistribution and geochemical behaviour of redox-sensi- lake basins. In: Pajunen, H. (ed.) Carbon in Finnish lake tive elements around S1m the most recent eastern Mediter- sediments. Geological Survey of Finland, Special Paper 29, ranean sapropel. Geochimica Cosmochimica Acta 59, 3487- 25 - 34 . 3501. Särkkä, J. 1996. Järvet ja ympäristö, limnologian perusteet. Zhang, M., Davison, W. & Ottey, C. 1999. Remobilization [Lakes and environment, limnological basics]. Tampere: of major ions in freshly deposited lacustrine sediment at Gaudeamus. 157 p. (In Finnish) overturn. Aquatic Sciences 61, 354-361.

44 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 45– 52 , 2003.

BARENTS ECOGEOCHEMISTRY - A LARGE GEOCHEMICAL BASELINE STUDY OF HEAVY METALS AND OTHER ELEMENTS IN SURFICIAL DEPOSITS, NW-RUSSIA AND FINLAND

by R. Salminen1), I. Bogatyrev3), V. Chekushin3), S. P. Glavatskikh2), V. Gregorauskiene4) H. Niskavaara6), L. Selenok5), M. Tenhola7) and O. Tomilina3)

1)Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND 2)Arkhangelskgeolrazvedka, ARKHANGELSK, RUSSIA 3)S/C Mineral, St. PETERSBURG, RUSSIA 4)Geological Survey of Lithuania, VILNIUS, LITHUANIA 5)JSC Mireko, Syktyvkar, KOMI REPUBLIC, RUSSIA 6)Geological Survey of Finland, P.O. Box 77, FIN-96101 ROVANIEMI, FINLAND 7)Geological Survey of Finland, P.O. Box 1237, FIN-70211 KUOPIO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): geochemical surveys, stream water, soils, Bryophyta, chemical elements, heavy metals, baseline studies, human activity, Russian Federation, Finland, Barents region

General background of the project Monchegorsk, Arkhangelskgeolrazvedka from Arkhangelsk, S/C Mireko from Syktyvkar, Voeikov From 1999 to 2003 a multipurposemultipurpose regional geo- Main Geophysical Observatory from St.Petersburg, chemical mapping project, “Ecogeochemical Map- VNIIOkeangeologia from St.Petersburg and the ping of Eastern Barents Region – Barents Eco- Geological Survey of Norway. In addition to these geochemistry”, will will bebe carried out jointlyjointly byby scientistsscientists main partners, many universities and research insti- from Finland, Russia and Norway. During the project tutes are participating in the project. The main finan- several different sampling media such as surface ciers of the project are the Ministry of Environment of water, terrestrial moss, organic and minerogenicminerogenic soils Finland, Ministry of Trade and Industry of Finland, are collected. The project project area area encompasses encompasses Finland Finland Ministry of Natural Resources of Russian Federation, and the NW-part of Russia (????????(ɋɚɞɦɢɧɟɧet etal. al. 2001). 2001). It Geological Survey of Finland and the participating isIt an is extension an extension of the of Kola the Ecogeochemistry Kola Ecogeochemistry project organizations. (Reimannproject (Reimann et al. 1998) et al. carried 1998) carriedout 1992-1997, out 1992-1997, which An important aim of the project is to define the whichdocumented documented levels and levels sources and sources of up to of more up tothan more 50 anthropogenic impact in relation to the natural varia- thanchemical 50 chemical elements elements including including radionuclides radionuclides in the cen- in tions in regional geochemical baselines of heavy thetral parts central of partsthe Barents of the Region. Barents At Region. the same At thetime, same the metals and other elements over a very large area time,data produced the data produced will be an will important be an important contribution contribu- to the containing several of the largest industrial emitters in tionIUGS/IAGC to the IUGS/IAGC Global GeochemicalGlobal Geochemical Baselines Baselines Pro- Europe but also some of its most pristine areas. The Programmegramme (Darnely (Darnely et al.et al.1995, 1995, Plant Plant et al.et al.2000). 2000). study area covers 1,500,000 km2 from Kittilä in The project is conducted by the Geological Survey Finland to the Ural Mountains in NW-Russia and from of Finland. The other main partners are S/C Mineral the Barents Sea in the North to St.Petersburg, includ- from St.Petersburg, Central Kola Expedition from ing the whole territory of Finland.

45 Geological Survey of Finland, Special Paper 36 R. Salminen, I. Bogatyrev, V. Chekushin et al.

Methods terrestrial moss in the project area. First results of the regional phase, including some anion, main element Stream sediment, stream water, terrestrial moss, and heavy metal concentrations of stream waters, humus and C-horizon soil samples were collected in element and some radionuclide concentrations of 2000-2001 from 1,085 sampling sites in Russia and organic soil layer and element concentrations of ter- 288 in Finland, giving an average density of one site restrial mosses are now ready. per 1 000 km2. Samples from vegetation such as tree As an example of the new regional geochemical and shrub layer and complete soil profiles were also maps, the distribution of arsenic in stream waters are collected from 30 special sampling sites in the whole shown in Figure 1. The map shows that the main project area. Monthly precipitation samples were geological features, such as some small zones of collected during the 12 months from May 2000 to June hydrothermal ore deposits in eastern and northern 2001 close to these special sites. An even larger Finland or larger Permian sedimentary sulphate-lime- variety of sampling materials (altogether more than stone rocks in central Russia from Kaninin peninsula 1000 samples) were collected during the pilot phase in to Kotlas and Vologda, are well reflected in the 1999 from the nine catchments (Salminen 2000). geochemistry of stream waters. Anthropogenic influ- The most modern analytical methods, such as ICP- ence, nevertheless, has changed the quality of stream MS and ICP-AES, are used to analyse the samples water in some place, such as the densely populated with very low detection limits, and the XRF method is and industrialized areas in southern Finland, the Len- used for minerogenic samples, too. The main part of ingrad oblast and the whole southern part of the the analytical work is done in the laboratory of the project area, in the vicinity of Arkhangelsk and Vorkuta Geological Survey of Finland. Part of the water and the immediate surroundings of the mining industry analysis was done in the Geological Survey of Nor- in the Kola area. way. Concentrations of more than 50 elements, The distribution of 134Cs-isotope concentrations in radionuclides, PAH’s and PCB’s will be determined. the organic soil layer (Fig. 2) still reflect well the Different extraction methods are used for humus and deposition from Chernobyl accident. The strongest minerogenic materials in order to study the speciation fall-out came to the southern Finland and Leningrad and bioavailability of elements. region, but part of it continued to central Karelia and Results from the pilot phase are documented as also reached the Arkhangelsk region. Although pluto- Technical reports of the Geological Survey of Finland nium isotopes were analysed only from 30 samples, and they are also available as CD-ROMs (Salminen the traces from Chernobyl were found from them in 2000). Based on the experiences from the pilot phase, Finland, too. The older nuclear power tests could be a very detailed field manual for the regional phase traced by the 137Cs isotope concentrations. sampling, both in English and in Russian, was com- Until now results from terrestrial moss (Hylocomium piled (Gregorauskiene et al. 2000). Nineteen digital sp. or Pleurozium sp.) are also available. The distri- base maps were also compiled covering the whole bution of elements, especially heavy metals in mosses, project area. They describe the background informa- describe the abundance of air borne elements. It is tion for the interpretation of the results including e.g. commonly believed that geochemical anomalies in maps of bedrock lithology, Quaternary sediments, soil mosses describe long distance transport. Our results, types, vegetation zones, morphology, human activi- however, show clearly that in the Barents region local ties, metallogenic zones, airborne geophysical data sources are more important. The sources can be and meteorological data (Bogatyrev et al. 2000). anthropogenic, as in the vicinity of the Montchegorsk smelters or the cities of Vorkuta and Arkhangelsk, Results where the highest Ni and also Cu concentrations exist (Fig. 3). But the origin may also be geogenic in the The geochemical processes prevailing in surficial areas where vegetation is weak as in the Ural moun- deposits including surface water, minerogenic and tains or generally in the tundra area (Fig. 3). Our organogenic soils, as well as, the vegetation zone, results also show that sulphur emissions from the were studied on the basis of data from the pilot phase Monchegorsk smelters have decreased because of (see e.g.e.g. (ReimannReimann etet alal 2001a2001a and 2001b). SeveralSeveral decreasing production (Fig. 4), and the S concentra- other publications are still in preparation based on this tions of mosses are no longer very anomalous. same data. The precipitation samples were collected monthly The main aim of the project is, however, to present from June 2000 to July 2001. The data of heavy metal the regional distribution of abundances of elements concentrations in precipitation is quite unique in Rus- and chemical compounds in the surficial deposits and sian territory. In Figure 5 are shown the results of

46 Geological Survey of Finland, Special Paper 36 Barents Ecogeochemistry - a large geochemical baseline study of heavy metals and other elements ... ere collected in 2000 (western part) and 2001 (Kola area and the eastern part of the project area.) Fig. 1. Arsenic concentrations in the stream water samples reflect mainly geochemistry of the major units of bedrock. Samples w

47 Geological Survey of Finland, Special Paper 36 R. Salminen, I. Bogatyrev, V. Chekushin et al. Cs concentrations in the organic soil layer. 134 Fig. 2. The fall-out from the Chernobyl accident can still be detected by the distribution of

48 Geological Survey of Finland, Special Paper 36 Barents Ecogeochemistry - a large geochemical baseline study of heavy metals and other elements ... eogenic sources in mountain and tundra areas. Fig. 3. In addition to the local anthropogenic pollution nickel concentrations in the moss samples show the distribution from g

49 Geological Survey of Finland, Special Paper 36 R. Salminen, I. Bogatyrev, V. Chekushin et al. d emissions from the Kola Fig. 4. Sulphur concentrations in the moss metal samples industry show mainly is anthropogenic seen pollution as in densely low populated concentrations. areas. The decrease

50 Geological Survey of Finland, Special Paper 36 Barents Ecogeochemistry - a large geochemical baseline study of heavy metals and other elements ...

Fig. 5. The results of factor analysis from the geochemical data of precipitation over a one year period classify different sources (Salminen, Vernigora et al. 2002). Factor 1 characterizes heavy metals from smelters in the Kola region; factor 2 is connected to human activities generally and especially to agriculture (Leningrad region and Finland); factor 3 is a consequence of sea spray; factor 4. describes emissions from Kandalaksha F, Al industries and factor 5 characterizes pollution from the dusty component of large metallurgical industrial enterprises (Vorkuta, Monchegorsk) factor analysis from the data covering the whole one REFERENCES year period. The factors classify the pollution sources Bogatyrev, I., Yegorov, A., Chekushin, V., Zhdanova, L., and show again that the main source of pollution in the Lavretsova, A., Tenhola. M., Korhonen, J. & Reimann, rain water is normally very local, such as sea spray at C. 2000. Digital basemaps for the computer database of the the seaside, metal industry (different types can be joint Russian-Finnish-Norwegian project of Ecogeochemical separated in some cases) in its vicinity, agriculture, and mapping in the eastern Barents region in 1999-2003. Pro- ceedings of International Conference GIS Sustainable Devel- normal dust. The content of pollutants in precipitation opment of Territories, Vol. 1. Apatity, Russia. displays quite a strong seasonal variation. Darnley, A.G., Björklund, A., Bölviken, B., Gustavsson, N., Koval, P.V., Plant, J.A., Steenfelt, A., Tauchid, M., Conclusions & Xie Xuejing 1995. A global geochemical database for environmental and resource management. Final report of IGCP Project 259. UNESCO Publishing, Earth Sciences 19. The results which until now are available show that 122p. local basic geology has a strong influence in element Gegorauskiene, V., Salminen, R., Reimann, C. & distribution in stream waters, and also in mosses in the Chekushin, V. 2000. Field Manual for Barents Eco- geochemistry project. Geological Survey of Finland, unpub- areas where the vegetation is not too dense. Anthro- lished report S/44/0000/2/2000, 54 p., 5 app. pogenic activities have a strong local influence in both Plant, J.A., Smith, D., Smith, B., & Williams, L. 2000. water and moss, and they show clearly the type of Global geochemical baselines: the sustainability of the earth’s pollution occuring. However, the results do not support life support systems and human health. [Electronic resource] In: 31st International Geological Congress, Rio de the idea of long distance airborne transport of heavy Janeiro, - Brazil, August 6-17, 2000: Abstracts Volume. metals to the Arctic regions. Instead, local pollution Geological Survey of Brazil. Optical disc (CD-ROM). diate vicinity. Reimann, C, Äyräs, M., Chekushin, V., Bogatyrev, I.,

