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Radioactive Environment Contamination and Abilities of the Modern Radiochemistry in the Field of Nuclear Waste Disposal and Monitoring

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Radioactive Environment Contamination and Abilities of the Modern Radiochemistry in the Field of Nuclear Waste Disposal and Monitoring International Conference on HAZARDOUS WASTE. Sources, Effects and Management 12-16 December 1998. Cairo-Ezvpt PL-2 EG0000108 Radioactive Environment Contamination and Abilities of the Modern Radiochemistry in the Field of Nuclear Waste Disposal and Monitoring B.F. Myasoedov and A.P. Novikov V.I. Vernadsky Institute of Geochemistry and Analytical Chemistry, Russian Academy of Sciences, 117975, Kosyginstr. 19, Moscow, Russia. Tel. (7-095) 137-19-17; Fax (7-095) 938-20-54. ABSTRACT The study of environmental contamination caused by anthropogenic impacts and, primarily, by radioactive nuclides is one of the main scientific problems facing contemporary science. This is known as Radioecological monitoring. Decisions regarding the remediation of polluted areas require detailed information about the distribution of radioactive nuclides in terrestrial and aquatic ecosystems, as well as, knowledge about radionuclides occurrence forms and migration patterns. Different sources of radionuclides penetration into the environment appoint their interaction with nature matrices in different ways and should be considered accordingly. An overview is given of the present radioecological situation around the reprocessing plant "Mayak", which was constructed more than 40 years ago for the production of plutonium for military purposes. Some new approaches, methods and tools developed at the Vernadsky Institute of Geochemistry and Analytical Chemistry for the isolation, concentration and determination of radionuclides in various environmental samples are discussed. Data regarding the distribution, occurrence, and migration processes of radionuciides wSr, 137Cs, MSPu and MlAm, in aquatic and terrestrial ecosystems of the impact zone of the "Mayak" plant, are presented. Key worlds: Radionuclides / Analytical Approaches / Speciation / Waste Disposal INTRODUCTION Ons of big challenges facing contemporary science and technology is problem of environmental protection. It is known that as result of technogenic activity of civilization a large amount of toxicants of both inorganic and organic nature have been discharged and continue entering environment Many of them are ©xtrectjely hazardous to people and living matter, but radioactive contamination of environment represents quite a specific issue and requires special consideration. • ~ Experimental nuclear tests, nuclear power engineering and numerous accidents that took place at the nuclear power plants (NPP), the atomic submarines and some other nuclear installations made artificial radionuclides a constant and unretrievable component of the modern biosphere, becoming an additional unfavorable ecological factor. The clarifying of the penetration sources, the study of the migration dynamics of hazardous radionuclides and the developing of the remediation approaches of the contaminated areas are the most serious ecological, economical and social problems. Solution of these should be based on a wide radioecologicai monitoring, which demands continual routine analysis of water, soil and various biological samples on contents and occurrence forms of radionuclides. As regards Former Soviet Union (FSU) the most unfavourable regions are Southern Ural, zones suffered from Chernobyl Accident, Altay, Novaya Zemlya, some parts of West Siberia near Seversk (Tomsk-7) and Zheleznogorsk (Krasnoyarsk-26). Investigation of main regularities in radionuclides behavior in environment and, in particular, at impact zones of the nuclear fuel cycle facilities is widely recognized as a very actual problem. Lack of data on radionuclides migration in the ground and aquatic ecosystems 13 nukss it difficult to assess and forecast correctly the radiational situation and to work out measures on remediation of contaminated areas. The latter, in turn, are directly related to further development of nuclear energy and safe operation of the corresponding facilities. A lot of data on radionuciides content and distribution in various ecosystems, which entered biosphere both as result of the global radioactive fallout and as accidental radioactive discharges have shown that radionuclides are getting engaged into biogeochemical migration cycles. This process is accompanied by radionuclides redistribution in the ground and aquatic ecosystems and by formation of their entrainment and secondary accumulation zones at the geochemical barriers. Direction, density and mechanisms of migration of radionuclides are greatly affected by their entering forms and forms of occurrence in ecosystems as well as environmental conditions they get into. The present report is devoted to up-to-date radioecological situation around the "Mayak" nuclear facility and description of some new approaches, methods and tools developed at Vernadsky Institute for determination of different radionuclides in the various environmental samples from impact zone of the facility. 