Exploring H2-effects on radiation-induced oxidative dissolution of UO2-based spent nuclear fuel using numerical simulations

Journal article, 2023

Using a recently developed approach for numerical simulation of radiation-induced oxidative dissolution of spent nuclear fuel, we have explored the impact of three possible contributions to the inhibiting effect of molecular hydrogen. The three contributions are (1) effect on oxidant production in irradiated water, (2) reduction of oxidized uranium catalyzed by noble metal inclusions (fission products) and (3) reaction with surface-bound hydroxyl radicals preventing the oxidation of uranium. The simulations show that the first contribution is of fairly small importance while the second contribution can result in complete inhibition of the oxidative dissolution. This is well in line with previous work. Interestingly, the simulations imply that the third contribution, the reaction between H2 and the surface-bound hydroxyl radical formed upon reaction between the radiolysis product H2O2 and UO2, can account for the inhibition observed in systems where noble metal inclusions are not present. This is discussed in view of previously published experimental data.