Effect of Alpha Radiolysis on UO2Dissolution under Reducing Conditions

Abstract

ABSTRACTEffects of water radiolysis on the dissolution rate of UO2were studied by irradiating UO2colloids 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 1.1×1011α.cm−2.s−1entering 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−1depending on the ratio of the irradiated UO2mass to the solution volume. This dependency is caused by hydrogen peroxide consumption at the UO2surface. The rate of hydrogen peroxide consumption by reaction with colloids corresponds to an equivalent rate of UO2oxidation/dissolution between 2 and 60 mg.m−2.d−1indicating that only a small fraction of produced H2O2is consumed by the dissolution reaction.