Title :

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

Author(s) :

Oher, Hanna [Auteur correspondant]
Service d'études analytiques et de réactivité des surfaces [SEARS]
Physico-Chimie Moléculaire Théorique [PCMT]
Ferru, Geoffroy [Auteur]
Commission des méthodes d'analyse du CEA [CETAMA]
Couston, Laurent [Auteur]
Commission des méthodes d'analyse du CEA [CETAMA]
Berthon, Laurence [Auteur]
Commission des méthodes d'analyse du CEA [CETAMA]
Guillaumont, Dominique [Auteur]
Commission des méthodes d'analyse du CEA [CETAMA]
Réal, Florent [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Vercouter, Thomas [Auteur]
Service d'études analytiques et de réactivité des surfaces [SEARS]
Vallet, Valérie [Auteur correspondant]
Physico-Chimie Moléculaire Théorique [PCMT]

Journal title :

INORGANIC CHEMISTRY

Pages :

890–901

Publisher :

American Chemical Society

Publication date :

2022-01-17

ISSN :

0020-1669

English keyword(s) :

uranyl
fluorescence spectroscopy
ab initio

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Chimie/Chimie de coordination

English abstract : [en]

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 ...
Show more >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.Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

ANR Project :

Physiques et Chimie de l'Environnement Atmosphérique
ULNE

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL