Polonium-210 and Other Radionuclides in Terrestrial, Freshwater And
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StrålevernRapport • 2012:3 Polonium-210 and other radionuclides in terrestrial, freshwater and brackish environments Results from the NKS project GAPRAD (Filling knowledge gaps in radiation protection methodologies for non-human biota) Reference: Gjelsvik R, Brown J, Holm E*, Roos P**, Saxen R*** and Outola I*** Polonium-210 and other radionuclides in terrestrial, freshwater and brackish environments. Results from the NKS project GAPRAD (Filling knowledge gaps in radiation protection methodologies for non-human biota) * University of Lund, Sweden until April 2009** Risø national laboratory, Denmark *** Radiation and Nuclear Safety Authority, Finland SrålevernRapport 2012:3. Østerås: Norwegian Radiation Protection Authority, 2012. Key words: Po-210, environmental impact assessment, levels, transfer, concentration ratios, human biokinetics Abstract: The background and rationale to filling knowledge gaps in radiation protection methodologies for biota are presented. Concentrations of Po-210 and Pb-210 are reported for biota sampled in Dovrefjell, Norway and selected lake and brackish ecosystems in Finland. Furthermore, details in relation to Po-210 uptake and biokinetics in humans based on experimental studies are recounted. Referanse: Gjelsvik R, Brown J, Holm E*, Roos P**, Saxen R*** and Outola I***. Polonium-210 and other radionuclides in terrestrial, freshwater and brackish environments. Results from the NKS project GAPRAD (Filling knowledge gaps in radiation protection methodologies for non-human biota) * Universitetet i Lund, Sverige ** Risø nationale laboratorium, Danmark *** Finske strålevernsmyndigheter, Finland StrålevernRapport 2012:3. Østerås: Norwegian Radiation Protection Authority, 2012. Language: English. Emneord: Po-210, konsekvenser for miljø, nivå, overføring, konsentrasjons ratio, biokinetikk på mennesker. Resymé: Bakgrunnen og viktigheten av å fylle kunnskapshull innen metoder for å beskytte biota fra stråling er presentert. Rapporten viser konsentrasjon av Po-210 og Pb-210 i biota fra Dovrefjell i Norge og utvalgte innsjøer og brakkvannssystemer i Finland. Videre er detaljer om opptak av Po- 210 og biokinetikk i mennesker utført i Sverige. Head of project: Runhild Gjelsvik Approved: Per Strand, director, Department for Emergency Preparedness and Environmental Radioactivity. 43 pages. Published Jan. 2012. Coverphoto: Runhild Gjelsvik Orders to: Norwegian Radiation Protection Authority, P.O. Box 55, N-1332 Østerås, Norway. Telephone +47 67 16 25 00, fax + 47 67 14 74 07. E-mail: [email protected] www.nrpa.no ISSN 0804-4910 ISSN 1891-5191 (online) 3.2.1 Sampling and study area 15 3.2.2 Sample treatment (STUK) 15 3.2.3 Analyses of 210Pb and 210Po (STUK) 16 3.2.4 Results 18 3.2.5 Discussion 23 4.3.1 Study area 26 4.3.2 Sampling 26 4.3.3 Analyses of 210Po and 210Pb 29 4.3.4 Results 29 4.3.5 Discussion 32 4.4.1 Samples and analyses 34 4.4.2 Results 34 measurements of 210Po in aquatic and terrestrial environments that would lead to the derivation of information on the levels of this radioisotope in plants, animals and the biotic components of their habitat (i.e. water, soil) This report summarises some of the key providing basic information on transfer where findings from the activity of filling knowledge practicable. Furthermore, it was envisaged that gaps in radiation protection methodologies for data on levels would allow more robust non-human biota, the GAPRAD project. The background dose calculations to be performed activity was funded as part of the Nordic subsequently. A further objective was to study Nuclear Safety Research (NKS) under the the biokinetics of polonium in humans thereby programme emergency preparedness including augmenting and improving the database upon radioecology and emergency preparedness which committed effective doses to humans related information and communication issues are derived. In this way the information (NKS B-programme), started in May 2007 and generated will be of direct relevance and was completed by December 2008. The project interest for both human and non-human impact was conducted as a collaborative effort assessments. between the Norwegian Radiation Protection Authority, University of Lund in Sweden, RISØ National Laboratory in Denmark and the The report has been spilt into 5 chapters. Nuclear Safety Authority (STUK) in Finland. Following the introduction, rationale and background to the study (chapters 1 and 2), the report describes the work performed in relation to determining 210Po in freshwater and brackish The subject of environmental protection from 210 radiation is highly topical as evidenced by the environments (chapter 3), followed by Po in terrestrial environments. The final chapter recent interest afforded the subject of by the 210 International Commission on Radiological deals with Po biokinetics in humans. Protection (ICRP 2007, ICRP 2003). Within this context, the rationale driving the activity related to the fact that numerous data gaps had been