期刊
INORGANIC CHEMISTRY
卷 56, 期 13, 页码 7416-7432出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.7b00572
关键词
-
资金
- CEA-SETAM project
In the frame of minor actinide transmutation, americium can be diluted in UO2 and (U, Pu)O-2 fuels burned in fast neutron reactors. The first mandatory step to foresee the influence of Am on the in-reactor behavior of transmutation targets or fuel is to have fundamental knowledge of the Am-O binary system and, in particular, of the AmO2-x, phase. In this study, we coupled HT-XRD (high-temperature X-ray diffraction) experiments with CALPHAD thermodynamic modeling to provide new insights into the structural properties and phase equilibria in the AmO2-x-AmO1.61+x-Am2O3 domain. Because of this approach, we were able for the first time to assess the relationships between temperature, lattice parameter, and hypostoichiometry for fcc AmO2-x. We showed the presence of a hyperstoichiometric existence domain for the bcc AmO1.61+x phase and the absence of a miscibility gap in the fcc AmO2-x phase, contrary to previous representations of the phase diagram. Finally, with the new experimental data, a new CALPHAD thermodynamic model of the Am-O system was developed, and an improved version of the phase diagram is presented.
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