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Oxygen potentials of pyrochlore-type Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$

パイロクロア型Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$の酸素ポテンシャル

音部 治幹; 高野 公秀; 林 博和; 荒井 康夫

Otobe, Haruyoshi; Takano, Masahide; Hayashi, Hirokazu; Arai, Yasuo

パイロクロア型Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$の1333Kでの酸素ポテンシャルと酸素不定比組成(${it y}$)の関係をジルコニア固体電解質を用いた電気化学的手法と酸化還元による重量変化測定法で明らかにした。${it y}$が0から0.56まで増加したとき、1333Kでの酸素ポテンシャルは、-516.52から0kJ/molまで一様に増加した。1333KでのAm$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$の酸素ポテンシャルは、同じO/MについてAmO$$_{2-x}$$よりも約130kJ/mol高いことがわかった。この酸素ポテンシャル差は、AmとPuのイオン半径の差を考慮すれば、Pu$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$とPuO$$_{2-x}$$の酸素ポテンシャル差と整合性があり、超ウラン元素酸化物の熱力学的性質の系統的な理解につながる結果である。

The relations between the oxygen potentials and the oxygen-nonstoichiometry (${it y}$) of the pyrochlore-type Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$ for 1333 K were measured by the electrochemical method using a zirconia solid electrolyte and the mass changes by the oxidation and reduction. It was found that the oxygen potential of Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$ smoothly increased from -516.52 to 0 kJ/mol with increasing ${it y}$ from 0.0 to 0.56 at 1333K. The oxygen potentials of Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$ were higher than those of AmO$$_{2-x}$$ at the corresponding O/M by approximately 130 kJ/mol. The difference of the oxygen potentials between Am$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$ and AmO$$_{2-x}$$ was consistent with that between Pu$$_{2}$$Zr$$_{2}$$O$$_{7+y}$$ and PuO$$_{2-x}$$ considering the difference of the ionic radii between Am and Pu. This leads to the systematical understanding of the thermodynamic properties of the transuraniumm oxides.

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パーセンタイル:85.87

分野:Materials Science, Ceramics

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