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The formalism of electronic density-functional-theory, with Hubbard-Ucorrections (DFT+U), is employed in a computational study of the energetics ofU_{1-x} Ce_x O_2 mixtures. The computational approach makes use of a procedurewhich facilitates convergence of the calculations to multiple self-consistentDFT+U solutions for a given cation arrangement, corresponding to differentcharge states for the U and Ce ions in several prototypical cationarrangements. Results indicate a significant dependence of the structural andenergetic properties on the nature of both charge and cation ordering. With theeffective Hubbard-U parameters that reproduce well the measuredoxidation-reduction energies for urania and ceria, we find that charge transferbetween U(IV) and Ce(IV) ions, leading to the formation of U(V) and Ce(III),gives rise to an increase in the mixing energy in the range of 4-14 kJ/mol offormula unit, depending on the nature of the cation ordering. The resultssuggest that although charge transfer between uranium and cerium ions isdisfavored energetically, it is likely to be entropically stabilized at thehigh temperatures relevant to the processing and service of urania-based solidsolutions.

First-principles study of the energetics of charge and cation mixing in U_{1-x} Ce_x O_2