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Oxygen potentials of (U$$_{0.685}$$,Pu$$_{0.270}$$,Am$$_{0.045}$$)O$$_{2-x}$$ solid solutions

Osaka, Masahiko  ; Sato, Isamu; Namekawa, Takashi; Kurosaki, Ken*; Yamanaka, Shinsuke*

Oxygen potentials of (U,Pu)O$$_{2-x}$$ containing AmO$$_{2-x}$$, (U$$_{0.685}$$Pu$$_{0.270}$$Am$$_{0.045}$$)O$$_{2-x}$$, were measured as functions of the oxygen to metal (O/M) ratios and temperatures by hermogravimetric analysis (TGA) and discussed from thermodynamic viewpoints. The (U$$_{0.685}$$Pu$$_{0.270}$$Am$$_{0.045}$$)O$$_{2-x}$$ solid solution was prepared by a traditional powder metallurgical route. Oxygen partial pressure (pO$$_{2}$$) was adjusted in the region from 10$$^{-22}$$ to 10$$^{-8}$$ MPa by using CO$$_{2}$$/H$$_{2}$$ and H$$_{2}$$O /H$$_{2}$$ equilibria. Changes of microgram order in the specimen weight were continuously monitored with a TGA apparatus and the dependences of oxygen potentials on the O/M ratios were obtained at 1123K, 1273K and 1423K. The oxygen potentials of (U$$_{0.685}$$Pu$$_{0.270}$$Am$$_{0.045}$$)O$$_{2-x}$$ were significantly higher than those in (U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2-x}$$. The partial molar entropy and enthalpy of oxygen have been calculated and compared with those of Am O$$_{2-x}$$, (Am$$_{0.05}$$U$$_{0.05}$$) O$$_{2-x}$$, and (U$$_{0.7}$$Pu$$_{0.3}$$)O$$_{2-x}$$. Finally, the oxygen potential isotherms of (U$$_{0.685}$$,Pu$$_{0.270}$$,Am$$_{0.045}$$)O$$_{2-x}$$ were examined in terms of defect structure.

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