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Present Situation of Radioactive Contamination in and Around the Former Soviet Union's Scmipalatliisk Nuclear Test Site

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Present Situation of Radioactive Contamination in and Around the Former Soviet Union's Scmipalatliisk Nuclear Test Site JP0150451 JAERI-Conf 2000-016 4.2 Present Situation of Radioactive Contamination In and around the Former Soviet Union's Scmipalatliisk Nuclear Test Site M. Yamamoto,1* M. Hoshi,2 J. Takada,2 T. Tsukatani,3 S. Oikawa,4 I. Yoshikawa,5 T. Takatsuji,5 A. Kh. Sekerbaev6 and B. I. Gusev6 'Low Level Radioactivity Laboratory, Kanazawa University, Ishikawa 923-1224, Japan 2InternationalRadiation Information Center, Research Institute for Radiation Biology and Medicine, Hiroshima University, Hiroshima 734-8553, Japan 3Kyoto Instituteof Economic Research, Kyoto University, Kyoto 606-8501, Japan 4Japan ChemicalAnalyticalCenter, Inage, Chiba 263-0002, Japan 5Faculty of EnvironmentalStudies, Nagasaki University, Nagasaki 852-8521, Japan 6Kazakh Scientific Research Institute for RadiationMedicineand Ecology, Semipalatinsk, The Kazakhstan Republic Abstract Field missions were sent to the Semipalatinsk regions to investigate the present radioecologicalsituationas a a result of the radioactivefalloutfrom nucleartest explosions carried out at the former Soviet Union's Semipalatinsk nuclear test site (SNTS). For this purpose, surface and core soil samples were collected at more than 60 sites, including several settlements such as Dolon, Chagan and Sarzhal, within and outside the SNTS territory. The radioactivities of long-lived radionuclides, l37Cs, 238Pu and 239-240Pu, and the atomic ratio of 24oPu/239Pu were determined in combination with non-destructive g-ray spectrometric method and radiochemical separation followed by a-particle spectrometric 137 239 a40 and/or ICP-MS methods. The results showed a distinction of Cs and - ptt inventories in soil depending on a sampling sites. Although 137Cs was within typical environmental levels except for the area near the first nuclear test site and Balapan, 239240Pu was at elevated levels in all areas we visited. This high Pu contamination was recognized to be due to the weapons-grade Pu from the SNTS by the measurement of 24OPu/239Pu atomicratioin soil samples. Keywords Atomic bomb, Semipalatinsk, Former USSR, Radioecology, Long-lived radionuclides, 137Cs, 239>24° Pu, ^Pu/^Pu atomicratio, Residual radioactivity, Soil * To whom all correspondence should be addressed. -172- JAERI-Conf 2000-016 Introduction The Former USSR nuclear weapons testing program was mainly carried out at two test sites: one is the Novaya Zemlya test site in the Russian Arctic for large yield tests (total yield of atmospheric tests about 240 megatons) and the other the Semipalatinsk nuclear test site ( hereafter referred to as SNTS) in the northeast corner of Kazakhstan for smaller yield tests (about 6.6 megatons). Most of the tests at the former site were conducted at high altitudes, minimizing local fallout At the latter test site (approximately 18,500 km2, see Fig. 1), 456 nuclear tests were conducted over a period of 40 years from the first nuclear explosion on 29 August 1949 through the last on 19 October 1989, including 86 atmospheric, 30 surface and 346 underground tests (Fig. 1) (Bocharov et al., 1989; Dubasox etaL, 1994; Shapiro etaL, 1998). In the SNTS, the experiments were performed at the different places within the territory and varied in type and size, and resulted in the local and global dispersion of radioactive materials. As a consequence, residual radioactivities in the soil from 137 90 23823924024t 241 long-lived radionuclides, such as Cs, Sr, pu and Am, are still observed in the area today. These nuclides remaining on the land have a potentialhuman hazard in the long time. The principal hazard from nuclear test explosions to human is from local (early) fallout from atmospheric ground and near -ground bursts. Some of the underground nuclear tests also emitted a huge amounts of gaseous radionuclides on the ground. Hence, the effects of human health by ionizing radiation - effects of long-term protracted low-dose radiation exposure on human in particular - of scientific and practical importance, together with an assessment of the impact of the nuclear tests on radioactive contamination of land. Information on the radiation situation there is, however, very limited (Tsyb etal., 1990;Gusev, 1993; Stepanov et al., 1994; Logachev, 1994; Shapiro etcd., 1998). Recently, in connection with the "opening" of the SNTS, intensive studies have, at long last, begun (Takada et al., 1996; Yamamoto et al., 1996a; Yamamoto et al., 1996b; Kazachevskiy et al., 1998; Shebell and Hutter, 1998; Yamamoto et al., 1998; Yamamotoef al, 1999). To serve as an aid to resolve such problems in the SNTS region, studies have begun to investigate the present situation of radioecology in and around the SNTS. Emphasis has been placed to the radioecology of Pu, because any systematic data or studies have not been performed