51 Geological Survey of Finland, Special Paper 36 R. Salminen, I. Bogatyrev, V. Chekushin et al.

Boyd, R., de Caritat, P, Dutter, D., Finne, T.E., ɧɨɜɵɟ ɮɨɧɨɜɵɟ ɝɟɨɯɢɦɢɱɟɫɤɢɟ ɞɚɧɧɵɟ ɫ ɫɟɜɟɪɨ ɡɚɩɚɞɚ Halleraker, J.H., Jäger, O., Kashulina, G., Lehto, O., Ɋɨɫɫɢɢ. ɉɪɢɤɥɚɞɧɚɹ Ƚɟɨɯɢɦɢɹ. Ɇɢɧɢɫɬɟɪɫɬɜɨɩɪɢɪɨɞɵɯ Niskavaara, H., Pavlov, V., Räisänen, M.L., Strand, & ɪɟɫɭɪɫɨɜ Ɋɨɫɫɢɣɫɤɨɣ Ɏɟɞɟɪɚɰɢɢ, Ɋɨɫɫɢɣɫɤɚɹ Ⱥɤɚɞɟɦɢɹ T., Volden, T. 1998. Environmental Geochemical Atlas of ɧɚɭɤ, ɂɧɫɬɢɬɭɬ ɦɢɧɟɪɨɥɨɝɢɢ, ɝɟɨɯɢɦɢɢɢɤɪɢɫɬɚɥɥɨɯɢɦɢɢ the Central Barents Region. NGU-GTK-CKE Special Pub- ɪɟɞɤɢɯ ɷɥɟɦɟɧɬɨɜ (ɂɆȽɗ), ɜɵɩ. 2, 169-177. lication, Grytting AS. 745 p. Salminen, R. 2000. Results of the catchment stage of BARENTS Reimann, C., Koller, F., Kashulina, G., Niskavaara, H. & Ecogeochemistry project– summary of technical reports. Englmaier, P. 2001a. Influence of extreme pollution on the Geological Survey of Finland, unpublished report S/41/ inorganic chemical composition of some plants. Environ- 0000/1/2000. 14 p. mental Pollution 115, 239 – 252. Salminen, R., Vernigora, N., Polischuok, A., Chestyakova Reimann, C., Koller, F., Frengestad, B., Kashuylina, G. M. & Tomilina, O. 2002. Heavy metal Concentrations of Niskavaara, H. & Englmaier, P. 2001b. Comparison of Precipitation and their Seasonal Variation at Thirty Monitor- the element composition in several plant species and their ing Stations in the Barents Region in NW Russia and Finland. substrate from 1 500 000 km2 area in Northern Europe. The The Second AMAP International Symposium on Environ- Science of the Total Environment 278, 87 – 112. mental Pollution of the Arctic. Extended abstracts. AMAP ɋɚɥɦɢɧɟɧ, Ɋ.Ƚɪɟɝɨɪɚɭɫɤɟɧɟ, ȼ. Ɍɟɧɯɨɥɚ, Ɇ. & ɑɟɤɭɲɢɧ, Report 2002:2, P – M18. (Available also as electronic version ȼ. 2001. ɉɪɨɟɤɬ «ɗɤɨɝɟɨɯɢɦɢɹ Ȼɚɪɟɧɰɟɜɨɝɨ ɪɟɝɢɨɧɚ»– http://www.amap.no/symposium2002/index.html)

52 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 53– 59 , 2003.

GEOCHEMISTRY OF LOCAL GROUND WATER IN RELATION TO THE INCIDENCE OF CHRONIC DISEASES

by Anne Kousa and Maria Nikkarinen

Geological Survey of Finland, P.O. Box 1237, FIN-70211 KUOPIO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): medical geology, geochemistry, ground water, drinking water, hydrochemistry, trace elements, Bayesian analysis, Finland

Introduction elements and major elements in ground water. The most important single cardiovascular disease Geological Survey of Finland (GTK), the Kuopio is CHD, including acute myocardial infarction (AMI). unit and National Public Health Institute (KTL), De- Our recent study of the spatial distribution of the first partment of Epidemiology and Health Promotion (Hel- AMI event showed that despite the decreasing trend sinki) have carried out a study of the spatial variation in AMI incidence, the geographical difference in of some chronic disease incidence and geochemical incidence and high-risk areas remain (Karvonen et al. compounds in the ground water. Case data and popu- 2002). The spatial pattern of AMI incidence showed lation data processing and statistical analysis were an increasing risk from the south-west to the north- performed at KTL and the geochemical data process- east (Fig.1). The presence of high-risk areas for AMI ing was performed at GTK. The study group and the suggests that certain genetic or environmental risk steering group consist of researchers from many factors have accumulated in certain geographic loca- different scientific branches and include geographers, tions in Finland. There were indications that death statistical experts, geologists and medical and public from, or development of CHD was connected to the health professionals. quality of the water, particularly with low concentra- The rates of coronary heart disease (CHD) mortal- tions of constituents (Punsar et al. 1975). ity and morbidity and childhood type 1 diabetes (DM1) The incidence of type 1 diabetes in Finnish children are among the highest in the world in Finland (Uemura aged 14 years or under is the highest in the world and & Pisa 1988, Kuulasmaa et al. 2000, Karvonen et al. is constantly increasing at the rate of nearly 3 % per 1993). Also the occurrence of DM1 and CHD are year (Karvonen et al. 2000, Onkamo et al. 2000, known to have a large geographical variation in Fin- Tuomilehto et al. 1999). Geographical small area land (Karvonen et al. 1997, Kannisto 1947, Tuomilehto studies have shown a clear within-country variation in et al. 1992). The recent advances in GIS, the availabil- the risk of type 1 diabetes among children in Finland ity of geo-referenced data and the developments in (Karvonen et al. 1997, Rytkönen et al. 2001). Al- spatial methodology are valuable tools for the study of though the etiology of type 1 diabetes is not fully medical geology. Our study group examined the asso- understood, according to recent knowledge, both ge- ciation of acute myocardial infarction (AMI) and netic and environmental factors operate together, childhood type 1 diabetes (DM1) incidence with trace leading to an uncontrolled attack by the immune

53 Geological Survey of Finland, Special Paper 36 Anne Kousa and Maria Nikkarinen

A. B.

Fig. 1 Risk of AMI among 35-74 year old men in Finland in 1993. A. Posterior mean age-standardized incidence. B. Posterior probability of the risk exceeding the overall country risk (Karvonen et al. 2002). system on the insulin-producing beta-cells (Tuomilehto- using small areas, defined according to map coordi- Wolf & Tuomilehto, 1991, Cudworth et al. 1979, nates, offer an opportunity to avoid these problems. Verge et al. 1994). There is accumulating evidence The aim of this paper is to present recent studies of that the metabolism of several trace elements is medical geology carried out at GTK in collaboration altered in diabetic patients and that such nutrients with the National Public Health Institute using data might have a role in the pathogenesis and progression aggregated into 10 x 10 km grid cells. of the disease (Tuvemo et al. 1983-85, Underwood 1971). In Sweden, a low-level of zinc in the drinking Study area: geological characteristics water was associated with an increased incidence of type 1 diabetes (Haglund et al. 1996). The bedrock of Finland is mainly composed of silica The mineral composition of soil has a clear impact rich and calcium poor crystalline granitic rocks on water quality (Lahermo et al. 1990). Elements in (Korsman et al. 1997). The bedrock is overlain by a the natural environment known to be associated with glacial overburden of about seven metres of average human health can be distinguished as major- and trace thickness (Koljonen & Tanskanen 1992). The compo- elements. The first group includes sodium, potassium, sition of trace elements in the glacial sediment cover is chlorine, calcium and magnesium. Concentrations of not homogenous. Certain trace element associations the major elements in humans are roughly between characterize different geological regions. Based on 0.03 and 0.2 % (ICRP 1974). All others are present in the co-occurrence of elements, the country can be smaller concentrations and are therefore called trace divided into geochemical provinces (Koljonen 1992). elements. All trace elements are toxic if ingested or In Finland, two types of aquifers are used as drinking inhaled in sufficiently high quantities for long enough water supplies: (1) Quaternary deposits such as sandy periods of time (Plant et al. 1996). Selenium, iron, till and glaciofluvial gravel and sand deposits and (2) fluoride and molybdenum are examples of elements fracture zones in bedrock (Tarvainen et al. 2001). In which show a relatively narrow concentration range Finland, the groundwater is slightly acidic and very soft between the essential and toxic levels. (1-4 ºdH) or soft (4-8 ºdH) (Tarvainen et al. 2001). Traditional regional analyses carried out within Regionally, the hardest groundwater is met in the administrative areas suffer from the loss of informa- southern Finland coastal belt, while the softest waters tion or large random variation of the estimates and are encountered in northeast Finland. Besides the misinterpretation of the results. Analyses carried out geological factors affecting trace element composition

54 Geological Survey of Finland, Special Paper 36 Geochemistry of local ground water in relation to the incidence of chronic diseases

(radon, fluoride, nickel, copper etc.), atmospheric and The data on men aged 35-74 years with the first anthropogenic factors also contribute to the chemical AMI attack (18946 cases) in the years 1983, 1988 and composition of the ground water (Lahermo et al. 1993 were obtained from the nation-wide Death Reg- 1990). Nitrate is one of the most sensitive indicators of ister and the Hospital Discharge Register. The data on human activities. population at risk, provided by coordinates of the place Marine factors, such as sea spray and relict sea salts of residence, were obtained from Statistics Finland. In in the overburden and in the fracture zone of bedrock, this analysis the data on AMI cases from these three increase the concentrations of dissolved components cross sectional years were pooled together. in the ground water. Thus well water concentrations, Data on the incidence of childhood type 1 diabetes for example, of chloride, sulphate, sodium and water (aged 0-14 years) nation-wide were obtained from the hardness are higher in the coastal area than inland Prospective Childhood Diabetes Registry for the pe- (Lahermo et al. 1990). riod 1987-1996 (3649 cases). Since 1987 all the newly diagnosed cases have been registered in the Prospec- Materials and methods tive Childhood Diabetes Registry with a high level of case verification. The population data were obtained Geochemical data from the National Population Registry, which is up- dated continuously by Statistics Finland. The geochemical data were obtained from the The geo-referenced data sets (point data structure), hydrogeochemical database of GTK. The data on both the population at risk and case data, were con- - - verted into grid structure and aggregated into 10 x 10 total water hardness (ºdH), Ca, Mg, Fe, F , NO3 (mg/ l) and Cu, Zn and Al (µg/l) were available. The total km grid cells to ensure the protection of privacy of the water hardness was calculated by the formula (0.14 individuals. x Ca (mg/l)) + (0.23 x Mg (mg/l). Element concentrations were determined with different methods, e.g. Statistical methods ICP-MS, ICP-AES, ionography and AAS. Where the analytical methods in different sampling periods were The Bayesian spatial conditional autoregressive not comparable with each other, only the latest ana- model (CAR) with covariates, which is currently in lyse was included in the study. The original data wide use in the field of disease mapping, was applied contained from 3621 up to 12401 samples taken here (Ranta & Penttinen 2000, Osnes & Aalen 1999, mainly from dug wells and wells drilled in the bedrock. Clayton et al. 1993, Besag et al. 1991). The geochemical point data were interpolated into Because Finland is sparsely and unevenly inhabited, a regular 10 x 10 km grid by using the ALKEMIA we propose one modification, which is pertinent to the Smooth interpolation method (Ahlsved et al. 1991). sparsely populated areas. In the case of the 10 km x 10 Data conversion, linking, modifying and outputs were km grid over Finland (excluding Lapland), some grid done using ArcView and ArcInfo GIS software cells are empty and have to be omitted from the (version 8.0) in a PC and Unix environment. WinBUGS analysis; thus 5% of cells would be omitted. However, statistical software (Spiegelhalter et al. 1996) was once we take environmental factors into account, also used together with GIS for data modifying proce- assuming that the disease risk is influenced by both dures. demographic factors (i.e. people who actually live Finland is sparsely inhabited and only a quarter of within the grid cell) and environmental factors in each the population lives in the thinly populated area that cell whether or not it is inhabited, the omission of covers 95 % of the total area of Finland and 50 % of unpopulated cells result in the loss of information. the population lives in the urban areas (Rusanen et al. 1995). Because of the very low population density, Results and discussion cases and geochemical samples in northern Finland in the province of Lapland have been excluded from the Bayesian modeling of AMI and DM1 inci- analysis. dence and geochemical covariates

