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UO 2 fuel corrosion / Radionuclide release / Instant release fraction / Hydrogen effect / Coprecipitation / SorptionSummary. Even though chemical processes related to the corrosion of spent nuclear fuel in a deep geological repository are of complex nature, knowledge on underlying mechanisms has very much improved over the last years. As a major result of numerous studies it turns out that alteration of irradiated fuel is significantly inhibited under the strongly reducing conditions induced by container corrosion and consecutive H 2 production. In contrast to earlier results, radiolysis driven fuel corrosion and oxidative dissolution appears to be less relevant for most repository concepts. The protective hydrogen effect on corrosion of irradiated fuel has been evidenced in many experiments. Still, open questions remain related to the exact mechanism and the impact of potentially interfering naturally occurring groundwater trace components. Container corrosion products are known to offer considerable reactive surface area in addition to engineered buffer and backfill material. In combination, waste form, container corrosion products and backfill material represent strong barriers for radionuclide retention and retardation and thus attenuate radionuclide release from the repository near-field.

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Dissolution of spent fuel has been studied in saline, anaerobe, carbonate free solutions. Processes controlling spent fuel dissolution and associated radionuclide release are radiolytically controlled oxidative dissolution, sorption on container, solubility and coprecipitation. Upper limits for oxidative dissolution rates are given by the production rates of oxidative radiolysis products. This limitation leads to a strong decrease in surface area normalized reaction rates with increasing surface to volume ratio (S/V) and imposes geometric constraints on prediction of spent fuel behavior in a repository. Solution concentrations of Am during spent fuel corrosion were about 5 orders of magnitude lower than the solubility of Am(OH)3(s) and are likely controlled by coprecipitation. Pu concentrations may be controlled by Pu(VI) or Pu(IV) (hydr)oxides.