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Interactions between anionic complex species of actinides and negatively charged mineral surfaces

負電荷を持つアクチニド元素の錯イオンと負に帯電した鉱物表面との相互作用

山口 徹治 ; 中山 真一 ; 吉田 崇宏

Yamaguchi, Tetsuji; Nakayama, Shinichi; Yoshida, Takahiro

アクチニド元素等がおもに陰イオン種(Th(CO$$_{3}$$)$$_{5}$$$$^{6-}$$, Am(CO$$_{3}$$)$$_{3}$$$$^{3-}$$, Np(CO$$_{3}$$)$$_{2}$$(OH)$$_{2}$$$$^{2-}$$, UO$$_{2}$$(OH)$$_{4}$$$$^{2-}$$, NpO$$_{2}$$(OH)$$_{2}$$$$^{-}$$, Sn(OH)$$_{5}$$$$^{-}$$及びPb(OH)$$_{3}$$$$^{-}$$)として溶存する条件で、負に帯電した鉱物表面への吸着を調べた。これらの元素が溶存していることを溶液調整2日後に確認した後、鉱物($$gamma$$-アルミナ又はシリカ,AEROSIL製,比表面積:10$$^{5}$$m$$^{2}$$kg$$^{-1}$$)を添加した。2日間以上吸着させた後、分画分子量10$$^{4}$$daltonの限外フィルタで固液を分離し、溶液中におけるこれらの元素濃度を分析した。実験は室温(25$$^{circ}$$C)のアルゴン雰囲気下で実施した。求められた分配係数は、pHや炭酸イオン濃度に対して単調に減少し、下げ止まりが見られなかった。このことから、実験を行ったpH範囲では負電荷を持つ錯体と負に帯電した鉱物表面との間に作用していたのは、おもに静電的な反発作用であったと考えられる。

Adsorption of actinides onto negatively charged mineral surfaces was investigated under conditions that actinides were predominantly present as anionic complex species: Th(CO$$_{3}$$)$$_{5}$$$$^{6-}$$, Am(CO$$_{3}$$)$$_{3}$$$$^{3-}$$, Np(CO$$_{3}$$)$$_{2}$$(OH)$$_{2}$$$$^{2-}$$, UO$$_{2}$$(OH)$$_{4}$$$$^{2-}$$, NpO$$_{2}$$(OH)$$_{2}$$$$^{-}$$, Sn(OH)$$_{5}$$$$^{-}$$ and Pb(OH)$$_{3}$$$$^{-}$$. These solutions were left to stand for 2 days to confirm these elements stable in dissolved state, and then contacted with minerals, $$gamma$$-Al$$_{2}$$O$$_{3}$$ or SiO$$_{2}$$ (AEROSIL, specific surface area: 10$$^{5}$$ m$$^{2}$$ kg$$^{-1}$$). After desired contact time for 2 days or more, the solutions were ultra-filtered through 10$$^{4}$$-molecular-weight cutoff Millipore filters and the concentrations of the elements in the filtrates were determined. The sorption experiments were performed at room temperature (25$$^{circ}$$C) under Ar. Distribution coefficients decreased with the increasing pH and with increasing carbonate concentrations. The monotonous decrease in the distribution coefficients in the investigated pH range suggests that the electrostatic repulsion was a dominant interaction between anionic complex species of actinides and negatively charged mineral surfaces.

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パーセンタイル:40.72

分野:Chemistry, Inorganic & Nuclear

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