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The Kinetics and mechanism of H$$_{2}$$O$$_{2}$$ decomposition at the U$$_{3}$$O$$_{8}$$ surface in bicarbonate solution

炭酸塩水溶液中でのU$$_{3}$$O$$_{8}$$表面における過酸化水素反応の速度論とメカニズム

McGrady, J.  ; 熊谷 友多   ; 渡邉 雅之   ; 桐島 陽*; 秋山 大輔*; 北村 暁  ; 紀室 辰伍   

McGrady, J.; Kumagai, Yuta; Watanabe, Masayuki; Kirishima, Akira*; Akiyama, Daisuke*; Kitamura, Akira; Kimuro, Shingo

The rate of U release is affected by bicarbonate (HCO$$_{3}$$$$^{-}$$) concentrations in the groundwater, as well as H$$_{2}$$O$$_{2}$$ produced by water radiolysis. To understand the dissolution of U$$_{3}$$O$$_{8}$$ by H$$_{2}$$O$$_{2}$$ in bicarbonate solution (0.1 - 50 mM), dissolved U concentrations were measured upon H$$_{2}$$O$$_{2}$$ addition (300 $$mu$$M) to U$$_{3}$$O$$_{8}$$/bicarbonate mixtures. As the H$$_{2}$$O$$_{2}$$ decomposition mechanism is integral to U dissolution, the kinetics and mechanism of H$$_{2}$$O$$_{2}$$ decomposition at the U$$_{3}$$O$$_{8}$$ surface was investigated. The dissolution of U increased with bicarbonate concentration which was attributed to a change in the H$$_{2}$$O$$_{2}$$ decomposition mechanism from catalytic at low bicarbonate ($$leq$$ 5 mM HCO$$_{3}$$$$^{-}$$) to oxidative at high bicarbonate ($$geq$$ 10 mM HCO$$_{3}$$$$^{-}$$). Catalytic H$$_{2}$$O$$_{2}$$ at low bicarbonate was attributed to the formation of an oxidised surface layer.

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パーセンタイル:39.59

分野:Chemistry, Multidisciplinary

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