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Dissolution behavior of calcium uranate under oxidizing and reducing conditions

酸化・還元条件下におけるカルシウムウラネートの溶解挙動

加藤 雄斗*; 佐々木 隆之*; 頓名 龍太郎*; 小林 大志*; 岡本 芳浩  

Kato, Yuto*; Sasaki, Takayuki*; Tonna, Ryutaro*; Kobayashi, Taishi*; Okamoto, Yoshihiro

To assess the chemical stability of CaUO$$_{4}$$ in different aqueous environments, static immersion tests were performed under various redox conditions and carbonate ion concentrations. The dissolution mechanism of CaUO$$_{4}$$ was examined using data from solid and liquid analyses, along with chemical thermodynamic calculations. Under reducing conditions and without carbonate, U(VI) in CaUO$$_{4}$$ was reduced to U(V) and the mineral was converted into non-stoichiometric CaUO$$_{4-x}$$. The dissolved uranium was then further reduced to U(IV) in the aqueous media, forming UO$$_{2}$$(am), which controlled the U solubility. Under oxidizing conditions and in the absence of carbonate, dissolved uranium formed metaschoepite ((UO$$_{3}$$)2H$$_{2}$$O(cr)) at pH $$leqq$$ 7 and sodium diuranate (Na$$_{2}$$U$$_{2}$$O$$_{7}$$H$$_{2}$$O(cr)) at pH $$>$$ 7, which controlled uranium solubility. In oxidizing conditions with carbonate present, the apparent solubility of U was lower than predicted by the solid-phase solubility calculations. The concentration of U was constrained to levels similar to that of calcium when the calcium concentration reached saturation with CaCO$$_{3}$$. Additionally, the dissolution of calcium from CaUO$$_{4}$$ influenced uranium dissolution.

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分野:Geochemistry & Geophysics

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