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Dissolution of UO2 by One- and Two-Electron Oxidants

Published online by Cambridge University Press:  01 February 2011

Mats Jonsson ,
Ella Ekeroth  and
Olivia Roth
Mats Jonsson
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
Ella Ekeroth
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
Olivia Roth
Affiliation:
Department of Chemistry, Nuclear Chemistry, Royal Institute of Technology, SE-100 44 Stockholm, Sweden
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Abstract

In this work, the efficiency of one- and two-electron oxidants in oxidative dissolution of UO2 has been investigated. This was accomplished by measuring the U(VI)-concentration in solution after exposing UO2-powder to controlled amounts of oxidants in aqueous solution. The oxidants used in this study are H2O2, IrCl62−, CO3• and OH•. H2O2 acts as a two-electron oxidant while the remaining three oxidants are one-electron oxidants. CO3 and OH• were generated using γ-radiolysis. The results clearly show that the dissolution yields for one-electron oxidants (per electron pair) are lower than the yields for two-electron oxidants. Furthermore, the yields for one-electron oxidants increase with increasing amount of oxidant (especially at low amounts of oxidant). The rationale for this is that U(VI) is the main soluble species which is formed directly upon two-electron oxidation. For one-electron oxidants the primary oxidation product is U(V) which can form U(VI) upon reaction with a second oxidant. The probability for a second oxidation is however low at low concentrations of oxidant.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 807: Symposium Scientific Basis for Nuclear Waste Management XXVII , 2003 , 77
Copyright
Copyright © Materials Research Society 2004

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References

REFERENCES

1. Segall, R. L., Smart, R. S. C., and Turner, P. S., in “Surface and Near-Surface Chemistry of Oxide Materials” (Nowotny, J. and Dufour, L.-C., eds.), Vol. 47, p. 527–576. Elsevier Science Publishers B. V., Amsterdam, 1988.Google Scholar
2. Spinks, J. W. T. and Woods, R. J., “An Introduction to Radiation Chemistry.” John Wiley & Sons, Inc, New York, 1964.Google Scholar
3. Shoesmith, D. W., J. Nucl. Mater. 282, 1–31 (2000).Google Scholar
4. Eriksen, T. E., Eklund, U.-B., Werme, L., and Bruno, J., J. Nucl. Mater. 227, 76–82 (1995).Google Scholar
5. Bruno, J., Cera, E., Grivé, M., Eklund, U.-B., and Eriksen, T. E., SKB TR-99–26, 1–55 (1999).Google Scholar
6. Bruno, J., Cera, E., Grivé, M., Duro, L., and Eriksen, T. E., SKB TR-03–03, 1–52 (2003).Google Scholar
7. Glatz, J.-P., Carbol, P., Cobos-Sabaté, J., Gouder, T., Miserque, F., Gimenez, J., and Wegen, D., Mater. Res. Soc. Symp. Proc. 663, 449–458 (2001).Google Scholar
8. Ekeroth, E. and Jonsson, M., J. Nucl. Mater., in press (2003).Google Scholar
9. Robbins, J. C., CIM Bulletin 71, 61–67 (1978).Google Scholar
10. Nicol, M. J. and Needes, C. R. S., Electrochimica Acta 20, 585 (1974).Google Scholar