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Modeling of oxygen gas diffusion and consumption during the oxic transient in a disposal cell of radioactive waste

Abstract : The oxic transient in geological radioactive waste disposals is a key issue for the performance of metallic components that may undergo high corrosion rates under such conditions. A previous study carried out in situ in the argillite formation of Tournemire (France) has suggested that oxic conditions could have lasted several years. In this study, a multiphase reactive transport model is performed with the code HYTEC to analyze the balance between the kinetics of pyrite oxidative dissolution, the kinetics of carbon steel corrosion and oxygen gas diffusion when carbon steel components are emplaced in the geological medium. Two cases were modeled: firstly, the observations made in situ have been reproduced, and the model established was then applied to a disposal cell for high-level waste (HLW) in an argillaceous formation, taking into account carbon steel components and excavated damaged zones (EDZ). In a closed system, modeling leads to a complete and fast consumption of oxygen in both cases. Modeling results are more consistent with the in situ test while considering residual voids between materials and/or a water unsaturated state allowing for oxygen gas diffusion (open conditions). Under similar open conditions and considering ventilation of the handling drifts, a redox contrast occurs between reducing conditions at the back of the disposal cell (with anoxic corrosion of steel and H2 production) and oxidizing conditions at the front of the cell (with oxic corrosion of steel). The extent of the oxidizing/reducing front in the disposal cell is strongly dependent on the gas diffusion coefficient in partially saturated zones.
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Laurent de Windt, François Marsal, Jérôme Corvisier, Delphine Pellegrini. Modeling of oxygen gas diffusion and consumption during the oxic transient in a disposal cell of radioactive waste. Applied Geochemistry, Elsevier, 2014, 41, pp.115-127. ⟨10.1016/j.apgeochem.2013.12.005⟩. ⟨hal-00936851⟩

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