Melting behaviour of uranium-americium mixed oxides under different atmospheres

•The very high melting temperatures of (U,Am)-oxides (T > 2500 K) were measured.•The effect of the oxidation on the melting behaviour was studied.•Extensive post-melting characterizations were performed (SEM, XAS).•A CALPHAD thermodynamic modeling of the liquid in the U-Am-O system was obtained....

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Veröffentlicht in:The Journal of chemical thermodynamics 2020-01, Vol.140, p.105896, Article 105896
Hauptverfasser: Epifano, E., Prieur, D., Martin, P.M., Guéneau, C., Dardenne, K., Rothe, J., Vitova, T., Dieste, O., Wiss, T., Konings, R.J.M., Manara, D.
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Sprache:eng
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Zusammenfassung:•The very high melting temperatures of (U,Am)-oxides (T > 2500 K) were measured.•The effect of the oxidation on the melting behaviour was studied.•Extensive post-melting characterizations were performed (SEM, XAS).•A CALPHAD thermodynamic modeling of the liquid in the U-Am-O system was obtained. In the context of a comprehensive campaign for the characterisation of transmutation fuels for next generation nuclear reactors, the melting behaviour of mixed uranium-americium dioxides has been experimentally studied for the first time by laser heating, for Am concentrations up to 70 mol. % under different types of atmospheres. Extensive post-melting material characterisations were then performed by X-ray absorption spectroscopy and electron microscopy. The melting temperatures observed for the various compositions follow a markedly different trend depending on the experimental atmosphere. Uranium-rich samples melt at temperatures significantly lower (around 2700 K) when they are laser-heated in a strongly oxidizing atmosphere compressed air at (0.300 ± 0.005) MPa, compared to the melting points (beyond 3000 K) registered for the same compositions in an inert environment (pressurised Ar). This behaviour has been interpreted on the basis of the strong oxidation of such samples in air, leading to lower-melting temperatures. Thus, the melting temperature trend observed in air is characterized, in the purely pseudo-binary dioxide plane, by an apparent maximum melting temperature around 2850 K for 0.3 
ISSN:0021-9614
1096-3626
DOI:10.1016/j.jct.2019.105896