New insight on the simultaneous H2 and HNO2 production in concentrated HNO3 aqueous solutions under alpha radiation

Abstract

Knowledge of hydrogen and nitrous acid yields (G(H₂) and G(HNO₂)) from α radiolysis of nitric acid solutions is of critical importance for the technological aspects of reprocessing of spent nuclear fuel (SNF). This study provides critical information on the G values for external alpha irradiation of concentrated HNO₃ solutions. An investigation-specifically developed experimental setup allows performing this investigation without encountering issues related to extreme high local doses. In situ monitoring of the UV-visible induced absorption in irradiated HNO₃ solutions permitted quantification of HNO₂ production, and mass spectrometry was used to quantify H₂. The influence of the dose rate and HNO₃ concentration was investigated, and the primary yields of these two species were determined. It was found that dose rate increase leads to diminished production of HNO₂ and H₂, while HNO₃ concentration increase leads to increased HNO₂ formation and reduced H₂ production. The values of the primary yields of these two species were determined and compared to the literature reported values. While the determined values show similar trends as those reported, this study provides accurate radiolytic yields for H₂ and HNO₂ that are radioelement-independent compared to the α radiolysis using radioisotope/HNO₃ mixtures and provides the basis for perfecting numerical codes used for simulating the radiolytic processes associated with SNF reprocessing.