Hostname: page-component-5c6d5d7d68-sv6ng Total loading time: 0 Render date: 2024-08-09T07:27:05.219Z Has data issue: false hasContentIssue false
  • English
  • Français

Prediction of the Oxidative Dissolution Rates of Used Nuclear Fuel in a Geological Disposal Vault Due to the Alpha Radiolysis of Water

Published online by Cambridge University Press:  15 February 2011

S. Sunder ,
D.W. Shoesmith  and
N.H. Miller
S. Sunder
Affiliation:
AECL Research, Whiteshell Laboratories, Pinawa, Manitoba, CanadaROE 1L0
Get access

Abstract

Effects of alpha radiolysis of water on the corrosion of nuclear fuel (UO2) have been investigated in solutions at pH = 9.5, i.e., a value close to that expected in groundwaters at the depth of the disposal vault proposed in the Canadian nuclear fuel waste management program, CNFWMP. The corrosion potentials of UO2 electrodes exposed to the products of alpha radiolysis of water were monitored as a function of alpha flux and exposure time in a specially designed thin-layer cell. The oxidative dissolution rates of UO2 are calculated from the steady-state values of the corrosion potential using an electrochemical model. A procedure to predict the dissolution rate of used nuclear fuel in groundwater as a function of fuel cooling time is described, and illustrated by calculating the dissolution rates for the reference used fuel in the CNFWMP (Bruce CANDU reactor fuel, burnup 685 GJ/kg U). It is shown that the oxidative dissolution of used fuel in the CNFWMP will be important only for time periods ≤ 600 a at this burnup and assuming no decrease in pH.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 353: Symposium – Scientific Basis for Nuclear Waste Management XVIII , 1994 , 617
Copyright
Copyright © Materials Research Society 1995

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Forsyth, R.S. and Werme, L.O., J. Nucl. Mater. 190, 3 (1992).Google Scholar
2. Gray, W.J., Leider, H.R. and Steward, S.A.. J. Nucl. Mater. 190, 46 (1992).Google Scholar
3. Johnson, L.H. and Shoesmith, D.W., in Radioactive Waste Forms for the Future. Edited by Lutze, W. and Ewing, R.C. (Elsevier, Amsterdam, 1988) p. 635.Google Scholar
4. Sunder, S. and Shoesmith, D.W., Chemistry of UO2 Fuel Dissolution in Relation to the Disposal of Used Nuclear Fuel, Atomic Energy of Canada Limited Report, AECL-10395 (1991).Google Scholar
5. Shoesmith, D.W. and Sunder, S., An Electrochemistry-based Model for the Dissolution of UO2 , SKB Technical Report, 91–63 (1991).Google Scholar
6. Shoesmith, D.W. and Sunder, S., J. Nucl. Mater. 190, 20 (1992).Google Scholar
7. Shoesmith, D.W., Sunder, S.. and Hocking, W.H., in Electrochemistry of Novel Materials, edited by Lipkowski, J. and Ross, P.N. (VCH Publishers, Inc. New York, 1994) pp 297–337.Google Scholar
8. Gascoyne, M. and Kamineni, D.C., Groundwater Chemistry and Fracture Mineralogy in the Whiteshell Research Area: Supporting Data for the Geosphere and Biosphere Transport Models, Technical Record, Whiteshell Laboratories, TR-516*, Atomic Energy of Canada Limited (1992).Google Scholar
9. Bailey, M.G., Johnson, L.H. and Shoesmith, D.W., Corros. Sci. 25, 233 (1985).Google Scholar
10. Sunder, S., Shoesmith, D.W., Christensen, H., Bailey, M.G. and Miller, N.H., Mater. Res. Soc. Symp. Proc. 127, 317 (1989).Google Scholar
11. Sunder, S., Boyer, G.D. and Miller, N.H., J. Nucl. Mater. 175, 163 (1990).Google Scholar
12. Sunder, S., Shoesmith, D.W., Christensen, H. and Miller, N.H., J. Nucl. Mater. 190, 78 (1992) .Google Scholar
13. Smith, H.J., Tait, J.C. and von, R.E. Massow, Radioactive Decay Properties of Bruce “A” CANDUTM UO2 Fuel and Recycle Waste, Atomic Energy of Canada Limited Report, AECL-9072 (1987).Google Scholar
14. Sunder, S., Shoesmith, D.W., Miller, N.H. and Wallace, G.J., Mater. Res. Soc. Symp. Proc. 257, 345 (1992).Google Scholar
15. Sunder, S., Shoesmith, D.W., Bailey, M.G., Stanchell, F.W. and Mclntyre, N.S., J. Electroanal. Chem. 130, 163 (1981).Google Scholar
16. Allen, A.O., The Radiation Chemistry of Water and Aqueous Solutions (Van Nostrand, Princeton, New Jersey, 1961).Google Scholar
17. Christensen, H. and Sunder, S., Evaluation of Data from Calculations of Gamma-Radiolysis of Aqueous Solutions for UO2 Oxidation Studies. Studsvik Report, Studsvilc/M-93/29 (1993).Google Scholar
18. Rudnicki, J.D., Russo, R. and Shoesmith, D.W., J. Electroanal. Chem. 372, 63 (1994).Google Scholar
19. Lemire, R.J. and Garisto, F., The solubility of U, Nb, Pu, Th and Tc in a geological disposal vault for used nuclear fuel, Atomic Energy of Canada Limited Report, AECL-10009 (1989).Google Scholar
20. Sunder, S., Shoesmith, D.W. and Miller, N.H. (unpublished work).Google Scholar
21. Lahalle, M.P., Krupa, J.C., Guillaumont, R., Genet, M., Allen, G.C., and Holmes, N., Mater. Res. Soc. Symp. Proc. 127, 351 (1989).Google Scholar
22. Wronkiewicz, D.J., Bates, J.K., Gerding, T.J., Veleckis, E. and Tani, B.S., J. Nucl. Mater. 190, 107 (1992).Google Scholar
23. Hocking, W.H., Shoesmith, D.W. and Betteridge, J.S., J. Nucl. Mater. 190, 36 (1992).Google Scholar
24. Shoesmith, D.W., Sunder, S., Bailey, M.G. and Miller, N.H., Elctrochemical and SEM Studies of Corrosion of Used Nuclear Fuel in Aqueous Perchlorate and Carbonate Solutions. J. Nucl. Mater, (to be published).Google Scholar