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.
In accordance with the Belgian “supercontainer design”, spent nuclear fuel (SNF) will be encapsulated in carbon steel canisters, surrounded by a concrete overpack for disposal in poorly-indurated clay. After re-saturation of the barriers by porewater, interactions with the concrete will result in solutions rich in NaOH, KOH and Ca(OH)2. Corrosion studies of SNF in ECW-type solution (Evolved Cement Water) and YCWCa-type solution (Young Cement Water with Ca) were performed under externally applied H2 overpressures over 426 days. Directly after H2 application, Tc concentrations decreased from >10-8 M to concentrations below detection limit. Based on the fractional release of selected fission products, low matrix dissolution rates of ~10-8/day were found in both experiments. U concentrations decreased finally to 1.5•10-9 M (YCWCa) and to 2.1•10-10 M (ECW), respectively. Am, Np and Pu concentrations were found throughout the experiments below their detection limits indicating an effective retention process.
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