Geo-referenced data Age group and the geochemical elements such as total water hardness, Ca, Mg, Fe, F-, Cu, Al, Zn and Every resident in Finland has a unique personal - NO3 concentration in the ground water were in- identity number. Using this number, 95% of men with cluded in the analyses as the covariates. In the entire AMI and all children with diabetes were located at the country, the overall age-adjusted incidence of AMI time of diagnosis according to the map co-ordinates. (cross-sections years 1983,1988,1993 pooled) among

55 Geological Survey of Finland, Special Paper 36 Anne Kousa and Maria Nikkarinen

men aged 35-74 years was 480/100 000/year. The Table 1. The estimated effects of the geochemical covariates on the incidence of first AMI among 35-74 year old estimates of the effect of geochemical covariates in men in Finland. the ground water on the variation of the incidence of AMI are shown in Table 1. One unit (°dH) increment Element Posterior mean 95 % HDR in water hardness decreased the risk of AMI by 1 % Tot. water (Kousa et al., al., manuscript). submitted). TheThe levelslevels ofof other ele- hardness (ºdH)* -0.0097 (-0.0214, -0.0003) Zn (µg/l) -0.0007 (-0.0061, 0.0048) ments in the ground water included in this study did not Al (µg/l) -0.0003(-0.0007, 0.0002) have any additional effect on the spatial variation and Cu (µg/l) 0.0401 (-0.0653, 0.1477) F (mg/l) -0.0317 (-0.1453, 0.0899) in the incidence of AMI. Fe (mg/l) 0.1015 (-0.1298, 0.3176) NO (mg/l) 0.0006 (-0.0004, 0.0016) One unit (mg/l) increase in the concentration of 3 - * NO3 in the ground water resulted, on average, in 0.3% statistically significant increase in the risk of type 1 diabetes (Moltchanova et (Posterior mean column describes the effect of the geo- al., submitted). However, the increase was not statis- chemical element and the sign before value the direction tically significant at the 95% level. The composition of of the effect (e.g. one unit increment of Cu on average increases the AMI risk by 4 % (Cu = 0.0401). 95% HDR the ground water included in this study did not have column describes the statistical significance. If both of the any significant effect on the incidence variation of limit values have the same sign the result is statistically diabetes and spatial difference in incidence. significant). The geographical variation and changes in the the disagreement in this association in earlier studies incidence of AMI and type 1 diabetes in Finland may be related to the variation in methodological cannot be explained by individual lifestyle or genetic issues. factors alone; environmental exposures must also Fluoride (F-) concentrations of around one ppm contribute to the development of the disease. We (part per million) in household water may be beneficial carried out the most detailed ecological analysis to (Luoma et al. 1983). In our pilot study we reported investigate the putative association between the con- that low F concentration was a characteristic centration of trace elements and major elements in the geochemical feature in the high CHD mortality area ground water and the incidence of AMI and type 1 (Kousa & Nikkarinen 1997). In the present study one diabetes in Finland ever done in any population. mg/l increment in the F- concentration in the drinking The age distribution of the population did not have water was associated with a 3 % decrease in the risk an effect on the geographical variation in the incidence of AMI. The differences were not, however, statisti- of AMI. The results of our research support the early cally significant. Recent studies have provided evi- observations of the inverse relationship between the dence that high serum iron and copper (Salonen et al. AMI incidence and total water hardness. The other 1991 and 1992, McMaster et al. 1992) and low serum investigated elements in the ground water (well wa- zinc levels are associated with the CHD (Reunanen ter) included in this study did not have a significant et al. 1996). Iron and copper have been suspected to effect on the spatial difference in AMI incidence. induce atherosclerosis by promoting the oxidation of An inverse relationship between water hardness lipids (Salonen et al. 1992). In our study one µg/l and CHD mortality has been detected in several increment in copper and one mg/l increment in iron on studies (e.g. Crawford 1968 et al., Karppanen 1978 et average increased the risk of AMI by four and ten al., Nerbrand 1992 et al., Rylander 1991 et al., Piispanen percent, respectively, although these findings were 1993). Several studies have suggested that CHD not statistically significant. The non-significant results mortality can be related to the amount of magnesium in our study may be due to excessive smoothing in drinking water (mm. Rylander et al. 1991, Punsar & technique. Thus, our study provides further, though Karvonen 1979, Anderson et al. 1975, Luoma et al. relative weak evidence of the importance of the 1983, Kousa & Nikkarinen 1997). Rubenowitz et al. ground water fluoride, iron and copper concentrations (2000) reported that magnesium in drinking water was for the risk of AMI. associated with lower mortality from CHD but not The studies of the role of nitrate or zinc in the with the incidence of AMI. aetiology of type 1 diabetes are few but the results In some studies a clear association between cardio- have been widely discussed (Haglund et al. 1996, vascular disease and water hardness or magnesium Virtanen et al. 1994, Van Maanen et al. 1999, Casu et concentration in drinking water was not found (Huel al. 2000). However, thus far the results from earlier et al.1978, Smith et al. 1987, Maheswaran et al. 1999). studies have been contradictory, possibly because of No significant differences were observed in serum the complexity of the ecological analysis and the calcium and magnesium levels in the Finnish case- difficulty to apply results from ecological studies at control study, either (Reunanen et al. 1996). Much of the individual level (Moltchanova et al., manuscript).

56 Geological Survey of Finland, Special Paper 36 Geochemistry of local ground water in relation to the incidence of chronic diseases

Ecological studies describe the association be- REFERENCES tween a set of average variables defined in groups of individuals over geographically defined areas. It is Ahlsved, C., Lampio, E. & Tarvainen, T. 1991. ALKEMIA – a VAX minicomputer database and program package for important to recognize that these studies use aggre- geochemical exploration. Journal of Geochemical Explora- gate data and they describe only the relationship tion 41, 23-28. between an incidence of disease and the average Anderson, TW., Neri, LC., Schreiber, GB., Talbot, FD. & Zdrojewski, A. 1975. Ischemic heart disease, water hard- level of exposure to an environmental risk factor, but ness and myocardial magnesium. A letter. Canadian Medical not the causative role of the factor. CHD and type 1 Association Journal AUG 9;113 (3), 199-203. diabetes have a multifactorial etiology. Therefore the Anderson, R. 2000. Chromium in the prevention and control method of spatial analysis used in this study is appro- of diabetes. Diabetes & Metabolism Feb 26 (1), 22-7. Besag, J., York, J. & Mollié, A. 1991. Bayesian Image priate for testing the impact of several factors simul- Restoration, with two applications in spatial statistics. taneously. The validity of the method used in this study Annals of the Institute of Statistical Mathematics 43,1-59. has been demonstrated earlier (Ranta & Penttinen Casu, A., Carlini, M., Contu,A., Botazzo, GF. & Songini, 2000, Rytkönen et al. 2001, Karvonen et al. 2002). M. 2000. Type I diabetes in Sardinia is not linked to nitrate levels in drinking water. Diabetes Care 23,1043-44. Additional simulations have been run to check the Clayton, DG., Bernardinelli, L. & Montomoli, C. 1993. validity of the proposed alterations to it regarding the Spatial correlation in ecological analysis. International Jour- inclusion of the uninhabited cells in the analysis. nal of Epidemiology 22,1193-1202. Crawford, MD., Gardner, MJ. & Morris, JN. 1968. Mor- tality and hardness of local water supplies. Lancet 1, 827- Conclusions and future work 831. Cudworth, AG., Wolf, E., Gorsuch, AN. & Festenstien, H. The inverse relationship between the AMI inci- 1979. A new look at HLA genetics with particular reference dence and total hardness of ground water was to type-1 diabetes. Lancet 2, 389-91. Haglund, B., Ryckenberg, K., Selinus, O. & Dahlquist, G. reconfirmed by this study. Other geochemical con- 1996. Evidence of a relationship between childhood-onset stituents of ground water were not statistically signifi- type I diabetes and low groundwater concentration of zinc. cantly associated with the AMI or type 1 diabetes Diabetes Care 19, 873-5. incidence. Well water (ground water) reflects geo- Huel, G., Thomazeau, R., Derriennic, F. & Lazar, P. 1978. Water hardness and cardiovascular mortality. A study of logical content of soil and bedrock and its content of 947 Alsatian communities. Revue d’Epidemiolgie et de major elements and trace elements (Lahermo et al. Sante Publique 26 (5), 381-90 1990) but only a small proportion of the population use ICRP 1974. Publication 23. Oxford: Pergamon Press, 327-328 locally produced food supplies, cereals and vegeta- Kannisto,V. 1947. The Causes of death as demographical factors in Finland (in Finnish, English summary). bles. Individual studies on the role of intake of both Kansantaloudellisia tutkimuksia - Economic studies XV, food and water-borne nutrients should incorporate Helsinki. environmental exposure or control for it. Lack of Karppanen, H., Pennanen, R. & Passinen, L. 1978. Min- georeferenced data of food and water-borne nutri- erals, Coronary Heart Disease and Sudden Coronary Death. Advances in Cardiology 25, 9-24. ents might, however, complicate such individual study. Karvonen, M., Tuomilehto, J., Libman, I. & LaPorte R. Chromium is an essential nutrient involved in the 1993. A review of the recent epidemiological data in the metabolism of glucose, insulin and blood lipids worldwide incidence of Type I (insulin-dependent) diabe- (Anderson 2000). Suboptimal dietary intake of chro- tes mellitus. World Health Organization DIAMOND Project Group. Diabetologia 36, 883-392. mium is associated with increased risk factors asso- Karvonen, M., Rusanen, J., Sundberg, M., Virtala, E., ciated with diabetes and cardiovascular diseases. Colpaert, A., Naukkarinen, A. & Tuomilehto, J. 1997. Koskinen (1994) has concluded that the lack of Regional differences in the incidence of insulin-dependent diabetes mellitus among children in Finland from 1987 to chromium alone might be relevant in the regional 1991. Annals of Medicine 29, 297-304 variation in incidence of ischaemic heart disease in Karvonen, M., Viik-Kajander, M., Moltchanova, E., Finland. The role of chromium in the AMI and type 1 Libman, I., LaPorte, R. & Tuomilehto J. 2000. Incidence diabetes incidence, will be the main focus in the future of childhood type 1 diabetes worldwide. World Health Organization Diabetes Mondiale data from 50 countries. studies of medical geology. In the next phase, data Diabetes Care 23, 1516-26. gathered for drinking water will be widened and water Karvonen, M., Moltchanova, E., Viik-Kajander, M., from public waterworks will be utilised. Moltchanov, V., Rytkönen, M., Kousa, A. & Tuomilehto, J. 2002. Regional inequality in the risk of Acute Myocardial Infarction in Finland: A case study of 35- to 74-year-old Acknowledgements men. Heart Drug 2, 51-60. Koljonen, T. (ed.) 1992. Bedrock and associated geophysical This work was partly funded by the Academy of and other features. The Geochemical Atlas of Finland, Part Finland; project No. 41266 and the Finnish Foundation 2: Till. Espoo: Geological Survey of Finland. 218 p., 11 app. maps. for Cardiovascular Research. Koljonen, T. & Tanskanen, H. 1992. Quaternary sediments.

