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Study of Migration Behavior of Technogenic Radionuclides in the Yenisey River-Kara Sea Aquatic System

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Study of Migration Behavior of Technogenic Radionuclides in the Yenisey River-Kara Sea Aquatic System JP0150450 JAERI-Conf 2000-016 4. Invited presentation 4.1 STUDY OF MIGRATION BEHAVIOR OF TECHNOGENIC RADIONUCLIDES IN THE YENISEY RIVER-KARA SEA AQUATIC SYSTEM Yu. Kuznetsov1, E. Legin1, V.Legin \ A. Shishlov2, Yu. Savitskii2, A. Novikov3, and T. Goryachenkova3 1Khlopin Radium Institute, St. Petersburg 2Krasnoyarsk Mining and Chemical Combine, Krasnoyarsk-26 institute of Geochemistry and Analytical Chemistry, Russian Academy of Sciences, Moscow ABSTRACT For 35 years Krasnoyarsk Mining-Chemical Combine (MCC) manufactures weapon plutonium in single-pass production reactors cooled with water of the Yenisey River. Water discharge from these reactors is the major source of radioactive contamination of the Yenisey River. We have demonstrated that after putting the reactors out of operation (in late 1992) the contamination level of the Yenisey River with short-lived radionuclides considerably decreased, and now the radioactive contamination is caused essentially by Cs-137, Eu-152, Pu-239,240, Sr-90, and Am-241, whose concentration in the aqueous phase is lower than in bottom sediments and, particularly, flood-land deposits by several orders of magnitude (except for Sr-90). The flood-land deposits are classified with the most contaminated environmental objects in the territories under the impact of MCC: their radioactivity is comparable with that of low-level waste. Taking into account the considerable depth and area of the flood-land deposits, this allows their classification as a great technogenic radiation anomaly. Comparison of the maximal Cs-137 and Pu-239,240 levels in flood-land soils and bottom sediments of the Yenisey River with those in bottom sediments of the Pripyat' River and the Kiev reservoir shows that these values are close each to other. A direct correlation is found between the spatial distribution of Cs-137 on the one hand and Pu-239,240, Eu-152, and Am-241 on the other hand in the aqueous phase and bottom sediments, which is not the case for Sr-90. Data on the distribution coefficients of the indicated radionuclides between the deposits and aqueous phase (obtained with actual and model systems) and also on the radionuclide distribution throughout geochemical mobility forms suggest that the essential part of Cs, Pu, Eu, and Am migrates with fine-disperse suspended material, the transport and distribution of which is controlled by the hydrological regime of the Yenisey River. By contrast, strontium migrates as soluble species weakly sorbed by the solid phase, causing the observed low content of Sr-90 in flood-land deposits and bottom sediments of the Yenisey River. The indicated migration behavior of radionuclides is characteristic of the Yenisey Gulf and the adjacent part of the Kara Sea also. We made similar conclusions when studying the migration behavior of Cs-137, Pu-239,240, and Sr-90 in the Kiev reservoir (1987). The formation of radioactive flood-land deposits is provided by rapid deposition of suspended material in stagnant zones during periodical flood. Humus compounds contribute significantly to accumulation of radionuclides in. the flood-land deposits and bottom sediments, which is supported by the observed -138- JAERI-Conf 2000-016 correlation' between the radionuclide (Pu, Am, Eu) and total organic carbon distributions in them. Radiochemical analysis of separate fractions showed that about 20% of Pu and Am are associated with the organic fraction: Pu is nearly equally distributed between humic and fulvic acid fractions, whereas Am is preferentially associated with the fulvic acid fraction (the most mobile fraction of humus matter). It was demonstrated in model experiments that the calcium- hydrocarbonate type of water of the Yenisey River causes suppression of formation of mobile fulvate complexes of hydrolyzable radionuclides and, therefore, their transfer into the aqueous phase. In combination with the observed very high distribution coefficients of the radionuclides and low content of their mobile geochemical forms in flood-land deposits of the Yenisey River this suggest that they cannot contribute somewhat significantly to the secondary radioactive contamination of the river water by all mechanisms except migration by mechanical transfer. The major source of radioactive contamination of the Yenisey River is the Krasnoyarsk Mining-Chemical Combine (MCC), known as Krasnoyarsk-26, situated at the right bank of the Yenisey River, 60 km to the northeast from the Big Krasnoyarsk. The region is characterized by a complex lay of the ground, including rolling and plain parts. MCC lies partly in the rolling part belonging to the joint zone of the West Siberian platform and the Sayan-Altai-Yenisey folded area. The hydrological regime of the Yenisey