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Stability of Mineral Matter in Aqueous Media of the Chernobyl Unit-4 Shelter: Thermodynamic Evaluation

Published online by Cambridge University Press:  03 September 2012

V. A. Sinitsyn ,
D. A. Kulik ,
M. Skhodorivski ,
V. A. Kurepin ,
A. Y. Abramis ,
I. L. Kolyabina  and
N. A. Shurpach
V. A. Sinitsyn
Affiliation:
Institute of Geochemistry, Mineralogy & Ore Formation, NAS Ukraine, 252180 Kyiv, Ukraine R&D Centre “META”, Minchornobyl Ukraine, 255620 Chomobyl, Ukraine
D. A. Kulik
Affiliation:
State Scientific Centre for Environmental Radiogeochemistry, 252180 Kyiv, Ukraine
M. Skhodorivski
Affiliation:
R&D Centre “META”, Minchornobyl Ukraine, 255620 Chomobyl, Ukraine
V. A. Kurepin
Affiliation:
Institute of Geochemistry, Mineralogy & Ore Formation, NAS Ukraine, 252180 Kyiv, Ukraine
A. Y. Abramis
Affiliation:
R&D Centre “META”, Minchornobyl Ukraine, 255620 Chomobyl, Ukraine
I. L. Kolyabina
Affiliation:
R&D Centre “META”, Minchornobyl Ukraine, 255620 Chomobyl, Ukraine
N. A. Shurpach
Affiliation:
Institute of Geochemistry, Mineralogy & Ore Formation, NAS Ukraine, 252180 Kyiv, Ukraine
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Abstract

A special geochemical environment exists within the Shelter (”Sarcophagus”) erected in 1986 over the destroyed Unit-4 of Chernobyl nuclear power plant (NPP). Based upon the available in situ and compositional data, thermodynamic models of solid-aqueous interactions were developed to clarify the leaching behaviour of various materials within the Shelter. The “Selektor-A” code, based on a convex programming approach to Gibbs free energy minimization, was used for the calculations. A built-in flexible hybrid thermodynamic database for the system Na-K-Ca-Mg-Cl-S-N-H-O-Si-P-Fe-Al-Sr-Cs was extended with the critically selected and matched parameters for aqueous species and solid phases in the U-Zr-Si-O-H subsystem, secondary U-minerals, mineral phases of fully hydrated Portland cements and U-bearing zircons. Modeling results show that the “Shelter waters” can selectively leach a significant quantity of U and Si from the fuel-containing masses, while Zr, Fe, Ca, Mg and some other components are rather insoluble. Serpentinite, assemblages of fully-hydrated phases of Portland cements, and oxidation products of steel structural elements are estimated to be sufficiently stable in the aqueous environment of the Shelter. Our calculations also define some feasible pathways for secondary mineral formation from evaporation of Shelter water solutions and interactions between these waters with the mineral matter inside the Shelter.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 465: Symposium II – Scienfific Basis for Nuclear Waste Management XX , 1996 , 1327
Copyright
Copyright © Materials Research Society 1997

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References

REFERENCES

1. Burakov, B., Galkin, E., Pazukhin, E. et al. , Radiochim. Acta 65, 1994.Google Scholar
2. Kiselev, A., Nenaglyadov, A., Surin, A. et al. , Preprint 1AE, 5533/3, Moscow, 1992 (in Russian).Google Scholar
3. Khodorivski, M., Sinitsyn, V., Kulik, D. et al. , NRC4 Conf. Extended Abstracts. (Eds: David, F., Krupa, J.), St. Malo, 1996.Google Scholar
4. Kulik, D., Sinitsyn, V., Khodorivski, M. et al. , NRC4 Conf. Extended Abstracts. (Eds: David, F., Krupa, J.), St. Malo, 1996.Google Scholar
5. Abramis, A., Khodorivski, M., Sinitsyn, V. et al. , in Problems of Chernobyl Exclusion Zone 5, Naukova Dumka Publishers, Kyi v, 1996 (in Russian).Google Scholar
6. Vishnevskii, A., Kuzmina, I., Tkach, V. and Tokarevskii, V., in Problems of Chernobyl Exclusion Zone N 3, Nauková Dumka Publishers, Kyiv, 1996 (in Russian).Google Scholar
7. Karpov, I., Computer-aided physical-chemical modeling in geochemistry (Nauka Publishers, Novosibirsk, 1981) (in Russian).Google Scholar
8. Kulik, D., in Water-Rock Interaction 8, edited by Kharaka, Y. and Chudaev, O. (Balkema, Rotterdam, 1995).Google Scholar
9. Johnson, J., Oelkers, E. and Helgeson, H., Comput. Geosci. 18, 1992.Google Scholar
10. Lemire, R. and Tremaine, P., J. Chem. Eng. Data 25, 1980.Google Scholar
11. Nordstrom, I.D., Plummer, L., Langmuir, D. et al. , in Chemical modeling in aqueous systems II (ACS Symp. Series 416, 1990).Google Scholar
12. Fuger, J., Khodakovsky, I., Sergeyeva, E. et al. , The actinide inorganic complexes, Part 12 (IAEA, Vienna., 1992).Google Scholar
13. Grenthe, I., Fuger, J., Konings, R.J.M. et al. , Chemical thermodynamics of uranium (North-Holland, Amsterdam et al. 1992).Google Scholar
14. Aja, S., Wood, S. and Williams-Jones, A., Applied Geochem., 10, 1995.Google Scholar
15. Vasiliev, V., Kochergina, L. and Lytkin, A., J. Inorg. Chem. (11), 1974 (in Russian)Google Scholar
16. Samchuk, A. and Dorofey, E., Geokhimiya (2), 1983 (in Russian).Google Scholar
17. Sheka, S. and Pevzner, T., J. Inorg. Chem (5), 1960 (in Russian)Google Scholar
18. Robie, R. and Hemingway, B., U.S. Geol. Surv. Bull. 2141, 1995.Google Scholar
19. Melnik, Yu., Genesis of Precambrian Iron Formations (Naukova Dumka Publishers, Kyiv, 1986) (in Russian).Google Scholar
20. Kharaka, Y., Gunter, W., Aggarval, P. et al. , U.S. Geol. Surv. Water-res. Invest. Rep. 88–42, Menlo Park, CA 1988.Google Scholar
21. Ball, J. and Nordstrom, D., U.S. Geol. Surv. Open-File Rep. 91–183, Menlo Park, CA, 1992.Google Scholar
22. Urusov, V., Theory of isomorphous miscibility (Moscow, Nauka Publishers, 1977) (in Russian).Google Scholar
23. Bennett, D., Read, D., Atkins, M., and Glasser, F., Jour. Nucl. Materials, 190, 1992.Google Scholar
24. Lee, J., Roy, D., Mann, B. and Stahl, D., Mat. Res. Soc. Symp. Proc., 353, 1995.Google Scholar
25. Holland, T. and Powell, R.. Metamorphic Geol., 8 (1), 1990.Google Scholar