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In: Koljonen T. (ed.) The Geochemical Atlas of Finland, Publication 113. 7-22. Part 2: Till. Espoo: Geological Survey of Finland. 218 p., 11 Punsar, S., Erämetsä, O., Karvonen, MJ., Ryhänen, A., app. maps. Hilska, P. & Vornamo, H. 1975. Coronary heart disease Korsman, K., Koistinen, T., Kohonen, J., Wennerström, and drinking water. Journal of Chronic Diseases 28,259- M., Ekdahl, E., Honkamo, M., Idman, H. & Pekkala, Y. 287. (eds.) 1997. Bedrock map of Finland 1:1 000 000. Espoo: Punsar, S. & Karvonen, MJ. 1979. Drinking water quality Geological Survey of Finland. and sudden death: observations from West and East Finland. Koskinen, S. 1994. Origins of regional differences in mortal- Cardiology. 64 (1),24-34. ity from ischaemic heart disease in Finland. NAWH, Re- Ranta, J. & Penttinen, A. 2000. Probabilistic small area risk search reports 41, 204 p. assessment using GIS-based data: a case study on Finnish Kousa, A. & Nikkarinen, M. 1997. Geochemical environ- childhood diabetes. Statistics in Medicine 19,2345-2359. ment in areas of low and high coronary heart disease Reunanen, A., Knekt, P., Marniemi, J., Maki, J., Maatela, mortality. In: Autio S. (ed.) Geological Survey of Finland, J. & Aromaa, A. 1996. Serum calcium, magnesium, copper Current Research 1995-1996. Geological Survey of Finland, and zinc and risk of cardiovascular death. European Journal Special Paper 23, 137-148. of Clinical Nutrition Jul;50(7), 431-7. Kousa, A., Moltchanova, E., Viik-Kajander, M., Rytkönen, Rubenowitz, E., Molin, I., Axelsson, G. & Rylander, R. M., Tuomilehto J., Tarvainen, T. & Karvonen, M. 2000. Magnesium in drinking water in relation to morbidity Geochemistry of the ground water and the incidence of and mortality from acute myocardfial infarction. Epidemi- AcuteAcute Myocardial Myocardial Infarction Infarction (AMI) (AMI) in in Finland Finland (manu- (sub- ology 11 (4), 416-421. script).mitted). Rusanen, J., Räisänen, S., Naukkarinen, A. & Colpaert, Kuulasmaa, K., Tunstall-Pedoe, H., Dobson, A., Fortman, A. 1995. Definition of rural areas based on primary produc- S., Sans, S., Tolonen, H., Evans, A., Ferrario, M. & tion by means of GIS. Terra 107,101-111. Tuomilehto, J. 2000. Estimation of contribution of changes Rylander, R., Bonevik, H. & Rubenowitz, E. 1991. Magne- in classic risk factors to trends in coronary-event rates sium and calcium in drinking water and cardiovascular across the WHO MONICA project population. Lancet 355, mortality. Scandinavian Journal of Work, Environment and 675-687 Health, Apr; 17 (2), 91-4. Lahermo, P., Ilmasti, M., Juntunen,. R, & Taka, M. 1990. Rytkönen, M., Ranta, J., Tuomilehto, J. & Karvonen, M. The hydrogeochemical mapping of Finnish groundwater. The SPAT Study Group. 2001. The Finnish Childhood The Geochemical Atlas of Finland, Part 1. Espoo: Geologi- Diabetes Registry Group. Bayesian analysis of geographical Survey of Finland. 66 p. cal variation in the incidence of Type I diabetes in Finland. Luoma, H., Aromaa, A., Helminen, S., Murtomaa, M., Diabetologia 44, 37-44. Kiviluoto, L., Punsar, S. & Knekt, P. 1983. Risk of Salonen, JT., Salonen, R., Seppänen, K., Kantola, M., myocardial infarction in Finnish men in relation to fluoride, Sntioinen, S. & Korpela, H. 1991. Interactions of serum magnesium and calcium concentration in drinking water. copper, selenium, and low density lipoprotein cholesterol Acta Medica Scandinavica 213,171-176. in atherogenesis. British Medical Journal, Mar 30; 302 Maheswaran, R., Morris, S., Falconer, S., Grossinho, A., (6779), 756-60. Perry, I., Wakefield, J. & Elliot, P. 1999. Magnesium in Salonen, JT., Nyyssönen, K., Korpela, H., Tuomilehto, J., drinking water supplies and mortality from acute myocar- Seppänen, R. & Salonen, R. 1992. High stored iron levels dial infarction in northwest England. Heart 82,455-460. are associated with excess risk of myocardial infarction in McMaster, D., McCrum, E., Patterson, CC., Kerr, MM., eastern Finnish men. Circulation Sep; 86 (3), 803-11. O’Reilly, D., Evans, AE. & Love, AH. 1992. Serum copper Spiegelhalter, DJ., Thomas, A., Best, NG. & Gilks, WR. and zinc in random samples of the population of Northern 1996. BUGS: Bayesian Inference Using Gibbs Sampling. Ireland. American Journal of Clinical Nutrition 56 (2), Version 0.5. (version ii). 440-6. Smith, WC. & Crombie, IK. 1987. Coronary heart disease Moltchanova, E., Rytkönen, M., Kousa, A., Taskinen, O., and water hardness in Scotland—is there a relationship? Tuomilehto, J. & Karvonen, M. Zinc and nitrate in the Journal of Epidemiology and Community Health Sep; 41(3), ground water and the incidence of Type 1 Diabetes in 227-8 Finland for the SPAT Study Group and the Finnish Child- Tarvainen, T., Lahermo, P., Hatakka, T., Huikuri, P., hood Diabetes Registry Group. (manuscript) Ilmasti, M., Juntunen, R., Karhu, J., Kortelainen, N., Nerbrand, CH., Svärdsudd, K., Ekland, J. & Tibblin, G. Nikkarinen, M., & Väisänen, U. 2001. Chemical compo- 1992. Cardiovascular mortality and morbidity in seven sition of well water in Finland – main results of the “One counties in Sweden in relation to water hardness and geologi- thousand wells” project. In: Autio S. (ed.) Geological Sur- cal settings. European Heart Journal 3, 21-727. vey of Finland, Current Research 1999-2000. Geological Onkamo, P., Väänänen, S., Karvonen, M. & Tuomilehto, Survey of Finland, Special Paper 31, 57-76. J. 2000. Worldwide increase in incidence of Type I diabetes Tuomilehto-Wolf, E. & Tuomilehto, J. 1991. HLA antigens — the analysis of the data on published incidence trends. in insulin-depndent diabetes mellitus. Annals of Medicine Diabetologia 42,1395-1403. 23,481-488. Osnes, K. & Aalen, OO. 1999. Spatial smoothing of cancer Tuomilehto, J., Arstila, M., Kaarsalo, E., Kankaanpaa, J., survival: a Bayesian approach. Statistics in Medicine 18, Ketonen, M., Kuulasmaa, K., Lehto, S., Miettinen, H., 2087-2099. Mustaniemi, H. & Palomaki, P et al. 1992. Acute myo- Piispanen, R. 1993. Water hardness and cardiovascular mor- cardial infarction (AMI) in Finland—baseline data from the tality in Finland. Environmental Geochemistry and Health FINMONICA AMI register in 1983-1985. European Heart 15 (4), 201-8. Journal, Aug; 13 (8), 1153 Plant, JA., Baldock, W. & Smith, B. 1996. The role of Tuomilehto, J., Karvonen, M., Pitkäniemi, J., Virtala, E., geochemistry in environmental and epidemiological studies Kohtamaki, K., Toivanen, L. & Tuomilehto-Wolf, E. in developing countries. In Appleton JD et al. (ed) Environ- 1999. Record-high incidence of Type I (insulin-dependent) mental Geochemistry and Health with special reference to diabetes mellitus in Finnish children. 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Jun; 42 (6), 655-60. risk of childhood diabetes in the Netherlands. Diabetes Care Tuvemo, T. & Gebre-Medhin, M. 1983-85. The role of trace 22,1750. elements in juvenile diabetes mellitus. Pediatrician 12, Verge CF, Howard NJ, Irwig L, Simpson JM, Mackerras 213-9. D, & Silink M. 1994. Environmental factors in childhood Uemura, K. & Pisa, Z. 1988. Trends in cardiovascular disease IDDM. A population-based, case-control study. Diabetes mortality in industrialized countries since 1950. World Care 17,1381-9. Health Statistics Quaterly 41,155-178. Virtanen, S.M., Jaakkola, L., Rasanen, L., Ylönen, K., Underwood, EJ. 1971. Trace elements in human and animal Aro, A., Lounamaa, R., Akerblom, H.K., & Tuomilehto, nutrition. New York: Academic Press. J. 1994. Nitrate and nitrite intake and the risk for type 1 Van Maanen, J.M., Albering, H.J., Van Breda, S.G., Curfs, diabetes in Finnish children. Childhood Diabetes in Finland D.M., Ambergen, A.W., Wolffenbuttel, B.H., Kleinjans, Study Group. Diabetic Medicine 11,656-662. J.C. & Reeser, H.M. 1999. Nitrate in drinking water and

59 60 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 61– 65 , 2003.

