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For the long-term safety assessment of direct disposal of spent nuclear fuel in deep geologic repositories, knowledge on the radionuclide release rate from the UO2 matrix is essential. This work provides a conceptual model to explain the results of leaching experiments involving used nuclear fuel or simulant materials in confirmed reducing conditions. Key elements of this model are: direct effect of radiation from radiolytic species (including defects and excited states) in the solid and in the first water layers in contact with its surface; and excess H2 may be produced due to processes occurring at the surface of the spent fuel and in confined water volumes, which may also play a role in keeping the spent fuel surface in a reduced state. The implication is that the fractional radionuclide release rate used in most long-term safety assessments (10−7 year−1) is over estimated because it assumes that there is net UO2 oxidation caused by radiolysis, in contrast with the alternative conceptual model presented here. Furthermore, conventional water radiolysis models and radiation chemical yields published in the literature are not directly applicable to a heterogeneous system such as the spent fuel–water interface. Suggestions are provided for future work to develop more reliable models for the long-term safety assessment of spent nuclear fuel disposal.

An Alternative Conceptual Model for the Spent Nuclear Fuel–Water Interaction in Deep Geologic Disposal Conditions