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Release of Radiotoxic Elements from High Burn-Up UO2 and MOX Fuel in a Repository

Published online by Cambridge University Press:  21 March 2011

Jean-Paul Glatz
Affiliation:
European Commission, Directorate-General JRC, Institute for Transuranium Elements, Karlsruhe, GERMANY
Paul Carbol
Affiliation:
European Commission, Directorate-General JRC, Institute for Transuranium Elements, Karlsruhe, GERMANY
Joaquin Cobos-Sabaté
Affiliation:
CIEMAT, Av.da Complutense 22, E-28040 Madrid, SPAIN
Thomas Gouder
Affiliation:
European Commission, Directorate-General JRC, Institute for Transuranium Elements, Karlsruhe, GERMANY
Frédéric Miserque
Affiliation:
European Commission, Directorate-General JRC, Institute for Transuranium Elements, Karlsruhe, GERMANY
Javier Gimenez
Affiliation:
European Commission, Directorate-General JRC, Institute for Transuranium Elements, Karlsruhe, GERMANY
Detlef Wegen
Affiliation:
European Commission, Directorate-General JRC, Institute for Transuranium Elements, Karlsruhe, GERMANY
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Abstract

In a spent fuel repository the processes that govern the release of radionuclides are dissolution and transport in a possible groundwater flow. The cladding will be the last barrier before the water comes into contact with the fuel, namely with the outer rim of the pellet. Here the heterogeneity of the material due to the irradiation process is responsible for a complex release process. Fission products and minor actinides inventories are considerably higher at the pellet periphery as a result of increased epithermal neutron capture and of migration in the case of the volatile fission products.

The present paper gives a review of experimental activities at the Institute for Transuranium Elements (ITU). Both single effects studies and integral tests are carried out to study the behavior of spent fuel under storage conditions.

Leaching of irradiated UO2 (up to 50 GWd/tU) and MOX (up to 25 GWd/tU) fuel rods with preset cladding defects at 100°C under anoxic or reducing conditions should simulate the realistic case of groundwater coming into contact with a spent nuclear fuel repository. For all main radionuclides the release process can be described considering a two-step dissolution mechanism that includes the initial dissolution of an oxidized layer present on the fuel surface followed by a long-term oxidative matrix dissolution. By means of α-doped (238Pu) UO2 it could be demonstrated, that radiolysis has a significant influence on this dissolution. Especially high initial release rates were found for the volatile cesium and iodine for the reasons mentioned above.

Besides the conventional leaching experiments electrochemical techniques are used to investigate for instance the complex corrosion behavior of the heterogeneous MOX fuel materials or the influence of α-radiolysis on spent fuel dissolution.

In the integral tests mentioned above with large S/V values, reprecipitation of U is likely to happen. Therefore special dynamic test are conducted where this reprecipitation is prohibited and true U solubility can be determined.

Thin layer of UO2 and (U,Pu)O2 doped with various fission products and minor actinides are prepared to study the influence of these elements on the matrix dissolution. When Cs is for instance co-deposited, the U oxidation state changes from U4+ to U6+ for the same O2 pressure possibly indicating a stable Cs uranate. This could be an indirect proof of the existence of such a species in irradiated fuel (e.g. at the grain boundaries).

Type
Research Article
Copyright
Copyright © Materials Research Society 2001

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References

1. Gray, W.J. and Strachan, D.M., Mater. Res. Soc. Symp. Proc. 212 (1991) 205212 CrossRefGoogle Scholar
2. Forsyth, R. S., Werme, L. O. and Bruno, J., J. Nucl. Mater. 138 115 (1986).CrossRefGoogle Scholar
3. Giménez, J., Pablo, J. de, Torrero, M.E. and Casas, I., Radiochim. Acta 78 2125 (1997)CrossRefGoogle Scholar
4.Marc Lippens Yvon Vanderborck MOX Fuel Performance BELGONUCLEAIRE Views: Today and Tomorrow, Proc. GLOBAL '99, August 29 - September 3, 1999 Jackson Hole, WyomingGoogle Scholar
5. , Puigdomènech, Casas, I. and Bruno, J., “Kinetics of UO2(s) Dissolution under Reducing Conditions: Numerical Modelling”, SKB Technical Report 90-25, SKB (1990)Google Scholar
6. Fischer, U., Wiese, H.W., KfK report 3014 (1983)Google Scholar
7. Serrano, J.A., Glatz, J.-P., Toscano, E.H., Papaioannou, D., Barrero, J. and Coquerelle, M., J. Alloys Comp. 271–273 (1998) 573576 CrossRefGoogle Scholar
8. Walker, C.T., Goll, W. and Matsumura, T., J. Nucl. Mater. 228 (1996) 817 CrossRefGoogle Scholar
9. Spino, J., Vennix, K. and Coquerelle, M., J. Nucl. Mater. 231 (1996) 179190 CrossRefGoogle Scholar
10. WILSON, C.N. and OVERSBY, V.M., “Radionuclide Release from PWR Fuels in a Reference Tuff Repository Groundwater”, Mat.Res.Soc.Symp.Proc., 294 (1985) 497 Google Scholar
11. Stroes-Gascoyne, S., Johnson, L.H., Tait, J.C. and Sellinger, D.M., Mater. Res. Soc. Symp. Proc. 127 (1989) 301307 CrossRefGoogle Scholar
12. Shoesmith, D. W., Sunder, S., AECL Report 10488, Pinawa, Canada (1991)Google Scholar
13. Sunder, S., Shoesmith, D.W., Lemire, R.J., Bailey, M.G., Wallace, G.J., Corrosion science, 32 (1991) 373386 CrossRefGoogle Scholar
14. Berghe, S.Van Den, Laval, J.-P., Gaudreau, B., Terryn, H., Verwerft, M., J.Nucl. Mater. 277 (2000) 2836 CrossRefGoogle Scholar
15. Christensen, H., Sunder, S. and Shoesmith, D.W., J. Alloys Comp. 213/214 (1994) 93 CrossRefGoogle Scholar
16. Sunder, S., Shoesmith, D.W., Christensen, H., Miller, N.H., J. Nucl. Mat. 190 (1992) 78 CrossRefGoogle Scholar
17. Rondinella, V.V., Matzke, Hj., Cobos, J. and Wiss, T., Mater. Res. Soc. Symp. Proc. 556 (1999) 447454 CrossRefGoogle Scholar
18. Grambow, B. et al., EUR 19140 (2000)Google Scholar
19. Rimstidt, J. D., Dove, P. M.. Geochim. Et Cosmochim. Acta 50 25092516 (1986)CrossRefGoogle Scholar
20. Bruno, J., Casas, I., Cera, E., Pablo, J. de, Giménez, J. and Torrero, M. E., Mater. Res. Soc. Symp. Proc. 553 (1995) 601608.Google Scholar

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