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The Oxidative Dissolution Mechanism of Uranium Dioxide. The Effect of pH and Oxygen Partial Pressure

Published online by Cambridge University Press:  01 February 2011

Joan de Pablo
Affiliation:
Department of Chemical Engineering, Universitat Politècnica de Catalunya, ETSEIB, Diagonal, 647 H-4, 08028, Barcelona, Spain.
Ignasi Casas
Affiliation:
Department of Chemical Engineering, Universitat Politècnica de Catalunya, ETSEIB, Diagonal, 647 H-4, 08028, Barcelona, Spain.
Javier Giménez
Affiliation:
Department of Chemical Engineering, Universitat Politècnica de Catalunya, ETSEIB, Diagonal, 647 H-4, 08028, Barcelona, Spain.
Frederic Clarens
Affiliation:
Department of Chemical Engineering, Universitat Politècnica de Catalunya, ETSEIB, Diagonal, 647 H-4, 08028, Barcelona, Spain.
Lara Duro
Affiliation:
ENVIROS Spain, Avda. Rubí 29–31, 08197 Valldoreix, Spain.
Jordi Bruno
Affiliation:
ENVIROS Spain, Avda. Rubí 29–31, 08197 Valldoreix, Spain.
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Abstract

The dissolution of the unirradiated uranium dioxide, UO2, is largely affected by chemical variables like pe, pH and carbonate concentration in solution. In a previous paper [1], we studied the kinetics of the dissolution of UO2 as a function of pH and oxygen partial pressure and the experimental dissolution rates obtained showed a fractional dependence on both parameters. These fractional orders indicate a dissolution occurring via a surface mediated mechanism.

In this work we have developed a mechanism accounting for the oxidative dissolution of UO2, which depends on the oxygen concentration in solution and on the pH and a general rate equation has been deduced. This mechanism has been used to explain the results obtained by different authors and to explain and predict the dissolution of the spent nuclear fuel matrix.

Type
Research Article
Copyright
Copyright © Materials Research Society 2004

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References

1. Torrero, M.E.; Baraj, E.; de Pablo, J.; Giménez, J. and Casas, I. (1997), Kinetics of corrosion and dissolution of uranium dioxide as a function of pH. Int. J. Chem. Kinet. 29, 261267.3.0.CO;2-S>CrossRefGoogle Scholar
2. Casas, I.; Giménez, J.; Martí, V.; Torrero, M.E. and de Pablo, J. (1994) Kinetic studies of unirradiated UO2 dissolution under oxidizing conditions in batch and flow experiments. Radiochim. Acta 66/67, 2327.Google Scholar
3. Grambow, B. (1989) Spent fuel dissolution and oxidation. An evaluation of literature data. SKB Technical Report 89–13.Google Scholar
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5. Eriksen, T.E.; Eklund, U.-B.; Werme, L.O. and Bruno, J. (1995) Dissolution of irradiated fuel: a radiolytic mass balance study. J. Nucí. Mater. 227, 7682 (1995).CrossRefGoogle Scholar
6. Shoesmith, D.W. and Sunder, S. (1991) An electrochemistry-based model for the dissolution of UO2. Atomic Energy of Canada Limited Report, AECL-10488.Google Scholar
7. Thomas, G.F. and Till, G. (1984), Nucí. Chem. Waste Manag. 5, 141147.Google Scholar
8. Casas, I.; Giménez, J.; de Pablo, J. and Torrero, M.E. (1993) Dissolution of UO2(s) in MgCl2-brines under different redox conditions. Mater. Res. Soc. Symp. Proc. 294, 6772.CrossRefGoogle Scholar
9. Bruno, J.; Casas, I.; Cera, E.; de Pablo, J.; Giménez, J. and Torrero, M.E. (1995) Uranium (IV) dioxide and SIMFUEL as a chemical analogues of nuclear spent fuel matrix dissolution. Mater. Res. Soc. Symp. Proc. 353, 601608.Google Scholar
10. Davis, J.A. and Kent, D.B. (1990) Surface complexation modelling in aqueous geochemistry. In Review in Mineralogy: Mineral Water Interface Geochemistry (eds. Hochella, M.F. Jr And White, A.F.), Vol. 23 Chapter 5, pp. 177260. The Mineralogical Society of America.CrossRefGoogle Scholar
11. de Pablo, J., Casas, I., Giménez, J., Molera, M., Rovira, M., Duro, L. and Bruno, J. (1999) Geochim. Et Cosmochim. Acta 63, 3097.Google Scholar
12. Bruno, J.; Cera, E.; Duro, L.; Pon, J., de Pablo, J. and Eriksen, T. (1998) Development of a kinetic model for the dissolution of the UO2 spent nuclear fuel. SKB Technical Report TR-98–22.Google Scholar
13. Oversby, V. (1999) Uranium dioxide, SIMFUEL, and spent fuel dissolution rates. A review of published data. SKB Technical Report TR-99–22.Google Scholar
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