until now. Three objectives are considered in this paper: (1) an evaluation of geographic distribution of 239'240Pu, including 137Cs, in soil samples within and 239 240 outside the SNTS, (2) an information about geochemical association of ' pu with soil, and (3) an identification of the contamination sources of Pu and 137Cs in the soil with 24OPu/239Pu isotopic ratios. The data used in this paper include the field studies on -173- JAERI-Conf 2000-016 residual radioactivities in and around the SNTS carried out during the last five years and some of the data have been already published elsewhere (Yamamoto et al., 1996a; Yamamotoefai, 1996b; Yamamotoef al, 1998; Yamamotoe? al, 1999). Materials and Methods (A) Soil sampling Soil samples were collected for measurement At each site, three to five surface soil samples were taken at a spacing 2-3 m apart from each other, with a diameter of 4.7 cm and a depth of 10 cm. Furthermore, a A.I cm diameter core soil sample was taken at the center of the surface soil sampling spots by inserting a stainless steel pipe to a depth of about 30 cm. While 10 cm-deep soil samples were not divided, most of the 30 cm-deep core samples were subdivided carefully into 6 parts of 0-5, 5-10, 10-15, 15-20, 20-25 and 25-30 cm depth from the surface. After air-dried and crushed, these samples were sifted through a 2-mm mesh screen to remove pebbles. The following samples were used. (l)Soil samples within the territory of the SNTS (Fig. 2 and Appendix I) In 1995, in collaboration with the National Nuclear Center (NNC) in Kazakhstan, soil samples were collected along the road between Kurchatov and the hypocenter of the first nuclear test, around the hypocenter, and along the roads from Kurchatov to the underground nuclear test sites in the south direction (Balapan and Mt Degelen). Soil samples were also collectedin Sarzhal, settlementlocatedto the southeast of the SNTS. (2) Soil samples outside the SNTS (Fig. 4 and Appendixes I and II) From 1995 to 1997, soil samples were collected by the same method used for the soil samples within the SNTS as a collaborative study with the Kazakh Scientific Research Institute for Radiation Medicine and Ecology. Sampling sites are Mostik, Dolon, Chagan, etc., - adjoining settlements of the SNTS, where exposure doses are reported to be relatively high. The samples were also collected from Semipalatinsk City and some settlements including Korosteli, to the north of Semipalatinsk City in the direction of the Altai District, and the roads between Semipalatinsk City and Ust' -Kamenogork City and it's adjoining areas. (B) Radioactivity measurement Soil sample (50-80 g) was first placed into a plastic container with an inner diameter of 6 cm and a depth of 2 cm. After stored for about 3 weeks, gamma-emitting radionuclides were determined by gamma-ray spectrometry using a low background Ge detector for 137Cs and other gamma-ray emitters and a planar type Ge detector (low energy photon spectrometer: LEPS) for 210Pb and 234Th (238U). The spectrometers were calibrated with -174- JAERI-Conf 2000-016 standards prepared from New Brunswick Laboratory (NBL) reference materials No. 42-1 (4.04 % uranium) and anaiyticalgrade KG. As for Pu, Pu and ' Pu concentrations in soil were mainly determined together with 24oPu/239Pu atomic ratio. It is well known that Pu in soil contaminated with global fallout can be extracted almost quantitatively by leaching with heat using mineral acids such as nitric acid (Japanese Science and Technology Science, 1979). However, concerning local (close-in) fallout Pu in a nuclear test site, the studies of the U, S. Nevada nuclear test site and it1 s surrounding areas showed that there were refractories, and some fractions were trapped in melted atomic bomb components and hydrated silica soil grains ( Krey and Hardy, 1970; Hardy etal., 1972; Hardy, 1976; Krey and Bogen, 1987). Careful leaching or dissolution of Pu becomes , therefore, key point for analysis. For the 10 cm deep soil samples, a stepwise leaching for Pu analysis using 20-40 g of the dried samples was particularly adapted to get information on the geochemical association of Pu with soil components. Before starting the analysis, the dried sample was ashed at about 500 Ae* and the following method was used in order; (1) leaching with c.HNO3+H2O2 , (2) leaching with a mixture of 10M HNO3 and 0.1M HF and (3) complete decomposition of the residue by alkali (NaOH) fusion or decomposition with HNO3+HF+HC1O4 . As for core soil samples, aliquots (10-50 g) of the dried samples were at first ashed at about 500 Ae" and then were, without stepwise leaching, decomposed with a mixture of HNO3 a42 and HF, followed by HC1O4 , in the presence of Pu as a yield tracer. On the other hand, for the measurement of the 24OPu/239Pu atomic ratio, an aliquots of 20-50 g of the dried sample were decomposed in a manner similar to the method described above, in the absence of a yield tracer such as 242Pu by taking into account of the possible contamination of Pu isotopes from the added tracer.
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