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Reaction of hydrogen peroxide with uranium zirconium oxide solid solution; Zirconium hinders oxidative uranium dissolution

Kumagai, Yuta; Takano, Masahide ; Watanabe, Masayuki

We studied oxidative dissolution of uranium and zirconium oxide [(U,Zr)O$$_{2}$$] in aqueous H$$_{2}$$O$$_{2}$$ solution. The interfacial reaction is essential for anticipating how a (U,Zr)O$$_{2}$$-based molten fuel may chemically degrade after a severe accident under influence of ionizing radiation. We conducted our experiments with (U,Zr)O$$_{2}$$ powder and quantitated the H$$_{2}$$O$$_{2}$$ reaction via dissolved U and H$$_{2}$$O$$_{2}$$ concentrations. The dissolution yield relative to H$$_{2}$$O$$_{2}$$ consumption was far less for (U,Zr)O$$_{2}$$ compared to that of UO$$_{2}$$. The reaction kinetics indicates that most of the H$$_{2}$$O$$_{2}$$ catalytically decomposed to O$$_{2}$$ at the surface of (U,Zr)O$$_{2}$$. We confirmed the H$$_{2}$$O$$_{2}$$ catalytic decomposition via O$$_{2}$$ production (quantitative stoichiometric agreement). In addition, post-reaction Raman scattering spectra of the undissolved (U,Zr)O$$_{2}$$ showed no additional peaks (indicating a lack of secondary phase formation). The (U,Zr)O$$_{2}$$ matrix is much more stable than UO$$_{2}$$ against H$$_{2}$$O$$_{2}$$-induced oxidative dissolution.

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Category:Materials Science, Multidisciplinary

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