HEAVY METAL ENRICHMENT FACTORS FOR DIFFERENT ANALYTICAL METHODS

by Timo Tarvainen and Philipp Schmidt-Thomé

Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): geochemical surveys, heavy metals, enrichment, chemical analysis, Fennoscandia, Baltic region, Germany, Poland, Belarus

Introduction 1 sample/2500 km2 on agricultural soils. Two samples were collected from each site: topsoil 0 - 25 cm and Heavy metal enrichment factors have been pro- subsoil 50 - 75 cm. The samples were 8 L in volume posed to form part of a set of indicators for diffuse soil and a composite of 5 - 13 subsamples was collected contamination. The enrichment factors are calcu- from an area measuring 100 m x 100 m. The samples lated by dividing the heavy metal concentration in for Poland and Sweden were splits of samples taken topsoil by the subsoil concentration. Various analyti- originally for different projects. The <2 mm fraction of cal techniques are used to measure heavy metal each sample (Polish samples: <1 mm) has been concentration from soils in different geochemical analysed using four methods: mapping programmes. The enrichment factor can be 1. X-Ray Fluorescence (XRF) showing total con- dependent on the analytical method applied. centrations of the main elements and some trace The Baltic Soil Survey (BSS, Reimann et al. 2000) elements such as lead; has been used to test to what degree the enrichment 2. Total leach using strong concentrated mineral factor depends on the analytical method employed. acids (TOT) with ICP AES/ICP MS measurement, The Baltic Soil Survey covers ten of the Baltic Sea which gives almost total concentration of many trace countries (Belarus, Estonia, Finland, Northern Ger- elements which are missing from the XRF data; many, Latvia, Lithuania, Norway, Poland, NW Rus- 3. Aqua Regia extraction (AR) with ICP AES sia and Sweden) with a sampling density of 1 sample/ measurement or graphite furnace atomic absorption 2500 km2. Topsoil and subsoil samples are analysed spectrometry revealing the semi-total concentration using four methods, and enrichment factors for Cd, of 27 elements; and Cu, Pb and Zn were calculated for different analytical 4. Ammonium acetate extraction indicating out the methods. This paper analyses different analytical “bioavailable” concentration of selected elements. methods and the comparability of their results. Enrichment factors for Cd, Cu, Pb and Zn were Materials and methods calculated as follows:

The sampling density of the Baltic Soil Survey was

61 Geological Survey of Finland, Special Paper 36 Timo Tarvainen and Philipp Schmidt-Thomé

Factor M = ctMt / ctMs The enrichment factors for Cd, Cu, Pb and Zn that are based on various analytical methods (Ammonium where acetate extraction, Aqua Regia extraction, Total leach and X-Ray Fluorescence analysis) are pre- Factor M = enrichment factor for heavy metal M; sented in Table 1. Samples with topsoil LOI% > 15% ctMt = concentration of heavy metal M in are omitted. topsoil; Reimann et al. (2000) reported that most elements ctMs = concentration of heavy metal M in either have almost the same concentration in top- and subsoil. subsoil samples or are slightly depleted in the top- The organic carbon content was measured as layer. At least five different processes can cause a LOI%. depletion of elements in the top-layer:

Results and discussion 1. Plant uptake and removal of elements via har- vesting, insufficient replenishment via fertilizers, sew- The topsoil heavy metal concentration can reflect age sludge and / or liming; either natural, geogenic background or anthropogenic 2. Leaching of elements from top to bottom during enrichment in topsoils. Figure 1a shows the distribu- the development of soil profiles; tion of lead (Pb) in topsoils. Anomalies in southern 3. Higher weathering rates of minerals in the top- Finland and central Sweden, e.g., are similar in subsoil layer; samples and most of them are possibly of geological 4. Selective wind erosion of the fine fraction of soil; origin. On the other hand, high Pb concentration in and German topsoils are not related to Pb anomalies in 5. Lessivation, the removal of clay particles and subsoils. Elevated Pb concentration in Germany ap- generally the fine soil fraction from topsoil to deeper parently result of heavier traffic and industrial activi- layers. ties. a) b)

Fig.1. a). Distribution of total Pb in topsoil in the Baltic Soil Survey area. b) Enrichment factor of Pb (=Pb topsoil/Pb subsoil). In northernmost Lapland Pb concentrations are often below the analytical detection limit and the enrichment factor is elevated even when the topsoil concentrations are small.

62 Geological Survey of Finland, Special Paper 36 Heavy metal enrichment factors for different analytical methods

Table 1. Heavy metal enrichment factors for Cd, Cu, Pb and Zn. Countries: BLR = Belarus, EST = Estonia, FIN = Finland, GER = Germany, LAV = Latvia, LIT = Lithuania, NOR = Norway, POL =Poland, RUS = Russia, SWE = Sweden. Analytical methods: (AA) = Ammonium acetate extraction, (AR) = Aqua Regia extraction, (TOT) = Total leach, (XRF) = X-Ray Fluorescence analysis.

Country Count Median Minimum Maximum

BLR Cd factor (AR) 31 3.09 0.96 30.60 Cd Factor (AA) 31 2.00 0.534.67 Zn factor (TOT) 31 1.09 0.61 2.61 Zn factor (AR) 31 1.41 0.49 5.50 Zn factor (AA) 31 2.730.8359.06 Cu factor (TOT) 31 .93 0.42 2.67 Cu factor (AR) 31 .82 0.21 5.90 Cu factor (AA) 31 1.38 0.40 9.66 Pb factor (XRF) 31 1.230.40 2.14 Pb factor (TOT) 31 1.21 0.70 2.72 Pb factor (AR) 31 1.79 0.71 4.13 Pb factor (AA) 31 1.92 0.55 6.94 EST Cd factor (AR) 1 6 2.25 1.235.99 Cd Factor (AA) 1 6 2.00 0.81 2.00 Zn factor (TOT) 1 6 1.430.96 1.77 Zn factor (AR) 1 6 1.51 1.00 2.64 Zn factor (AA) 1 6 1.40 0.96 14.22 Cu factor (TOT) 1 6 1.22 0.75 4.10 Cu factor (AR) 1 6 1.11 0.11 14.60 Cu factor (AA) 1 6 2.88 1.00 12.01 Pb factor (XRF) 1 6 1.11 0.67 2.17 Pb factor (TOT) 1 6 1.18 0.90 1.45 Pb factor (AR) 1 6 1.50 0.71 2.36 Pb factor (AA) 1 6 1.36 0.38 6.23 FIN Cd factor (AR) 6 6 2.49 .41 15.17 Cd Factor (AA) 6 6 2.00 0.835.61 Zn factor (TOT) 6 6 1.06 0.532.71 Zn factor (AR) 6 6 1.21 0.17 5.02 Zn factor (AA) 6 6 2.030.57 23.87 Cu factor (TOT) 6 6 .77 0.39 4.68 Cu factor (AR) 6 6 .80 0.24 8.54 Cu factor (AA) 6 6 1.19 0.21 19.43 Pb factor (XRF) 6 6 1.130.22 4.00 Pb factor (TOT) 6 6 1.15 0.831.75 Pb factor (AR) 6 6 1.81 0.737.29 Pb factor (AA) 6 6 2.00 0.26 6.79 GER Cd factor (AR) 37 3.34 0.67 82.00 Cd Factor (AA) 37 2.00 0.736.58 Zn factor (TOT) 37 1.05 .24 3.56 Zn factor (AR) 37 1.62 0.6312.27 Zn factor (AA) 37 5.87 1.34 59.19 Cu factor (TOT) 37 .84 0.434.78 Cu factor (AR) 37 2.04 0.34 20.40 Cu factor (AA) 37 1.930.57 20.36 Pb factor (XRF) 37 2.00 0.6317.50 Pb factor (TOT) 37 1.70 0.94 4.57 Pb factor (AR) 37 2.78 0.87 17.97 Pb factor (AA) 37 2.07 0.33 15.44 LAV Cd factor (AR) 2 5 1.71 0.71 4.85 Cd Factor (AA) 2 5 2.00 0.57 2.00 Zn factor (TOT) 2 5 1.02 0.45 3.02 Zn factor (AR) 2 5 1.230.47 4.74 Zn factor (AA) 2 5 1.57 0.56 8.84 Cu factor (TOT) 2 5 .73 0.28 1.96 Cu factor (AR) 2 5 .58 0.15 3.25 Cu factor (AA) 2 5 .85 0.14 5.52 Pb factor (XRF) 2 5 1.430.43 6.00 Pb factor (TOT) 2 5 1.20 0.58 1.89 Pb factor (AR) 2 5 1.42 0.57 4.98 Pb factor (AA) 2 5 1.33 0.29 6.47 LIT Cd factor (AR) 2 6 2.18 1.16 7.03 Cd Factor (AA) 2 6 2.00 0.634.34 Zn factor (TOT) 2 6 1.08 0.60 3.33 Zn factor (AR) 2 6 1.20 0.60 3.48 Zn factor (AA) 2 6 1.48 0.67 7.88 Cu factor (TOT) 2 6 .80 0.33 2.01 Cu factor (AR) 2 6 .83 0.05 7.68 Cu factor (AA) 2 6 .82 0.234.74 Pb factor (XRF) 2 6 1.40 0.71 7.50 Pb factor (TOT) 2 6 1.40 0.90 2.03 Pb factor (AR) 2 6 1.76 0.86 4.84 Pb factor (AA) 2 6 1.45 0.236.55

63 Geological Survey of Finland, Special Paper 36 Timo Tarvainen and Philipp Schmidt-Thomé

Table 1. (cont.)

Country Count Median Minimum Maximum

NOR Cd factor (AR) 107 1.62 0.36 12.62 Cd Factor (AA) 107 2.00 0.21 3.91 Zn factor (TOT) 107 1.11 0.24 2.55 Zn factor (AR) 107 1.22 0.18 4.20 Zn factor (AA) 107 1.45 0.50 11.59 Cu factor (TOT) 107 1.07 0.24 5.28 Cu factor (AR) 107 1.09 0.07 11.10 Cu factor (AA) 107 1.40 0.21 12.05 Pb factor (XRF) 107 1.20 0.20 10.00 Pb factor (TOT) 107 1.130.14 1.77 Pb factor (AR) 107 1.54 0.76 4.72 Pb factor (AA) 107 2.00 0.17 12.00 POL Cd factor (AR) 129 2.60 0.42 39.20 Cd Factor (AA) 129 2.00 0.10 21.28 Zn factor (TOT) 129 1.25 0.58 6.18 Zn factor (AR) 129 1.48 0.37 6.48 Zn factor (AA) 129 3.92 0.37 23.80 Cu factor (TOT) 129 1.15 0.28 8.83 Cu factor (AR) 129 1.05 0.08 15.86 Cu factor (AA) 129 1.82 0.2317.50 Pb factor (XRF) 129 1.40 0.42 8.50 Pb factor (TOT) 129 1.36 0.57 4.43 Pb factor (AR) 129 1.58 0.49 9.00 Pb factor (AA) 129 2.02 0.25 17.52 RUS Cd factor (AR) 7 6 2.25 0.58 33.08 Cd Factor (AA) 7 6 2.00 2.00 5.34 Zn factor (TOT) 7 6 1.21 0.47 4.73 Zn factor (AR) 7 6 1.47 0.41 13.23 Zn factor (AA) 7 6 5.61 0.77 71.17 Cu factor (TOT) 7 6 .66 0.26 3.69 Cu factor (AR) 7 6 .61 0.08 9.36 Cu factor (AA) 7 6 .80 0.19 8.34 Pb factor (XRF) 7 6 1.17 0.57 6.00 Pb factor (TOT) 7 6 1.16 0.57 3.35 Pb factor (AR) 7 6 1.72 0.30 14.12 Pb factor (AA) 7 6 1.97 0.28 11.52 SWE Cd factor (AR) 133 2.230.70 24.48 Cd Factor (AA) 133 2.00 0.47 6.95 Zn factor (TOT) 133 1.10 0.07 2.68 Zn factor (AR) 133 1.21 0.34 4.84 Zn factor (AA) 133 4.86 0.0328.41 Cu factor (TOT) 133 .95 0.11 2.81 Cu factor (AR) 133 .98 0.04 18.24 Cu factor (AA) 133 1.31 0.29 23.78 Pb factor (XRF) 133 1.09 0.46 3.60 Pb factor (TOT) 133 1.10 0.632.71 Pb factor (AR) 133 1.19 0.27 5.39 Pb factor (AA) 133 1.55 0.31 10.48

Table 2. Pearson’s correlation coefficients between enrichment factors. ** = Correlation is significant at the 0.01 level (2-tailed). * = Correlation is significant at the 0.05 level (2-tailed).

Element XRF-TOT XRF-AR XRF-AA TOT-AR TOT-AA AR-AA

Cd .089* Cu .313** .294** .226** Pb .414** .473** .275** .565** .348** .541** Zn .738** .387** .492**

Enrichment of elements in the topsoil can be due to pheric deposition. Correlation coefficients between element input via fertilizers, liming, fungicides, pesti- enrichment factors based on different analytical meth- cides as well as sewage sludge application or atmos- ods are summarized in Table 2. Samples with topsoil pheric deposition. Some elements are strongly bound LOI% > 15% are omitted. Correlations are significant in the topsoil when the organic content is high. Also for all the enrichment factors, except for Cd. Enrich- bioaccumulation in living organisms can enhance en- ment factor values tend to be higher for ammonium richment in topsoils. For example, Cd enrichment is acetate extractions compared to those based on often caused by application of Cd-bearing fertilizers stronger extractions. Anthropogenic enrichment is whereas Pb enrichment is usually related to atmos- more clearly seen in bioavailable concentrations with

64 Geological Survey of Finland, Special Paper 36 Heavy metal enrichment factors for different analytical methods the only exception of Cd, due to very low natural samples, thus all samples with LOI% > 15% were concentrations. The total (XRF, TOT) and semi-total eliminated. Very low heavy metal concentration may (Aqua Regia) analytical methods lead to enrichment lead to artificially high enrichment factors, even when factors that are at the same level and correlated to the topsoil concentrations are near the analytical each other. detection limit.

