Resolving the H2 effect on radiation induced dissolution of UO2-based spent nuclear fuel

In recent years, the impact of H2 on α-radiation induced dissolution of UO2-based spent nuclear fuel has been studied and debated extensively. Experimental results on the effect of H2 on the concentration of H2O2 during α-radiolysis have been shown to disagree with numerical simulations. For this reason, the reaction scheme used in simulations of aqueous radiation chemistry has sometimes been questioned. s work, we have studied the impact of H2 on the H2O2 concentration in α-irradiated aqueous solution using numerical simulations. The effects of H2 pressure, α-dose rate and HCO 3 - concentration were investigated by performing systematic variations in these parameters. The simulations show that the discrepancy between the previously published experimental result and numerical simulations is due to the use of a homogeneous dose rate (the energy is assumed to be equally distributed in the whole volume). Taking the actual dose rate of the α-irradiated volume into account, the simulation is in perfect agreement with the experimental results. This shows that the H2 effect is strongly α-dose rate dependent, and proves the reliability of the reaction scheme used in the simulations. mulations also show that H2 influences the H2O2 concentration under α-radiolysis. The magnitude of the effect depends on the dose rate and the H2 pressure as well as on the concentration of HCO 3 - . The impact of the radiolytic H2 effect on the rate of α-radiation induced dissolution of spent nuclear fuel is discussed along with other (α- and γ-) radiation induced processes capable of reducing the concentration of uranium in solution. The radiolytic H2 effect is quantitatively compared to the previously presented noble metal catalyzed H2 effect. This comparison shows that the noble metal catalyzed H2 effect is far more efficient than the radiolytic H2 effect. Reduction of U(VI) in solution due to low dose rate γ-radiolysis in the presence of H2 is proposed to be the cause of the H2 effect observed in leaching experiments on α-doped UO2.