Can redox sensitive radionuclides be immobilized on the surface of spent nuclear fuel? - A model study on the reduction of Se(IV)(aq) on Pd-doped UO2 under H-2 atmosphere

摘要

Spent nuclear fuel contains noble metal particles composed of fission products (Pd, Mo, Ru, Tc, Rh and Te, often referred to as epsilon-particles). Studies have shown that these particles play a major role in catalyzing oxidative dissolution as well as H-2 reduction of the oxidized UO2 fuel matrix, depending on the conditions. Thus it is possible that these particles also could have a major impact on the state of other redox sensitive radionuclides (such as the long lived fission product Se-79) present in spent nuclear fuel. In this study, Pd-doped UO2 pellets are used to simulate noble metal particles inclusions in spent nuclear fuel and the effect on dissolved selenium in the form of selenite (250 mu M selenite) in simulated ground water solution (10 mM NaCl, 10 mM NaHCO3) at 1 and 10 bar hydrogen pressure. The selenite was found to be reduced to elemental Se, forming colloidal particles. At hydrogen pressures of 10 bar, the rate of selenite reduction was found to be linearly correlated to the fraction of Pd in the UO2 pellets. No selenium was detected on the surface of the pellets. For the lowest Pd loading (0.1% Pd) the selenite reduction does not appear to proceed to completion indicating that the surface becomes less active.