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The Role of surface-bound hydroxyl radicals in the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$

Fidalgo, A. B.*; Kumagai, Yuta; Jonsson, M.*

In this work, we have studied the reaction between H$$_{2}$$O$$_{2}$$ and UO$$_{2}$$ with particular focus on the nature of the hydroxyl radical formed as an intermediate. Experiments were performed to study the kinetics of the reaction at different initial H$$_{2}$$O$$_{2}$$ concentrations. The results show that the consumption rates at a given H$$_{2}$$O$$_{2}$$ concentration are different depending on the initial H$$_{2}$$O$$_{2}$$ concentration. This is attributed to an alteration of the reactive interface, likely caused by blocking of surface sites by oxidized U/surface-bound hydroxyl radicals. The U dissolution yield decreases with increasing initial H$$_{2}$$O$$_{2}$$ concentration. This is expected from the mechanism of catalytic decomposition of H$$_{2}$$O$$_{2}$$ on oxide surfaces. As the experiments were performed in solutions containing 10 mM and a strong concentration dependence was observed in the 0.2 - 2.0 mM H$$_{2}$$O$$_{2}$$ concentration range, we conclude that the intermediate hydroxyl radical is surface bound rather than free.

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Category:Chemistry, Inorganic & Nuclear

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