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Effect of Alpha Radiolysis on UO2 Dissolution under Reducing Conditions
Published online by Cambridge University Press: 01 February 2011
Abstract
Effects of water radiolysis on the dissolution rate of UO2 were studied by irradiating UO2 colloids with an alpha particle beam of a cyclotron. The solution was kept under reducing conditions by applying a current of -10 or -50 nA and an ultrahigh purity argon bubbling. The solution pH was fixed at 6 during experiment. The particle flux was 1.1×1011 α.cm−2.s−1 entering in solution with an energy of 5 – 6 MeV. Despite initial reducing conditions water radiolysis increased the dissolution rate of uranium dioxide due to reaction with oxidizing radiolytic species such as H2O2, O2, OH•, HO2•, ClO3−. The monitoring of the redox potential showed that the solutions became rapidly oxidizing. The dissolution rate values were between 0.01 and 26 mg·m−2·d−1 depending on the ratio of the irradiated UO2 mass to the solution volume. This dependency is caused by hydrogen peroxide consumption at the UO2 surface. The rate of hydrogen peroxide consumption by reaction with colloids corresponds to an equivalent rate of UO2 oxidation/dissolution between 2 and 60 mg.m−2.d−1 indicating that only a small fraction of produced H2O2 is consumed by the dissolution reaction.
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- Copyright © Materials Research Society 2004
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