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Time Trends of Anthropogenic Radionuclides at Utsira

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Time Trends of Anthropogenic Radionuclides at Utsira Time trends of anthropogenic radionuclides at Utsira Gordon C. Christensen', Elisabeth Strålberg' and Elis Holm2 'Institute for Energy Technology (IFE), N-2027 Kjeller (Norway) 2Department of Radiation Physics, Lund University, S-221 85 Lund (Sweden) Introduction Institute for Energy Technology has annually collected the brown alga Fucus vesiculosus at several sampling locations along the Norwegian coast since 1980, mainly in August and September [1,2]. At the south-western location Utsira, monthly samples have been collected regularly since January 1986. Time series for 99Tc and 137Cs in Fucus samples from Utsira are presented in this study. The results will be discussed with regard to Sellafield discharges and outflow from the Baltic Sea. Materials and methods The Fucus vesiculosus samples were dried and homogenised before analysis. The pretreatment and the gamma spectrometric analyses have been performed at Kjeller and the analysis of 99Tc at Lund. The Fucus samples were dried at 105 'C, homogenised and analysed for gamma emitters using high purity germanium gamma spectrometry and computerised spectrum analysis. Technetium was extracted by TBP from sulphuric acid-hydrogen fluoride media. Backextraction was done from sodium hydroxide solution from which media technetium was electrodeposited onto stainless steel discs. As radiochemical yield determinant 99mTc was used. After decay of the yield determinant technetium was measured by an anticoincidence shielded GM counter [3]. Results and discussion Caesium-1 37 The transit time from Sellafield to the southern coast of Norway has been estimated to 3-4 years [4]. Knowledge of the annual discharge of 137Cs from Sellafield year i [5,6] allow us to calculate Fucus transfer factors (FTFs) from Sellafie]d to the southernmost locations based on concentrations in Fucus in year i+4. The calculations were done for the years 1980-85 when other sources than Sellafield were negligible. For transport of 137Cs from the Baltic Sea, the transit time from the Kattegat is estimated to be 2 years to Utsira. The annual net water outflow from the Belt Sea to the Kattegat has been estimated to 1170 km3 [7]. By using published data for the 137Cs concentrations (Bq m-3) in the Kattegat waters (box 71 of the RisØ box model [7]) for year i [8] and measured concentrations of '37Cs in Fucus (Bq kg-' d.w.) at Utsira for year i+2, "Baltic" FTFs have been calculated. These calculations were done for the years 1990-95 when other sources than the Chernobyl fallout were negligible. An average value of 0.035 (Bq kg-' d.w. per TBq year-1) was found. The calculated FTFs do in fact 61 include the outflow of 137Cs via Norwegian rivers to the Skagerrak, as this source also influences on the concentration of '37Cs in the Fucus. Calculations show, however, that it probably contributes to much less than one third of the total input to these waters of Chernobyl related 137Cs [9]. The Fucus transfer factors were then used to calculate the contribution from the different sources compared to the total amount of radiocaesium present in the Fucus at Utsira. The results are shown in Figure 1. Our calculations show that in the early 1980's, approximately all the radiocaesium in the seaweed at these sampling locations originated from Sellafield. After 1990 the contribution from Sellafield is nearly negligible. Since 1986, fallout from the Chernobyl accident makes the most important contribution to radiocaesium in Fucus. Based on measured 137Cs concentrations of 40-60 Bq m-3 in Kattegat sea water [8] and a net annual outflow of 1170 km3 [7], calculations show that 50-70 TBq of 137Cs has been transported annually out of the Baltic Sea the last five years. Technetium-99 The results for 99Tc in the Fucus samples from Utsira from January 1995 to November 1999 are shown in Figure 2. The discharges of Tc from the EARP plant at Sellafield started in April 1994. It is evident from the results that the discharge front has reached Utsira waters already in January 1997, a little less than 3 years later. This is somewhat faster than the average transport time of 3-4 years calculated for 137Cs [4]. The annual discharges reached a peak in 1995 [5], as shown in Figure 3. The reduction in the 99Tc concentration found in 1999 (see Fig. 