Energetics of Ce and Pu incorporation into zirconolite waste-forms

文献情報

出版日 2011-06-21

DOI 10.1039/C0CP01478H

インパクトファクター 3.676

著者

M. Gilbert, J. H. Harding

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要旨

The General Utility Lattice Program (GULP) has been used to model the zirconolite lattice, calculate the energies of substituting Ce3+, Ce4+, Pu3+, Pu4+ and Fe3+ into the lattice both as single and multi-defect systems and model the formation of Ce3+, Ce4+, Pu3+ and Pu4+ doped zirconolite lattices. These results have been compared against experimental observations, with particular emphasis on those Ce containing solid solutions that exhibit Ce3+/Ce4+ mixed valence characteristics. It is found that the Ce3+/Ce4+ mixed valence is as a result of reduction within the lattice, with the Ce3+ being stabilised on the Ca site, and that this behaviour would not be expected for the corresponding Pu solid solutions.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

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