On the effects of fission product noble metal inclusions on the kinetics of radiation induced dissolution of spent nuclear fuel

摘要

Radiation induced oxidative dissolution of UO2 is a key process for the safety assessment of future geological repositories for spent nuclear fuel. This process is expected to govern the rate of radionuclide release to the biosphere. In this work, we have studied the catalytic effects of fission product noble metal inclusions on the kinetics of radiation induced dissolution of spent nuclear fuel. The experimental studies were performed using UO2 pellets containing 0%, 0.1%, 1% and 3% Pd as a model for spent nuclear fuel. H2O2 was used as a model for radiolytical oxidants (previous studies have shown that H2O2 is the most important oxidant in such systems). The pellets were immersed in aqueous solution containing H2O2 and HCO3- and the consumption of H2O2 and the dissolution of uranium were analyzed as a function of H-2 pressure (0-40 bar). The noble metal inclusions were found to catalyze oxidation Of UO2 as Well as reduction of surface bound oxidized UO2 by H-2. In both cases the rate of the process increases with increasing Pd content. The reduction process was found to be close to diffusion controlled. This process can fully account for the inhibiting effect of H-2 observed in several studies on spent nuclear fuel dissolution. (c) 2008 Elsevier B.V. All rights reserved.