2), indicates about the same average transport time for 99Tc as for 137Cs. Analyses of samples from 2000 may confirm this. The variations of the concentration of 99Tc shown in Figure 2 may be a combined effect of Sellafield discharge patterns and annual biophysical/-chemical mechanisms of uptake in the Fucus. The lower concentrations in the summer season indicate that 99Tc is governed by some different mechanisms compared to '37Cs which shows a concentration peak in Fucus in the summer season. Annual mean concentrations of 99Tc in monthly Fucus samples from Utsira have been calculated and is shown in Figure 3 together with annual Sellafield discharges. The Fucus values for 1995 and 1996 reflect the small discharges before 1994. Calculations give Sellafield FTFs of 4.2, 4.3 and 10.3 (Bq kg-' d.w. per TBq year-1) for transit times of 3, 3.5 and 4 years, respectively. Conclusions The major source of 137Cs in Fucus vesiculosus at the coast of southern Norway has since 1990 been the Chernobyl fallout, and most of this activity is due to the outflow from the Baltic Sea. The increased Sellafield discharges of 99Tc as from 1994 reached Utsira early 1997. Preliminary calculations show average transit times of 3-4 years and Fucus transfer factors of 4-10 Bq kg-' d.w. per TBq year-1 at Utsira. 62 References [1] Christensen, G.C., Radioactivity in Fucus vesiculosus along the Norwegian North Sea and Skagerrak coast 1980 - 1983, pp. 133-140 in "Study of radioactive materials in the Baltic Sea", IAEA-TECDOC-362 (1986). [2] Christensen, G.C., Selnaes, T.D., Study of marine radioactivity along the Norwegian coast 1980-1994, pp. 618-622 in Proceedings of an International Symposium on Environmental Impact of Radioactive Releases, IAEA, Vienna, Austria, 8-12 May 1995. [3] Holm, E., Rioseco, J., Garcia-Leon, M., Determination of 99Tc in environmental samples, Nucl. Instr. Meth. Phys. Res., 223, 204 (1984). [4] Dahlgaard, H., Bergan, T.D.S., Christensen, G.C., Technetium-99 and caesium-137 time series at the Norwegian coast monitored by the brown alga Fucus vesiculosus, in Proceedings Part 1 of International Symposium on Radionuelides in the Ocean - RADOC 96-97, Cherbourg-Octeville, France, 7-11 October 1996, Radioprotection - Colloques, Volume 32, C2 (1997) 353-358. [5] BNFL, Annual Report on Radioactive Discharges and Monitoring of the Environment 1994. Directorate of Health, Safety and Environmental Protection, Risley, UK (1995). [6] Dahlgaard, H., personal communication (2001). [7] Nielsen, S.P., Modelling and Assessment of Doses to Man, In Proceedings from the Marina- Balt Seminar, Stockholm, 9-11 June 1998, The radiological exposure of the population of the European Community to radioactivity in the Baltic Sea, Radiation Protection 110, EUR 19200, 177-317 (2000). [8] Herrmann, J., Levels of Radioactivity, In Proceedings from the Marina-Balt Seminar, Stockholm, 9-11 June 1998, The radiological exposure of the population of the European Community to radioactivity in the Baltic Sea, Radiation Protection 110, EUR 19200, 77-129 (2000). [9] Christensen, G.C., Stralberg, E., Can the outflow of radiocaesium from the Baltic Sea be detected in brown algae along the Norwegian coast? In Proceedings from the Marina-Balt Seminar, Stockholm, 9-11 June 1998, The radiological exposure of the population of the European Community to radioactivity in the Baltic Sea, Radiation Protection 110, EUR 19200, 433-438 (2000). 63 20,0 18,0 r Measured - Calculated Sellafield origin 16,0 /--- Calculated Baltic origin 14,0 12,0 a10,0 8,0 - 6,0 4,0 2,0 0,0 80 81 82 83 84 85 86 87 88 89 90 91 92 93 94 95 96 97 98 99 Year Figure 1. Calculated contributions from Sellafield and the Baltic Sea to the measured concentrations of 137Cs in Fucus vesiculosus at Utsira. 600 500 400- <> 300 200- 100 LO LO LO LO tD tO LO CD r- r- r r- æ CD æ 00 æO aæ æ o LO LO LO Lo LO LO LO LO LO LO LO LO LO LO LO LO LO LO LO LO 0 LO LO LO LO LO o LO LO LO LO LO LO LO LO LO LO LO LO LO LO 0 - r-:- d *4* r- o - -- r- o _- r- o 0o - ri - - .i -r =-t - . r - ,2 r -r r4w - Date Figure 2. 99Tc in Fucus vesiculosus at Utsira January 1995- November 1999. 64 450 400 = * Sellafield discharge (Tbq/year) 350 - 10Utsira Fucus ves. Tc-99 300 - (Bq/kg dw) 250- 200- 150 100 _ 50- 1990 1991 1992 1993 1994 1995 1996 1997 1998 1999 Figure 3. Annual means of 99Tc discharges from Sellafield 1990-1999 and 99Tc concentrations in Fucus vesiculosus at Utsira 1995-1999. 65.
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