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Modeling of UO2 Aqueous Dissolution Over a Wide Range of Conditions

Published online by Cambridge University Press:  25 February 2011

Steven A. Steward
Affiliation:
Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94550
Homer C. Weed
Affiliation:
Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94550
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Abstract

Previously it was not possible to predict reliably the rate at which spent fuel would react with groundwater because of conflicting data in the literature. The dissolution of the UO2 spent fuel matrix is a necessary step for aqueous release of radioactive fission products. Statistical experimental design was used to plan a set of UO2 dissolution experiments to examine systematically the effects of temperature (25-75°C), dissolved oxygen (0.002-0.2 atm overpressure), pH (8-10) and carbonate (2-200x10-4 molar) concentrations on UO2 dissolution. The average dissolution rate was 4.3 mg/m2/day. The regression fit of the data indicate an Arrhenius type activation energy of -8750 cal/mol·K and a half-power dependence on dissolved oxygen in the simulated groundwater.

Type
Research Article
Copyright
Copyright © Materials Research Society 1994

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References

REFERENCES

1 Grambow, B., “Spent Fuel Dissolution and Oxidation. An Evaluation of Literature Data,” SKB Technical Report 89-13 (1989).Google Scholar
2 McKenzie, W. F., “UO2 Dissolution Rates: A Review,” Lawrence Livermore National Laboratory Report UCRL-III-111663 (September 1992).Google Scholar
3 Nguyen, S.N., Weed, H.C., Leider, H.R., and Stout, R. B., “Dissolution Kinetics of UO2. I. Row-Through Tests on UO2.00 Pellets and Polycrystalline Schoepite Samples in Oxygenated, Carbonate/Bicarbonate Buffer Solutions at 25ºC,” Mat. Res. Soc., Strasbourg, France, Nov. 4–7, 1991, Lawrence Livermore National Laboratory Report UCRL-JC-107478 (October 1991).CrossRefGoogle Scholar
4 Knauss, K.G. and Wolery, T.J., Geochim. Cosmochim. Acta 53 (1989) 1493.CrossRefGoogle Scholar
5 Knauss, K.G., Bourcier, W.L., McKeegan, K.D., Merabacher, C.I., Nguyen, S.N., Ryerson, F.J., Smith, D.K., Weed, H.C. and Newton, L., “Dissolution Kinetics of a Simple Analogue Nuclear Waste Glass as a Function of pH, Time and Temperature,” MRS Symposium Proceedings, 176 (1990) 371.Google Scholar
6 Lasaga, A.D., in Kinetics of Geochemical Processes, eds., Lasaga, A.D. and Kirkpatrick, R.J., (Mineral Soc. Amer., Reviews in Mineralogy, 8 (1981) 1.CrossRefGoogle Scholar
7 BBN Software Products Corporation, RS/Discover, Version 2 (1989).Google Scholar
8 Stumm, W. and Morgan, J., Aquatic Chemistry: An Introduction Emphasizing Chemical Equilibria In Natural Waters, John Wiley and Sons, New York (1981), Chapter 2.14.Google Scholar
9 Gray, W.J., Leider, H.R. and Steward, S.A., J. Nucl. Mater. 190 (1992) 46.CrossRefGoogle Scholar