Studies on Spent Fuel Alterations During Storage and Radiolysis Effects on Corrosion Behaviour Using Alpha-Doped UO₂

UO₂ containing different fractions of short-lived alpha-emitters, the so-called alpha-doped UO₂ simulates the level of activity of spent fuel after different storage times, and can be used to study the effects of radiolysis on the corrosion behaviour of aged spent fuel exposed to groundwater in a geologic repository. Furthermore, the integral over time of the alpha-decay in alpha-doped UO₂ can simulate the decay damage accumulated in spent fuel during storage. This allows investigating property modifications occurring to the fuel during storage periods of interest (e.g. in view of spent fuel retrieval or in view of final disposal) within a laboratory-acceptable timescale. Periodical measurements of lattice parameter are performed on high activity alpha-doped UO₂ to investigate the build-up of radiation damage and evaluate possible dose rate effects. Additionally, annealing tests combined with He-release measurements using a Knudsen cell and with microstructure examination using TEM are performed to establish a correlation among the annealing of damage in the microstructure (mainly characterized by dislocation loops) and the release behaviour of He. The effects on the microstructure due to the accumulation of He and α-decay damage are of interest as they may considerably affect the mechanical integrity of the fuel rods, by causing e.g. swelling or cracking in the fuel and/or overpressurization of the cladding. Alpha-doped UO₂ with specific activities spanning over three orders of magnitude and undoped UO₂ were used in static leaching experiments at room temperature in deionized water under nominally anoxic conditions. Under these experimental conditions (single effect studies) a clear dissolution enhancing effect of alpha-radiolysis was observed coupled with the establishment of higher redox potential due to the radiolytic process. An alpha-activity dependence of the dissolution behaviour was observed.