Vapor Pressures and Vapor Compositions in Equilibrium with Hypostoichiometric Plutonium Dioxide at High Temperatures PDF Download

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Vapor pressures and vapor compositions have been calculated for 1500 less than or equal to T less than or equal to 4000°K. Thermodynamic functions for the condensed phase and for each of the gaseous species were combined with an oxygen-potential model extended into the liquid region to obtain the partial pressures of O2, O, Pu, PuO and PuO2. The calculated oxygen pressures increase very rapidly as stoichiometry is approached. At least part of this increase is a consequence of the exclusion of Pu/sup 6 +/ from the oxygen-potential model. No reliable method was found to estimate the importance of this ion. As a result of large oxygen potentials at high temperatures, extremely high total pressures that produced unreasonably high vapor densities were calculated. The highest temperature was therefore limited to 400 K, and the range of oxygen-to-metal ratios was limited to 1.994 to 1.70. These calculations show that vapor in equilibrium with hypostoichiometric plutonium dioxide is poorly approximated as PuO2 for most of the temperture and composition range of interest. The vapor is much more oxygen-rich than the condensed phase. Implications for the (U, Pu)O/sub 2-x/ system are discussed. (DLC).