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Smith, A.L.; Guéneau, C.; Flèche, J.-L.; Chatain, S.; Beneš, O.; Konings, R.J.M., E-mail: a.l.smith@tudelft.nl2017
AbstractAbstract
[en] Highlights: • A CALPHAD model is reported for the Na-O and Na-U-O systems. • The CALPHAD model reproduces well the experimental data. • The CALPHAD model predicts the stability of the UO2-Na3UO4-Na4UO5 phase field. • Thermodynamic data are calculated by ab initio calculations and quasi-harmonic model. • The oxygen potential threshold to form Na3UO4 in liquid sodium at 900 K is 0.7 ppm. - Abstract: A thermodynamic model for the Na-O system was developed for the first time using the CALPHAD method after review of the structural, thermodynamic, and phase diagram data available on this system. Differential Scanning Calorimetry measurements were moreover performed to assess the phase equilibria and liquidus temperature in the Na2O-Na2O2 composition range. A CALPHAD model for the Na-U-O system was furthermore developed on the basis of both reviewed experimental data, and thermodynamic functions of the sodium uranates derived by combining ab initio calculations and a quasi-harmonic statistical model. The phase equilibria in this ternary system are particularly relevant for the safety assessment of the nuclear fuel-sodium coolant interaction in Sodium-cooled Fast reactors (SFRs). The model predicts the stability of the ternary phase field UO2-Na3UO4-Na4UO5, which is consistent with the most recent literature data. Further optimization was moreover performed to fit the sodium partial pressures measured experimentally in the NaUO3-Na2U2O7-UO2 and NaUO3-Na2UO4-Na2U2O7 phase fields, yielding an overall consistent description. Finally, the oxygen content required to form pentavalent Na3UO4 and hexavalent Na4UO5 in liquid sodium at 900 K were calculated to be 0.7 and 1.5 wppm, respectively, which are levels typically encountered in SFRs.
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S0021-9614(17)30108-8; Available from http://dx.doi.org/10.1016/j.jct.2017.04.003; Copyright (c) 2017 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
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Journal Article
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Numerical Data
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ACTINIDE COMPOUNDS, ALKALI METAL COMPOUNDS, DATA, DIAGRAMS, ENERGY, ENERGY SOURCES, FREE ENTHALPY, FUELS, INFORMATION, LIQUID METAL COOLED REACTORS, MATERIALS, MATHEMATICAL MODELS, NUMERICAL DATA, OXYGEN COMPOUNDS, PARTICLE MODELS, PHYSICAL PROPERTIES, REACTOR MATERIALS, REACTORS, SODIUM COMPOUNDS, STATISTICAL MODELS, THERMODYNAMIC PROPERTIES, URANATES, URANIUM COMPOUNDS
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