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The Effect of Alpha-Radiolysis on UO2 Dissolution Determined from Batch Experiments with 238Pu-Doped UO2

Published online by Cambridge University Press:  17 March 2011

Simcha Stroes-Gascoyne
Affiliation:
Atomic Energy of Canada Limited, Whiteshell Laboratories, Pinawa, MB R0E 1L0, Canada, stroess@aecl.ca
James S. Betteridge
Affiliation:
Atomic Energy of Canada Limited, Whiteshell Laboratories, Pinawa, MB R0E 1L0, Canada
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Abstract

Dissolution experiments were performed with 238Pu-doped UO2 containing doping levels of ∼1–100 Ci/kg UO2, in 0.1M perchlorate with or without 0.1M carbonate, at pH 9.5, to investigate the effects of α dose-rate on UO2 dissolution rates and on Geff, the fraction of radiolytically produced H2O2 supporting dissolution. Dissolution rates increased by only about 10 times for a ∼100-fold increase in doping level in both solutions, but increased between 10 and 100 times in 0.1M carbonate, compared to dissolution rates in 0.1M perchlorate. Geff values increased with decreasing doping level, suggesting that the dissolution reaction is limited by the reaction rate between UO2 and H2O2 at high dose rates, but becomes limited by the rate of production of H2O2 at lower dose rates.

Type
Research Article
Copyright
Copyright © Materials Research Society 2004

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