River is controlled by the Krasnoyarsk Hydroelectric Power Plant (HPP) put into service in 1967, which is situated approximately 85 km upstream from MCC. It reduces the annual fluctuations in the river flow in the areas affected by water discharge from MCC. Near MCC the river is not frozen throughout the year. The average annual temperature of water is 7°C, the current velocity is 1.7 m/sec, the average width is 1000 m, and the average annual discharge is 2760 m3/sec. The section of the Yenisey River from MCC (discharge of contaminated water) to the Kara Sea is about 2500 km long. Mean annual run-off of the Yenisey River (603 km3/a) is the highest among all the rivers flowing into the Arctic Ocean. For 35 years MCC manufactures weapon plutonium in 3 single-pass production reactors cooled with water of the Yenisey River. It is water discharge from these reactors that the major source of radioactive contamination of the Yenisey River. Two single-pass production reactors were put out of operation in late 1992. The third, close-cycle power reactor provides heat supply of the town; only control rod cooling water is discharged to the river from it. The radioactive contamination of the Yenisey River before putting the reactors out of service was determined by short-lived activated and fission products (Na-24,P-32,Sc-46,Cr- 51,Mn-54,56,Co-58,Fe-59,Cu-64,Zn-64,Nb-95,Ru-103,106,Sb-124,Cel41,144,Np-239). Contribution of long- and medium-lived radionuclides (Cs-137, Sr-90, Pu-239,240, Co-60, Eu-152) to the total specific radioactivity of water was small [1.2]. Major part of these radionuclides (except Sr-90) was accumulated in flood-land deposits and bottom sediments. When the production reactors were in service, considerable supply of short-lived radionuclides to water, biota, bottom sediments and flood-land deposits was observed [1, 2]. Although at all times the contamination level of most radionuclides in the Yenisey River water was substantially lower than the maximal permissible values for drinking water (in correspondence with NRB-96 regulations), the Na-24 and P-32 concentrations in some species of industrial fish were close to the maximal permissible radiation dose accepted for the critical group of population eating river fish [2]. After putting the reactors out of service -139- JAERI-Conf 2000-016 the radioactive • contamination of river water and fish abruptly decreased, and the concentration of long-lived radionuclides in it were close to the global level. Somewhat different pattern is observed in the flood-land soils and bottom sediments, which, in contrast to water bulk, are characterized by certain inertia with respect to changing concentration of long- and medium-lived radionuclides in them: thus, even after putting the single-pass reactors out of operation, these sediments preserve high contamination levels with Cs-137, Pu-239,240, Co-60, Eu-152, and Eu-154. In contrast to other studies, where the major attention was paid to short-lived radionuclides, in this work, aimed at long-term prognosis of the radiation situation in the territories under the impact of MCC, we focused, naturally, on the migration behavior oif i i yi ddu 6 au 0 a of long- and medium-lived radionuclides (Cs-137, Sr-90, Pu-239,240 Am-241, Eu-152, Co-60). In the most thoroughly studied section of the riverbed (up to 600 km downstream the discharge point of contaminated water from MCC) unconsolidated bottom sediments are not typical, since the river bottom is largely rocky, covered by coarse pebble. The bottom sediments are found in stagnant parts of the river (tail parts of island, inlets, etc.), where suspended material is actively deposited. The sediments are composed essentially of various fractions of silted sand. It is these sediments that are most strongly contaminated with radionuclides (except Sr-90). Thus, the maximal radionuclide contents (Bq/kg dry sample) found in them are presented in Table 1: Table 1. Maximal radionuclide contents (Bq/kg dry sample) in bottom sediments and flood-land soils of the Yenisey River. Bottom sediments Content Cs-137 Sr-90 Pu-239,240 Am-241 Eu-152 Co-60 Bq/kg 950 20 6.4 1.5 265 310 dry sample Flood-land soils Content Cs-137 Sr-90 Pu-239,240 r Am-241 Eu-152 Co-60 Bq/kg 4000 25 30 5 2000 1500 dry sample The most contaminated objects in the Yenisey River basin are flood-land deposits (soils). The comparable contamination levels with Cs-137 and Pu-239,240 were observed in bottom sediments of the estuarine parts of the Pripyat' River after Chernobyl accident [4-6]. Let us compare these data with those obtained for flood-land soils of the Yenisey River (Table 2). It should be noted, that, in contrast to the territories contaminated with Chernobyl radionuclides, flood-land areas of the Yenisey River are not permanently populated; the residence time of people in them is limited, resulting in considerably lower radiation doses taken by them as compared to the case of Chernobyl. -140- JAERI-Conf 2000-016 Table.
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