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Homogeneity of (U, $$M$$)O$$_2$$ ($$M$$ = Th, Np) prepared by supercritical hydrothermal synthesis

超臨界水合成による(U, $$M$$)O$$_2$$ ($$M$$ = Th, Np)の均質性

白崎 謙次*; 田端 千紘*; 砂賀 彩光*; 酒井 宏典  ; Li, D.*; 小中 真理子*; 山村 朝雄*

Shirasaki, Kenji*; Tabata, Chihiro*; Sunaga, Ayaki*; Sakai, Hironori; Li, D.*; Konaka, Mariko*; Yamamura, Tomoo*

添加剤を変えながらウラン酸化物(U, $$M$$)O$$_2$$ ($$M$$=Th, Np)固溶体を超臨界水熱合成で調製した。それらの試料の均質性をVegard則に基づいた結晶構造解析や、(U, Np, Na)O$$_2$$固溶体については、$$^{23}$$Na核核磁気共鳴(NMR)によって調べた。その結果、(i) (U, Th)O$$_{2+x}$$固溶体の場合は、炭酸アンモニウムを添加剤として、IV価ウランから出発し、(ii) (U, Np)O$$_{2+x}$$の場合は、エタノールを添加剤として、VI価ウランから出発すると、均質な試料が得られることがわかった。

We focused on the direct synthesis of (U, $$M$$)O$$_2$$ solid solution ($$M$$=Th, Np) by extending our recent progress in hydrothermal synthesis with additives. The homogeneity of the (U, $$M$$)O$$_2$$ ($$M$$ = Th, Np) systems prepared by supercritical hydrothermal reactions was investigated through crystallographic analysis based on Vegard's law, and the $$^{23}$$Na nuclear magnetic resonance (NMR) measurement of (U, Np, Na)O$$_2$$ solid solutions. Our experimental and analytical results revealed that (i) an optimal additive is ammonium carbonate and starting uranium valence is IV in the case of (U, Th)O$$_{2+x}$$, and (ii) an optimal additive is ethanol and starting uranium valence is VI in the case of (U, Np)O$$_{2+x}$$, for producing the homogeneous solid solutions by hydrothermal synthesis.

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