Conclusions REFERENCES

Comparable heavy metal enrichment factors can be Reimann, C., Siewers, U., Tarvainen, T., Bityukova, L., based either on total/semi-total concentration of heavy Eriksson, J., Gilucis, A., Gregorauskiene, V., Lukashev, metals in subsoil and topsoil samples or on bioavailable V., Matinian, N.N. & Pasieczna, A. 2000. Baltic Soil Survey: Total concentrations of major and selected trace concentrations such as ammonium acetate extrac- elements in arable soils from ten countries around the Baltic tions. Samples with very high organic carbon content Sea. The Science of the Total Environment 257 (2-3), 155- in topsoil are not comparable with typical mineral soil 170.

65 66 Geological Survey of Finland, Current Research 2001–2002, Edited by Sini Autio. Geological Survey of Finland, Special Paper 36, 67– 75 , 2003.

SURVEY OF A BURIED ICE-MARGINAL DEPOSIT BY AIRBORNE EM MEASUREMENTS – A CASE FROM KYRÖNJOKI VALLEY PLAIN IN SOUTHERN OSTROBOTHNIA, FINLAND

by P. Lintinen, I. Suppala, H. Vanhala and M. Eklund

Geological Survey of Finland, P.O. Box 96, FIN-02151 ESPOO, FINLAND E-mail: [email protected]

Key words (GeoRef Thesaurus, AGI): ice-marginal features, glaciofluvial features, buried features, geophysical methods, electromagnetic methods, airborne methods, field studies, resistivity, Kyrönjoki, Finland

Introduction measurements arises from the fact that the glaciofluvial and fine-grained sediments have a distinct resistivity In Finland glaciofluvial eskers and ice-marginal contrast – the resistivity of clays and silts is distinc- deposits are important sources of raw material for the tively lower than the resistivity of the sand and gravel aggregate industry. Also glaciofluvial aquifers are of eskers and ice-marginal deposits. vital for municipal water supply. Although glacifluvial Huotari (2002) has made a model calculation of the deposits are relatively uniformly distributed in Finland, feasibility of the GTK’s AEM system to mapping there are several populated regions lacking exploitable buried valleys. This test area was situated in northeast glaciofluvial deposits. In some of these areas glacio- Estonia. No buried valleys were found there, but the fluvial deposits are covered by thick clay or silt calculations strongly suggest that the AEM system is deposits. Accidental penetrations of those aquifers sensitive for detecting buried valley type deposits, i.e., have sometimes caused unpredicted artesian wells. resistive bodies situated in more conductive ground. In favourable locations buried glaciofluvial deposits There are, however, many open questions related to have been mapped by ground geophysical methods the usefulness and restrictions of AEM in detecting verified by drilling results. In many cases the high buried resitive deposits in conductive environment. costs have limited the conducted survey activities and For example, how thick clay layer masks the anomaly therefore the lateral extent of continuous or discon- caused by the buried deposit. The question as to what tinuous chain of glaciofluvial deposits has not been kind of information we can obtain from the buried properly mapped. In view of the unquestionable im- target by AEM measurements, is also of great impor- portance of the mapping of buried glaciogluvial depos- tance. Is it only the approximately location, or can we its, an effective mapping tool is needed. also interpret the depth, shape and the true electrical In this study we have tested the airborne electro- resistivity of the deposit. The last would give us a way magnetic (AEM) measurements in order to survey to classify the anomalies, for example to discriminate clay and silt covered glaciofluvial deposits in a test bedrock anomalies from anomalies caused by sedi- area where ice-marginal deposits have already been ment material. In order to get answers to these known to exist but their lateral extent has not been questions and to develop interpretation of AEM data, mapped. The idea of mapping buried deposits by AEM we started the present study. In addition to AEM data,

67 Geological Survey of Finland, Special Paper 36 P. Lintinen, I. Suppala, H. Vanhala and M. Eklund

ground EM measurements and reference drillings and mica schists (Mäkitie & Lahti 1991, Mäkitie et al. sampling were done. Special emphasis has been put 1991). Till covering the bedrock outcrops is described on AEM and EM inversion techniques and modelling. by Kukkonen et al. (1983) as basal till and it is coarse grained, containing less than 5 % clay (∞ <0.002 m) Geology of the study area fraction. A few glaciofluvial deposits are also found in the area. A small but prominent esker, running from The study area is situated in the Kyrönjoki valley northwest to southeast, is situated northwest of the about 10 km west of the city of Seinäjoki, partly Kyrönjoki river (Fig.3). A smaller glaciofluvial deposit situated in the municipalities of Seinäjoki and Ilmajoki outcrops through fine-grained sediments close to the (Fig.1).The landscape is typical in southern Ostro- Kyrönjoki and Seinäjoki rivers (Fig. 3), called tenta- bothnian with low-lying river valleys filled with lacustrine tively Vuolle by Kurkinen et al. (1992). Also a sand and glacilacustrine sediments. Bedrock outcrops, partly deposit, about 0.15 x 1.1 km in size (called tentatively covered by till, delineate river valleys. The study area Aavala by Kurkinen et al. 1992) outcrops through is cultivated and it is situated at an altitude of 40 m a.s.l. fine-grained sediments in the central part of the river The altitude of the adjacent gently undulating hills is valley. This deposit is elongated from southwest to often at an altitude of 60-90 m a.s.l. The surface relief northeast, i.e., perpendicular to the regional ice flow of silt and clay deposits is relatively flat. The minor direction as recorded by esker and striae directions topographical differences have mainly been caused (Kukkonen 1990b). Based on the evidence of drilling by recent human activities related to ditching and data and seismic soundings, Kurkinen et al. (1992) prevention of spring flooding of the Kyrönjoki and have shown that the Aavala deposit is far more Seinäjoki rivers. extensive than was previously known. They postu- Bedrock in the study area is mostly composed of lated that the clay and silt covered glaciofluvial deposit

Fig. 1. Location map of the airborne survey area in the Kyröjoki valley in southern Ostrobothnia, Finland. The 8x12 km2 study area is situating in the municipalities of Seinäjoki and Ilmajoki. Note the northwest to southeast trend of eskers marked in green in the map. Modified after Kujansuu & Nimelä (1984).

68 Geological Survey of Finland, Special Paper 36 Survey of a buried ice-marginal deposit by airborne EM measurements – A case ... could be part of an extensive ice-marginal deposit Airborne and ground EM data deposited at the ice margin, which could be delineated by isolated deposits all interpreted to be deltas in In order to test the applicability of GTK’s dual- origin. Kurkinen et al. (1992) suggest that the hypo- frequency AEM-system in mapping buried ice-mar- thetical ice-margin could have been situated between ginal deposit, a survey flight was conducted in a study Pohjankangas and Hietakangas, south of Lappajärvi, area using a Twin Otter aircraft. Measurements were being about 80 km in length. carried out in an area of 8x12 km2 (Fig. 2) during one Previous drilling results show that the clay and silt day. The nominal line spacing was 100 m and the sediments are typically about 20 m in thickness nominal flight altitude 30 m. The median flight altitude (Kukkonen 1990a,b) and they were deposited during was 32.5 m. Because of power lines, the flight altitude the earlier, more extensive stages of the Baltic Sea. varied between 20 and 60 m. The airborne EM system According to Kukkonen et al. (1983), the lower part of uses dual frequency vertical coplanar coils. The two the fine-grained sediment cover was deposited during frequencies are 3.1 kHz and 14.4 kHz. The coil pairs the Ancylus Lake period and the upper part of was for the systems are mounted on the wingtips so that deposited during the Litorina Sea period. The highest the coil spacing is 21.36 meters. The measured quan- sec pri shoreline of Litorina Sea is at an altitude of 60 m a.s.l. tity is the ratio Hh /Hh , expressed in unit part per sec pri The uppermost sediment unit, usually less than 1 m in million (ppm), so that Hh and Hh are the horizontal thickness, is found only at close distance from the components of the secondary and primary magnetic Kyrönjoki river, where annual spring flooding has field. Measurements have in-phase and quadrature maintained wetland areas. Now these presently culti- components (in-phase and 90° out-of-phase with re- vated areas are peat or organic rich silt sediments. spect to the primary magnetic field). A detailed de-

Fig. 2. Colour-shaded airborne apparent resistivity map (LFA map) of the study area. Line spacing is 100 m, nominal flight altitude 30 m, and frequency 3.1 kHz (see Fig. 1). The high-resistivity anomaly marked by white dotted lines is related to the subject of this study, the partially buried ice-marginal deposit. The survey flight was made September 9, 2002.

69 Geological Survey of Finland, Special Paper 36 P. Lintinen, I. Suppala, H. Vanhala and M. Eklund

Fig 3. Map of apparent resistivity (HFA map), middle part of the study area. Line spacing is 100 m, nominal flight altitude 30 m, and frequency 14.4 kHz (see Figs. 1 and 2). D-1 and D-2 are drilling sites, L-1 - L-4 ground EM lines (horizontal loop slingram), and L-31 and L-32 the flight lines discussed in Fig. 6. The areas marked by dotted lines are exposed gravel to fine sand sized sorted sediments delineated by Kukkonen (1990a,b).

scription of the measuring system is given by Poikonen 1 m intervals or in intervals related to the changes of et al. (1998). penetration rate indicating consistency differences of Ground EM measurements were carried out using the sediment. Flow-through-bit samples were studied the multi frequency horizontal loop slingram method, in the field and they reveal only scattered information with the APEX MaxMin I+8S system. Six frequen- on major sediment units. cies (880, 1760, 3520, 7040, 14080 and 28160 Hz) were used. The nominal coil separation of 40 m was Lithostratigraphy used in all ground EM survey profiles (Fig. 3). The results are expressed as normalized in-phase and Drilling localities are marked in Figure 3. Drilling at quadrature components in percentage (%) of the locality D-1 terminated at a depth of 20.1 m. Neither primary field. bedrock nor till was detected. The whole drilled sequence is comprised of soft clay or silt sediments, Drilling and sampling which are divided into three sedimentary units. The lowermost unit from a depth of 20.1 m to 17 m is The drillings we conducted by GM 100 drilling rig composed of laminated silt and clay. In each rhythmite applying a piston sampler with a sampling tube 2 m in coarser layers are from 2 to 10 cm in thickness and length and with a 45 mm inner diameter. The drilling finer layers are from 0.3 to1.0 cm in thickness. locations are shown in Figure 3. Standard procedures Dropstone structures with pebble size clasts were were applied for logging of drilled samples. Continu- observed in this unit. The lamina thickness gradually ous piston core samples of soft sediments, i.e., clay, decreases and dark sulphide rich laminated clay and silt or fine sand were opened in the laboratory. silt with 1-3 mm lamina thickness overlies the lowermost Sediments difficult to penetrate with the piston corer unit. At a depth of 12-11 m the laminated sediment unit were sampled by flow-through-bit and only studied in gradually changes to upper weakly laminated or

