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Influence of the first coordination of uranyl on its luminescence properties: study of uranyl binitrate with N,N-dialkyl amide DEHiBA and water

Hanna Oher 1, 2, * Geoffroy Ferru 3 Laurent Couston 3 Laurence Berthon 3 Dominique Guillaumont 3 Florent Réal 1 Thomas Vercouter 2 Valérie Vallet 1, *
* Corresponding author
1 PCMT - Physico-Chimie Moléculaire Théorique
PhLAM - Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523
3 CETAMA - Commission des méthodes d'analyse du CEA
DMRC - Département de recherche sur les procédés pour la mine et le recyclage du combustible : DES/ISEC/DMRC
Abstract : Uranyl binitrate complexes have a particular interest in the nuclear industry, especially in the reprocessing of spent nuclear fuel. The modified PUREX extraction process is designed to extract U(VI) in the form of UO2(NO3)2(L)2 as it has been confirmed by EXAFS, XRD and TRLFS measurements. In this study, the L ligands are two molecules of N,N-di-(ethyl- 2-hexyl)isobutyramide (DEHiBA) monoamide used to bind uranyl in its first coordination sphere. DEHiBA ligands can coordinate uranyl in either trans- or cis-positions with respect to the nitrate ligands and these two conformers may co-exist in solution. In order to use luminescence spectroscopy as a speciation technique, it is important to determine whether or not these conformers can be discriminated by their spectroscopic properties. To answer this question, the spectra of trans- and cis-UO2(NO3)2(DEiBA)2 conformers were modeled with ab initio methods and compared to the experimental time-resolved luminescence spectra on the UO2(NO3)2(DEHiBA)2 systems. Moreover, the hydrated uranyl binitrate UO2(NO3)2(H2O)2 complexes in the same trans and cis configurations were modeled to quantify the impact of organic DEHiBA on the luminescence properties.
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https://hal.archives-ouvertes.fr/hal-03325299
Contributor : Valérie Vallet Connect in order to contact the contributor
Submitted on : Tuesday, August 31, 2021 - 11:19:03 AM
Last modification on : Tuesday, January 18, 2022 - 4:16:04 PM
Long-term archiving on: : Wednesday, December 1, 2021 - 9:01:38 PM

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Hanna Oher, Geoffroy Ferru, Laurent Couston, Laurence Berthon, Dominique Guillaumont, et al.. Influence of the first coordination of uranyl on its luminescence properties: study of uranyl binitrate with N,N-dialkyl amide DEHiBA and water. Inorganic Chemistry, American Chemical Society, In press, ⟨10.1021/acs.inorgchem.1c02618⟩. ⟨hal-03325299⟩

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