Theoretical Study of Plutonium(IV) Complexes Formed within the PUREX Process: A Proposal of a Plutonium Surrogate in Fire Conditions - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Journal of Physical Chemistry A Année : 2014

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

Résumé

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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Dates et versions

hal-01077523 , version 1 (25-10-2014)

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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, 2014, 118, pp.10073-10080. ⟨10.1021/jp507684f⟩. ⟨hal-01077523⟩
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