1. Moden situation at regions of Russia contaminated by radioactive fallout The influx of artificial radionuclides into the atmosphere began with the first nuclear explosions in 1945, and grew with the ensuing development of the nuclear industry. Table 1 shows estimates of radionuclide emission from various sources (PBq) and radiation doses obtained by the population from these sources (man-Sievert). Chernobyl accident. During the Chernobyl accident of April 26, 1986, «50MCi of radionuclides were released to the environment, which comprised «3.5% of the total amount of radionucldes accumulated in the reactor of the fourth unit(2>3). The fallout of radioactive materials resulted in considerable radioactive pollution of the environment, mainly in the European part of the Former USSR (Table 2). However, the inflow of radionuclides into the biosphere due to the Chernobyl accident accounted for no more than 3% of the amount of radionuclides released to the environment by the tests of nuclear weapons. The Central Black Soil Regions proved to be the most heavily contaminated by the accident. The western regions of the Bryansk oblast received the greatest impact (some of the regions show a contamination of 40 Ci/km2, and the largest territory contaminated with !37Cs is in the Bryansk and Tula oblasts. In the latter 45% of the total area has a level of 137Cs higher than 1.0 Ci/km2. On the whole, in the Russian Federation, a 137Cs pollution of 1.0 Ci/km2 and higher is detected on the total area of 57650 km2, which equals 1.6% of the area of the country. Except for several localities in the Bryansk and Kaluga oblasts, the doses acquired by the population are controlled mainly (>90%) by the natural background and not by the precipitated artificial isotopes. Thus, according to the data of-2'4), the Chernobyl accident did not significantly increase the total radiation impact on the population of European Russia, and it may be assumed that the dose due to nuclear power will not exceed 1% of the natural background by the year 2000. Altay. Population of Altay is excited due to many nuclear explosions at the Semipalatinsk test field. But nowadays average contamination level of Altay is 0.1-0.2 Ci/km 137Cs, 10-50 mCi/km2 90Sr and 5-20 mCi/km2 239Pu. Only two relatively small areas with content 0.2-0.5 Ci/km were determined. Main part of this radiation (80%) is due to the first nuclear explosion in 1949. Western Siberia. Two of Russia radiochemical centers producing weapon plutonium are the Mining and Chemical Plant (MCP), located underground 40 km from Krasnoyarsk, and the Siberian Chemical Plant (SCP), located near Seversk (Tomsk-7), 20 km from Tomsk. There are several dangerous sources of radioactive pollution at these plants. At MCP, these are industrial nuclear reactors cooled with Yenisei River water, a radiochemical factory for the processing of irradiated uranium blocks, and set-ups for the processing and storage of active waste. The Severnyi site for the disposal of liquid MLW is located 60 km from Krasnoyarsk, downstream the Yenisei. Radioactive waste (108 Ci on the whole) is injected 14 there into sand - clay strata. Thus, this factory defines the level of hurnan-induced pollution of the environment in the adjacent territory and the whole Yenisei basin(6>7). Table 1. Estimates of the emission of artificial radionuclides and cumulative effective dose according to the data of UNSCEAR, 19930). Emission, PBq Total effective Source dose, man-Sv 3H 14C Noble 90Sr ml I37Cs local and Global gases regional Nuclear tests in the atmosphere Global 24x104 220 604 65x10* 910 223xlO5 Local Semipalatinsk 4600 Nevada 500b Australia 700 Pacific Ocean 160b Underground nuclear 50 15 200 explosions Production of nuclear weapons Initial tests Hanford 8000a Chelyabinsk 15 000* Later tests 1000 10* Nuclear energy production Mining technology 2700 Reactor operation 140 1.1 3200 0.4 3700 Fuel reprocessing 57 0.3 1200 6.9 0.004 40 4600 Fuel cycle 3x105a 105 Production and use of 2.6 1.0 52 6.0 2000 8xlO4 radioisotopes Accidents Three Mile Island 370 0.0006 40 Chernobyl 630 70 60xl04 Kyshtym 5.4 0.04 2500 Windscaie 1.2 0.7 0.02 2000 Palomares 3 Tule 0 SNAP 9A 2100 Kosmos-954 0.003 0.2 0.003 20 Tundad Juarez 150 Mohammedia 80 Goiania 0.05 60 Total 38xl04 231xlO5 Cumulative effective 235xlO5 dose, man-Sv "»rt /\ /\ ._. _ _ F~~ , m. atmosphere;d after outflow of radionuclides to the Techa River;e total dose due to extraction of 222Rn from waste. The SCP is no less dangerous in terms of possible radioactive emission. It also includes plutonium production, a radiochemical factory, and a factory for isotope separation. 15 Russia's largest field
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