70 Geological Survey of Finland, Special Paper 36 Survey of a buried ice-marginal deposit by airborne EM measurements – A case ... massive sulphide clay and silt unit. 1978, Peltoniemi 1982) is the simplest 1D interpreta- Drilling at locality D-2 terminated at a depth of 25 tion method. Especially in areas of low-resitivity, m, when bedrock or a large boulder was hit. The visual interpretation of the apparent resistivity and whole drilled sequence is divided into three units, apparent depth maps is the first step to evaluate the which are described starting from the base. The AEM data. The apparent resistivity and apparent lowermost unit from a depth of 25 to 17.8 m is depth, da, (da = Da - sensor height) per frequency can composed of till rich in stones, comparable to the be easily estimated by lookup tables or by simple common sandy till in the Seinäjoki district. The till model-based inversion. Today these estimates are overlies stratified sand and silt sediment with each delivered together with the measuring quantities. lamina 1-5 cm in thickness. At a depth of about 11 m In this study 1D layered-earth interpretation of EM the nature of the sediment gradually turns to sulphide data has been done with model norm-based inversion rich weakly laminated or massive silt and clay. (see Figs. 5-7). The earth is composed of many layers of uniform resitivity. The 1D resistivity structure, i.e., Laboratory resistivity measurements the resistivity of each layer, is sought by the regularized inversion. The goal is to find for every measuring Laboratory resistivity measurements of core sam- point a minimum-structure model, which can fit the ples were performed in order to record the electrical measurement data sufficiently well. The 1D responses resistivity of the reference sequence. The laboratory and sensitivity matrices has been calculated by the system consists of HP 35665A Signal Analyser and a Airbeo –program (Chen & Raiche 1998). The minimi- Wenner-type electrode array with 1 cm long steel electr- zation of objective function (data misfit + ß x model odes and 1 cm electrode spacing. Measurements were norm) has been carried out with the damped Gauss- conducted at an interval of 10 cm in drilled cores. The Newton algorithm of Haber (1997). laboratory resistivity values in drill core D-1 decrease The smoothness of the inversion results depends on from about 8 Nm at a depth of 2 metres to 4-5 Nm at the information content and errors of the measured a depth of 8 metres. Between 8-18 metres, the data. The proper calibration and adjustment of zero laboratory resistivity values were mostly between 4 levels of the EM measurements are essential for the and 5 Nm (Fig. 4). inversion. The movement of AEM system during measurement causes many types of noise, e.g. a small low-pass filtering effect to the responses, and also the measured altitudes contain some errors. Accordingly, we have slightly smoothed the measured altitude values. The regional zero levels are slightly adjusted by constant factors. The resolution of the dual-frequency system is lower than the ground EM system and so the inverted results are slightly smoother. In ground measurements, errors in positioning and alignment of the loops are likely to be the largest sources of error in the horizontal loop measurements. The reference cable connects the transmitter and receiver loops and with the help of the cable the coil separation is attempted to be kept at the constant value (in this study 40 m). The error in coil separation is most evidently seen in the in-phase component caused by the incompletely compensated primary magnetic field (e.g. Frischnecht et al. 1991). In this study, in the clay Fig. 4. Resistivity as a function of depth, drilling site D-1. The drill core was measured in the laboratory using a Wenner-type area, a change of 10 cm in coil spacing causes array with a 1.0 cm electrode spacing. maximally a change of 1.1 % in the in-phase component reading and 0.4 % in the quadrature component Interpretation of airborne and ground EM reading. That is why we have also considered the coil data separation as an unknown parameter and estimated it carefully from the field data. The estimation of the coil Transforming the AEM data to the apparent resis- separation could be done almost independently on the tivity of a half-space, and to the apparent distance (Da) resistivity model if the EM system operates also in low of that half-space from the sensor system (Fraser induction number domain, i.e., at low enough frequen-

71 Geological Survey of Finland, Special Paper 36 P. Lintinen, I. Suppala, H. Vanhala and M. Eklund

Fig 5. Resistivity sections from lines L-1 and L-2 (ground horizontal loop slingram data) obtained by smooth 1D inversion. The high- resistivity anomalies between 600-1200 m (Line-1) and around 1080 m (Line-2) arise from clay and silt covered, or partially covered, ice-marginal deposit. cies. In this low-resistive study area, the induction constant 40 m coil spacing. In this study the median for number (skin depth/coil separation) at the frequency estimated coil separation was 39.7 m. of 880 Hz (the lowest frequency) is about 1. The The assumption of the layered 1D earth means that estimated coil separation and estimated resistivity a large enough volume of the ground should have show some correlation. Nevertheless, at least in the laterally homogeneous resistivity structure. By “the case of effectively 1D resistivity structure the used illumination footprint” of the EM system we could model for the layered ground and for measuring describe the volume of the earth contributing to the system works better than the inversion assuming response (Liu & Becker 1990). We have studied that

Fig 6. A detail from line L-2 – Resistivity section (ground horizontal loop slingram data) obtained by smooth 1D inversion. D-1 and D-2 are the sampling sites.

72 Geological Survey of Finland, Special Paper 36 Survey of a buried ice-marginal deposit by airborne EM measurements – A case ...

Fig. 7. Resistivity sections from flight lines L-32 and L-31 (airborne EM data) obtained by smooth 1D inversion. The high-resistivity anomalies arise from the ice-marginal material partially covered clay and silt. subject briefly, calculating 3D sensitivity distributions tive sediments apparent resistivity values for 3125 Hz of these two coil systems (e.g. Spies & Habashy are higher than for 14368 Hz. The apparent distances 1995). 3D sensitivities visualize the region of the earth of the half-space model for 14368 Hz are generally contributing to the response of AEM system, in a greater than the flight altitudes, which indicate that the sense like a footprint of the system. For the AEM clay deposit seems to behave as a homogeneous half- system of Twin Otter, the most sensitive region is space at higher frequency. So, these apparent resistiv- below the coil system and elongated perpendicular to ity values should be near the true overall resistivity of the flight direction. Vertical coils, whose axes are sediments. oriented parallel to the flight line, mean good spatial Constraining with the minimum structure model, i.e., resolution along the flight line and adequate lateral minimal spatial derivatives with respect to conductiv- coverage perpendicular to the flight line. For the ity, has made the inverted resistivity sections too ground horizontal loop slingram system, the most smooth (in Figs. 5-7). It was expected that the resis- sensitive region is elongated along the profile. In this tivity would decrease smoothly from the surface to the case a very rough estimation of the length of the most deeper part of the deposit (e.g. Puranen et al. 1999a, sensitive region is 60-80 meters and the width is 40 m 1999b). That kind of resistivity variation fulfils the or less. For the AEM system the footprint is larger. used model norm assumption. If severe resistivity discontinuities appear, the inversion result will anyway Results be more or less smooth. If we could assume that thicker sections have uniform resistivity, we should In Figure 2 is shown the apparent resistivity map modify the used model norm assumptions, or simply do calculated from the 3125 Hz data and in Figure 3 the a 1D inversion with a couple of layers. In that case we apparent resistivity calculated from the 14368 Hz have to choose the optimum number of layers and data. The area covered by lacustrine or glacilacustrine estimate the layer resistivity and thickness (e.g. Chen sediments is clearly seen showing low resistivity & Raiche 1998). We have done also calculations using values. These very conductive sediments cover more this type of model-based inversion. At some measur- resistive overburden and bedrock. Over the conduc- ing points, using the Twin Otter AEM data, this method

73 Geological Survey of Finland, Special Paper 36 P. Lintinen, I. Suppala, H. Vanhala and M. Eklund

works and therefore gives a 1D resistivity structure here used EM systems also increases. Thus with this that (at that point) is reliable. Nevertheless, along the EM data we can only interpret variations in resistivity measuring profiles in these few-layer inversion re- and thickness of the overlying low resistive sediments. sults, several clearly erroneous results are likely to appear. The approach of smooth inversion seems to Discussion be a less laborious way to do the approximate resistivity imaging along the flight lines (Fig. 7). The draw- AEM survey results show an elongated, discontinu- back of the chosen model norm based method is that ous high-resistivity anomaly, which runs from SW to the results at some degree underestimate the thick- NE crossing the whole flight survey area 8 x 12 km2 ness of the sediments. Due to the electrical attenua- in size. The width of the anomaly varies from 100 m tion (and the geometrical attenuation) the capability of to more than 1000 m (Figs. 2 and 3). In the SW part the AEM system to resolve variation in resistivity of the flight area, the anomaly show distinct wedge decreases with increasing depth. In the case of sedi- shape. ment having a resistivity of 7 Nm, e.g. clay, the skin The AEM results verified by lithostratigraphy re- depths are 23.8 and 11.1 m for the low and high vealed by drilling sampling support the conclusions of frequency, correspondingly. Kurkinen et al. (1992) that the buried ice-marginal The result of horizontal loop slingram measure- deposit is far more extensive than the outcropping ments should give more accurate information from glaciofluvial deposits show in the study area. The horizontally layered resistivity structure. The slingram triangular deltaic shape of the resistivity anomaly profile L-2 is also measured with EM-31 and GEM- around the Aavala deposit and the transverse direc- 300 EM resistivity meters (Bäck 2002). These results tion related to the main esker and ice flow direction show that the resistivity in the uppermost part of the support the suggestion of Kurkinen et al. (1992) that sediments varies along that profile, indicating notable the clay and silt covered deposit is an ice-marginal resistivity variations also within the distance of the coil deposit in origin. Our evidence shows that the sug- separation. This contradictsis the 1D model assump- gested ice-marginal deposits laterally continues at tion and causes error to the inverted results. We have least 10 km and is composed of a narrow ridge calculated from the inverted slingram results the consisting of till and a wedge shaped deposit of sand apparent resistivity responses of EM-31 and GEM- and gravel closely connected to the esker further 300. The modelled and measured results have clear northwest. The suggested connection of the Aavala visual correlation in a larger scale. Figure 6 shows that and Vuolle deposits by Kurkinen et al. (1992) could not the estimated thickness of the low-resistive layered be verified in this study because the flight survey area deposit is too shallow. The fits are below the used did not extend to Vuolle. noise level except where the structure is effectively The survey flight was conducted with the nominal 3D. The inversions of AEM data from the nearest line spacing of 100 m. Normally, especially in regional flight lines give a slightly thicker formation. mapping flights, the line spacing has been 200 m. In many cases, the ground and airborne EM sys- Dense data help the visual interpretation. In the study tems “see” the buried ice-marginal deposits as 2D or area the apparent resistivity images give only qualita- 3D targets, and any kind of 1D interpretation does not tive estimates of the ground resistivity, but the spatial necessarily give reasonable results. Interpretation by pattern is more important. Estimation of the apparent 2D or 3D modelling or even inversion would be resistivity and depth for both frequencies is based on possible but nowadays still time-consuming. The 2D/ the model of the 1D homogeneous half-space. In this 3D interpretation will give information about the ge- case the buried deposit could be delineated well even ometry. Could we interpret the cause of the thickness with the low frequency in-phase component. Also the variation? Is it caused by a buried deposit or by a in-phase/quadrature response ratio could be used here variation in bedrock topography? We have briefly (Puranen et al.1999a, 1999b). modelled these cases using the program Arjuna_Air Nevertheless, we can obtain more quantitative (Chen & Raiche 1998). It calculates EM responses of results from this two-frequency AEM data. If the a coil system caused by a 2D structure. If the resistiv- calibration and levelling is done properly, we can ity of the covering sediments is less than 10 Nm and assume, for example, that calculated apparent resis- the thickness is several meters, the formation resistiv- tivity values are related to each other in a rigorous ity can be 3000 or 300 Nm without any significant way. These maps serve as a starting point to qualita- differences in measured responses. If the resistivity of tive interpretation. Here we presented results from a the covering sediments increases, the possibility to smooth, regularized 1D inversion. We expected that define the resistivity of the underlying body with the the resistivity values smoothly decrease from surface

74 Geological Survey of Finland, Special Paper 36 Survey of a buried ice-marginal deposit by airborne EM measurements – A case ... to deeper parts of the sedimentary bed, but the Conclusions inverted vertical resistivity sections can be even too smooth. The prior knowledge of the in-situ resistivity Our results demonstrate that AEM-measurements and resistivity structure (e.g. Fig. 4) has not been are applicable to mapping of glaciofluvial and ice- taken into account. We should constrain the inversion marginal deposits beneath a lacustrine or glacilacustrine results with that prior information too. sediment layer in the study area in Kyrönjoki river We were able to interpret variations in resistivity valley. Interpretations of AEM-results in the study and thickness of the low-resistivity sediments from the area are favoured by the relatively low resistivity of airborne data. The estimation of the resistivity struc- fine-grained Litorina sediments compared to underly- ture of the material that lays under the clay is a more ing till, glaciofluvial sand and gravel units with higher difficult task and it is essential to have ground-refer- resistivity values. Furthermore, AEM measurements ence data. Also the ground EM measurements help show great potential as a mapping tool for glaciofluvial the interpretation of AEM data. deposits or associated ice-marginal complexes covered by fine-grained lacustrine and glacilacustrine sediments in Ostrobothnia and in other similar localities.

