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Etude théorique de complexes d'éléments f trivalents pour le retraitement des déchets nucléaires

Abstract : Current energetic and environmental concerns have made the nuclear waste reprocessing to be a major issue in numerous countries. One avenue to treat nuclear spent fuel requires separating selectively trivalent minor actinides An (Am3+, Cm3+) from lanthanides Ln. In this regard, nitrogen extractants are under study. Their selectivity toward actinides is still unclear, but could be the result of enhanced covalency effects with trivalent minor actinides with respect to lanthanides(III). In this thesis, we have performed DFT calculations (Density Functional Theory) to study covalency effects within the actinide-ligand bond, following three main axes of research: advanced study of the nature of the chemical bonding, spectroscopic characterization of covalency, and preliminary tests of ab initio molecular dynamics for future calculations in solvent. Methods that are not regularly applied to trivalent actinides complexes have been used: topological methods, TDDFT, LDDFT, ab initio molecular dynamics. We have managed to show that the selectivity of the BTP ligand - the most effective An/Ln extractant to date - comes at least for a part from stronger covalency effects within the An-BTP bond with respect to the Ln-BTP bond, which has never been proved before.
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https://tel.archives-ouvertes.fr/tel-00198899
Contributor : Laurence Petit <>
Submitted on : Tuesday, December 18, 2007 - 10:26:25 AM
Last modification on : Wednesday, November 4, 2020 - 2:34:00 PM
Long-term archiving on: : Monday, April 12, 2010 - 8:16:40 AM

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  • HAL Id : tel-00198899, version 1

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Laurence Petit. Etude théorique de complexes d'éléments f trivalents pour le retraitement des déchets nucléaires. Autre. Université Joseph-Fourier - Grenoble I, 2007. Français. ⟨tel-00198899⟩

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