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Analysis of oxygen potential of (U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2pm x}$$ and (U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2pm x}$$ based on point defect chemistry

点欠陥化学による(U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2pm x}$$及び((U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2pm x}$$の酸素ポテンシャルの解析

加藤 正人; 小無 健司*; 中江 延男

Kato, Masato; Konashi, Kenji*; Nakae, Nobuo

(U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2pm x}$$及び(U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2pm x}$$の不定比性について、点欠陥化学により実験データから解析を行った。定比組成からのずれXと酸素分圧の関係を評価し、Kr$"o$ger-Vink図を用いてMOXの点欠陥濃度を酸素分圧と温度の関数として見積もった。定比組成近傍では、Xは$$Delta$$に比例し、電気的欠陥が支配することを示した。また、酸素ポテンシャルを計算するためのモデルを導き、実験データを精度よく再現した。定比組成の(U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2.00}$$及び(U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2.00}$$について、それぞれ、-552.5kJ/mol及び-149.7J/mol, -674.0kJ/mol及び-219.4J/molと決定した。

Stoichiometries in (U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2pm x}$$ and (U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2pm x}$$ were analyzed from the experimental data of oxygen potential based on point defect chemistry. The relation between the deviation x from stoichimetric composition and oxygen partial pressure were evaluated. The concentrations of the point defects in MOX were estimated from the measured data of oxygen potential as functions of temperature and using Kr$"o$ger-Vink diagram. The analysis results showed that x was proportional to near stoichiometric region of both (U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2pm x}$$ and (U$$_{0.8}$$Pu$$_{0.2}$$)O$$_{2pm x}$$, which suggested that intrinsic ionization was dominant defect. The model to calculate oxygen potential was derived and represented the experimental data with precision, and thermodynamic data.

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パーセンタイル:18.28

分野:Materials Science, Multidisciplinary

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