Theoretical Study of Plutonium(IV) Complexes Formed within the PUREX Process: A Proposal of a Plutonium Surrogate in Fire Conditions

Abstract : We present a relativistic quantum chemical study to determine the best surrogate for plutonium(IV) to be used in experimental investigations of the behavior of plutonium-nitrate-TBP in fire conditions that might occur in the nuclear fuel refining process known as PUREX. In this study geometries and stabilities of Pu(NO3)62− and Pu(NO3)4(TBP)2 complexes were compared to that of equivalent complexes of selected elements from the lanthanide and actinide series (Ce, Th, U) chosen on the basis of similar ionic radii and stability as tetravalent species. PBE and PBE0 DFT functionals have proven to be sufficient and affordable for qualitative studies, performing as good as the wave function based correlated method MP2. On the basis of our results, cerium(IV) appears to be a good surrogate for plutonium(IV).
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Article dans une revue
Journal of Physical Chemistry A, American Chemical Society, 2014, 118, pp.10073-10080. 〈10.1021/jp507684f〉
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https://hal.archives-ouvertes.fr/hal-01077523
Contributeur : Valérie Vallet <>
Soumis le : samedi 25 octobre 2014 - 11:52:55
Dernière modification le : mardi 3 juillet 2018 - 11:21:47

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Martin Šulka, Valérie Vallet, Laurent Cantrel. Theoretical Study of Plutonium(IV) Complexes Formed within the PUREX Process: A Proposal of a Plutonium Surrogate in Fire Conditions. Journal of Physical Chemistry A, American Chemical Society, 2014, 118, pp.10073-10080. 〈10.1021/jp507684f〉. 〈hal-01077523〉

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