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PAPERS PUBLISHED BY GEOLOGICAL SURVEY OF FINLAND STAFF IN 2001-2002

The following list includes references from the database Alexejev, Nikolay L.; Balagansky, Viktor V.; Belyatsky, FINGEO (situation at 28th February 2003) to papers Boris V.; Zinger, Tatiana F.; Kislitsyn, Roman V.; Huhma, publihedpublished in in 2001 2001 and and 2002 2002 (or(or inin 2000,2000, ifif notnot reportedreported in the Hannu 2001. Palaeoproterozoic PT regimes in the lower previous Current Research publication with at least one crust of the Belomorian Mobile Belt (BMB), Fennoscandian author from GTK staff (name in bold). Shield. In: EUG XI. European Union of Geosciences, April Aatos, Soile; Ahtonen, Niina; Breilin, Olli; Nikka- 8th - 12th, 2001, Strasbourg, France : abstract volume. rinen, Maria; Paalijärvi, Miikka; Björk, Erkki; Merikoski, Strasbourg: European Union of Geosciences, 356. Raisa; Vuento, Aimo; Turtiainen, Tuukka; Weltner, Anne; Alvi, Kimmo; Winterhalter, Boris 2001. Authigenic Linnainmaa, Markku; Alm, Sari; Junttila, Vesa 2001. mineralisation in the temporally anoxic Gotland Deep, the Luonnonkivituotannon ympäristötietojärjestelmän kehit- Baltic Sea. In: Paleoenvironment of the Baltic Sea. Baltica 14, täminen ja elinkaari : alustavia tuloksia luonnonkivi- 74-83. tuotannon elinkaaren aikaisista ympäristö- ja ympäristö- Alviola, R.; Mänttäri, I.; Mäkitie, H.; Vaasjoki, M. talousvaikutuksista. Abstract: Preliminary results about 2001. Svecofennian rare-element granitic pegmatites of the environmental impacts during the life cycle of the Finnish Ostrobothnia region, western Finland : their metamorphic natural stone production. In: Inkeröinen, J. (ed.) Eko- environment and time of intrusion. In: Mäkitie, H. (ed.) tehokkuus, yhteistyö ja yrittäminen : ympäristöklusterin Svecofennian granitic pegmatites (1.86-1.79 Ga) and quartz tutkimus-ohjelman ensimmäisen vaiheen (1997-1999) monzonite (1.87 Ga), and their metamorphic environment in tuloksia. Suomen ympäristö 474, 57-60. the Seinäjoki region, western Finland. Geological Survey of Abels, A.; Bergman, L.; Lehtinen, M.; Pesonen, L. J. Finland. Special Paper 30, 9-29. 2000. Structural constraints and interpretations on the Antikainen, Merja; Breilin, Olli; Lyytikäinen, Ari 2001. formation of the Söderfjärden and Lumparn impact struct- Pohjavesien suojelun ja kiviaineshuollon yhteensovittaminen ures, Finland. In: Plado, J. & Pesonen, L. J. (eds.) Meteorite : loppuraportti Ilomantsin seudulta. Abstract: The harmon- impacts in Precambrian shields, May 24-28, 2000, Lappa- ization of groundwater protection and aggregate service - final järvi-Karikkoselkä-Sääksjärvi, Finland : programme and report from the surroundings of Ilomantsi, Pohjois-Karjala. abstracts. Espoo : Helsinki: Geological Survey of Finland : Alueelliset ympäristöjulkaisut 221. 39 p. + 1 app. map. University of Helsinki, 26. Antikainen, Merja; Breilin, Olli; Lyytikäinen, Ari 2001. Ahonen, Lasse 2001. Permafrost : occurrence and physico- Pohjavesien suojelun ja kiviaineshuollon yhteensovittaminen chemical processes. Tiivistelmä: Ikirouta : esiintyminen ja : loppuraportti Pielisen-Karjalan seudulta. Abstract: The fysikaalis-kemialliset prosessit. Posiva-raportti 2001-05. harmonization of groundwater protection and aggregate 42 p. service - final report from the surroundings of Pielisen- Ahonen, Lasse; Luukkonen, Ari; Pitkänen, Petteri; Rasi- Karjala. Alueelliset ympäristöjulkaisut 220. 52 p. + 1 app. lainen, Kari 2002. Jääkaudet ja ydinjätteen loppusijoitus. In: map. Korkka-Niemi, K. (ed.) Geologian tutkijapäivät 13.- Antikainen, Merja; Backman, Birgitta; Rusanen, Kaisa; 14.3.2002 Helsinki : ohjelma, tiivistelmät, osallistujat. Finér, Leena 2002. Vaikuttaako metsänkäsittely pohjavesi- Helsinki: Geologian valtakunnallinen tutkijakoulu, 18. alueiden veden laatuun? In: Metsätalouden ympäristökuor- Ahonen, Lasse; Luukkonen, Ari; Pitkänen, Petteri; mitus ja sen vähentäminen - tutkimustietoa ja työkaluja, 23.- Rasilainen, Kari; Ruskeeniemi, Timo 2002. Jääkaudet ja 24.9.2002 Kolin luontokeskus ja Kuohattijärvi. Joensuu: ydinjätteen loppusijoitus. Abstract: Ice ages and nuclear Joensuun yliopisto, 13. waste disposal. Geologian tutkimuskeskus. Ydinjätteiden Antikainen, Merja; Lyytikäinen, Ari; Pihlaja, Jouni sijoitustutkimukset. Tiedonanto YST-110. 45 p. 2002. Pohjavesien suojelun ja kiviaineshuollon yhteen- Airo, Meri-Liisa; Karell, Fredrik 2001. Interpretation of sovittaminen : loppuraportti Joensuun seudulta. Abstract: airborne magnetic and gamma-ray spectrometric data related The harmonization of groundwater protection and aggregate to Hammaslahti Cu-Zn-Au deposit in eastern Finland. In: service : final report from the surroundings of Joensuu. Autio, S. (ed.) Geological Survey of Finland, Current Alueelliset ympäristöjulkaisut 259. 55 p. + 1 app. map. Research 1999-2000. Geological Survey of Finland. Special Arvola, Lauri; Kortelainen, Pirkko; Bergström, Irina; Paper 31, 97-103. Kankaala, Paula; Ojala, Anne; Pajunen, Hannu; Käki, Airo, M.-L.; Mertanen, S. 2001. Magnetic signatures Tiina; Mäkelä, Suvi; Rantakari, Miitta 2002. Carbon path- related to Precambrian greenstone-hosted Au mineralizations, ways through boreal lakes : a multi-scale approach (CARBO). northern Fennoscandia. In: Vietnam 2001 : IAGA-IASPEI In: Käyhkö, J. & Talve, L. (eds.) Understanding the global joint scientific assembly, 19-31 August 2001, Hanoi, system : the Finnish perspective. Helsinki: Finnish Global Vietnam : abstracts. Hanoi: IAGA : IASPEI, 263. Change Research Programme FIGARE, 97-106. Airo, M.-L. 2002. Aeromagnetic and aeroradiometric Autio, Sini 2000. Kullan kimalluksesta Kultalaksi. Vuori- response to hydrothermal alteration. Surveys in Geophysics teollisuus 58 (1), 12-14. 23 (4), 273-302. Autio, Sini 2001. Teollisuusjätteet uhkaavat Unkarin Alakukku, Laura; Jaakkola, Antti; Hänninen, Pekka; Tisza-jokea. Vuoriteollisuus 59 (3), 18-21. Ristolainen, Antti 2002. Relationship between spatial Autio, Sini (ed.) 2001. Geological Survey of Finland, variability of soil physical properties and yield - MaSa- Current Research 1999-2000. Geological Survey of Finland. study. In: Implementation of precision farming in practical Special Paper 31. 167 p. agriculture, 10-12 June 2002, Skara, Sweden : NJF seminar Backman, Birgitta; Mäkinen, Risto; Suokko, Tuulikki no. 336. [S.l.]: Nordic Association of Agricultural Scientists 2001. Valtakunnallinen pohjaveden seuranta Suomessa. (NJF), 1 p. Abstract: Nation-wide groundwater monitoring in Finland. Alapassi, Markus; Rintala, Jari; Sipilä, Pekka 2001. Maa- In: Idman, H. & Rönkä, E. (eds.) Kestävä kehitys - tutki- ainesten ottaminen ja ottamisalueiden jälkihoito. 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Layer-charge BRIDGE and SVEKALAPKO projects on “Archaean and evaluation of expandable clays from a chronosequence of Proterozoic plate tectonics : geological and geophysical podzols in Finland using an alkylammonium method. Clay records”, November 1-3, 2001, VSEGEI, St. Petersburg, Minerals 36 (4), 571-584. Russia. St. Petersburg: VSEGEI, 20. Gornostayev, Stanislav S.; Hanski, Eero J.; Laajoki, Elo, S.; Zhdanova, L.; Chepik, A.; Pesonen, L. J.; Philip- Kauko V. O.; Popovchenko, Sergiy E.; Kornienko, Peter K. pov, N.; Shelemotov, A. 2000. Comparative geophysical 2002. New data on mineralogy of the Kapitanovskoe chrom- description and modelling of Lappajärvi and Jänisjärvi ite deposit, Ukrainian Shield. In: Cook, N. J. (ed.) Metal- impact structures, Fennoscandian Shield. In: Plado, J. & logeny of Precambrian shields, Kyiv, Ukraine, September 13- Pesonen, L. J. (eds.) Meteorite impacts in Precambrian 26, 2002 : the abstracts. 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September 2001, Perth, Western Australia : Workshop WS1 Balykin, P. A.; Tran, T. H.; Ngo, T. P. 2002. Permian- : Orogenic lode-gold deposits : nature, global distribution, Triassic komatiites and their Os isotopic characteristics in tectonic setting, genesis, wallrock alteration, and computer northwestern Vietnam. In: Abstracts of the 12th Annual V. based exploration. Perth: Geoconferences. 224 p. M. Goldschmidt Conference, Davos, Switzerland, August Groves, D. I. (comp.); Eilu, P. (ed.) 2002. Metallogeny of 18-23, 2002. Geochimica et Cosmochimica Acta 66 (15A), Precambrian shields : orogenic gold workshop : nature, global A309. distribution, tectonic setting, genesis, wallrock alteration, and Hanski, Eero 2002. Vikajärvi. Suomen geologinen kartta computer-based exploration, Kiev, Ukraine, 17 September 1:100 000 : kallioperäkartta lehti 3614. 2002 [Electronic resource]. 224 p. Optical disc (CD-ROM). 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