identified in the transfer and background characterisation components of existing environmental impact assessment methodologies. Informed by the identification of such gaps, focus was placed on collation of activity concentrations of 210Po and 210Pb in selected biota and fauna from terrestrial, freshwater and brackish water environments. Furthermore, in response to the observation that often conflicting data has been published in the biokinetics of polonium in humans, an objective was introduced to collate information on gastrointestinal uptake and residence times in Man. The key aim of this report is to provide new information on 210Po (and where appropriate its grandparent 210Pb) behaviour in environmental systems including pathways to humans. The plan was primarily to achieve this through Atmospheric 210Pb concentrations are positively correlated with the size of underlying landmasses, whereas terrestrial areas covered by ice and snow and marine areas including islands have reduced atmospheric concentrations of 210Pb (El- Daoushy 1988a, El-Daoushy 1988b). Polonium was discovered by Pierre and Marie 210 Currie in 1898 in the course of research on the Furthermore, the deposition of Pb is directly radioactivity of uranium and thorium minerals. correlated with the level of precipitation (Hill They found that polonium (Po) behaved in a 1960). The annual deposition varies from a few Bq per m2 such as in the Antarctic (Roos et al. similar way to bismuth (Bi) and subsequently -2 were able to separate it from Bi by vacuum 1994) to several hundred Bq m for Japan (El- sublimation. Polonium-210 is highly radiotoxic Daoushy 1988a). The annual deposition in central Sweden was estimated to be about 63 with a specific activity of 166 TBq/g. It is a -2 -1 daughter product in the 238U decay chain Bq m year (Persson 1970) and in through 210Pb and 210Bi but can also be Scandinavia, the radionuclide is deposited produced by neutron activation of 209Bi. It is continuously to earth at a rate of approximately 55 Bq m-2 annually (El-Daoushy 1988a). the alpha emitter which gives the highest dose 210 210 to humans via food intake. Figures 2.1, 2.2 and 2.3 show the Pb, Po activity concentration in air and the activity ratio 210Po/210Pb over the North and South The main source of 210Pb in the atmosphere is Atlantic measured during Swedish Antarctic 222Rn which is exhaled from the ground at a and Arctic Expeditions. The equilibrium ratio 10 rate of 18 mBq m-2 s-1 producing a total of U to Po is 1.19 x 10 , so that the Po inventory of 48 EBq per year. This concentration in uranium ores is less than 0.1 corresponds to an annual production rate of mg/ton. With the advance of nuclear reactors atmospheric 210Pb of 23 PBq (Persson 1970). and their intense neutron fluxes, the reaction 209 210 210 This is a surprising figure compared to the Bi (n, γ) Bi → Po became economically amount of 137Cs from the Chernobyl accident feasible. This process is currently used for the and is further contextualised by noting that the production of Po. 210 radiotoxicity of Po is much higher than that of 137Cs. Burton and Stuart (Burton and Stuart 1960) found that the concentration gradient of 210Pb increased sharply in the vicinity of the tropopause. The source of 210Pb in the stratosphere is explained by the presence of A number of other isotopes of Po also appear ascending air at the equator which carries not in naturally occurring decay series. However, only 210Pb but also 222Rn and its daughter- 210 they have all short half-lives. One difficulty in products, from which Pb will be formed. working with 210Po is its high specific activity (166 TBq/g). The intensive radiation of 210 milligrams quickly decomposes most organic Deposition of Pb, associated with aerosols in complexing agents and even solvents. Crystal the atmosphere, occurs via mesoscale structures of solids are quickly destroyed or transportation process, sedimentation and altered. Therefore, 209Po is used instead which precipitation. Early models concerning the 209 210 can be produced by bombarding Bi with atmospheric Pb transport were based on the protons or deuterons in a cyclotron. However, vertical movement of the radioisotope into the more 208Po is produced than 209Po. Both 209Po troposphere at the equator followed by lateral and 208Po can be used as radiochemical yield movement to mid-latitudes and deposition, determinants. whereas more recent, refined models have included regional sources of 222Rn to account 210 more robustly for the Pb deposition rates Polonium is in the same group as Se and Te in observed across the major continents the periodic system with oxidation state +4. It (Macdonald et al. 1996). is a silver coloured half metal. The melting point is 527 K and the boiling point 1235 K. It environmental levels appears to involve the is however clear that Po generally evaporates formation of a MnO2 co-precipitate. Polonium at much lower temperatures. Table 2.1 shows is strongly absorbed in HCl media on anion the decay properties of the most important Po exchangers. It can be extracted into isopropyl isotopes.