The high-temperature heat capacity of the (Th,U)O-2 and (U,Pu)O-2 solid solutions

SO Valu and O Benes and D Manara and RJM Konings and MWD Cooper and RW Grimes and C Gueneau, JOURNAL OF NUCLEAR MATERIALS, 484, 1-6 (2017).

DOI: 10.1016/j.jnucmat.2016.11.010

The enthalpy increment data for the (Th,U)O-2 and (U,Pu)O-2 solid solutions are reviewed and complemented with new experimental data (400-1773 K) and many-body potential model simulations. The results of the review show that from room temperature up to about 2000 K the enthalpy data are in agreement with the additivity rule (Neumann-Kopp) in the whole composition range. Above 2000 K the effect of Oxygen Frenkel Pair (OFP) formation leads to an excess enthalpy (heat capacity) that is modeled using the enthalpy and entropy of OFP formation from the end-members. A good agreement with existing experimental work is observed, and a reasonable agreement with the results of the many-body potential model, which indicate the presence of the diffuse Bredig (superionic) transition that is not found in the experimental enthalpy increment data. (C) 2016 Published by Elsevier B.V.

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