Issue 1, 2017
From the journal:

Chemical Communications

Characteristics of chemical bonding of pentavalent uranium in La-doped UO2

Sergei M. Butorin,*a   Kristina O. Kvashnina,bc   Damien Prieur,d   Murielle Rivenete  and  Philippe M. Martinf  

* Corresponding authors

a Molecular and Condensed Matter Physics, Department of Physics and Astronomy, Uppsala University, P.O. Box 516, SE-751 20 Uppsala, Sweden
E-mail: sergei.butorin@physics.uu.se

b The European Synchrotron, CS40220, 38043 Grenoble Cedex 9, France

c Helmholtz Zentrum Dresden-Rossendorf (HZDR), Institute of Resource Ecology, P.O. Box 510119, Dresden, Germany

d European Commission, Joint Research Centre, Institute for Transuranium Elements, P.O. Box 2340, D-76125 Karlsruhe, Germany

e Université Lille, CNRS, Centrale Lille, ENSCL, Université Artois, UMR 8181, UCCS, Unité de Catalyse et Chimie du Solide, F-59000 Lille, France

f CEA Marcoule, CEA, DEN, DTEC/SECA/LCC, F-30207 Bagnols-sur-Cèze Cedex, France

Abstract

The effect of La doping on the electronic structure of U in UO2 was studied using an advanced technique, namely, X-ray absorption spectroscopy (XAS) in the high-energy-resolution fluorescence-detection (HERFD) mode, at the U 3d3/2 (M4) edge. Thanks to a significant reduction of the core–hole lifetime broadening and distinct chemical shifts of the HERFD-XAS lines, the U(V) formation as a result of La doping was identified. The isolated contribution of U(V) in the M4 HERFD-XAS spectrum reveals the so-called charge-transfer satellites due to the U 5f–O 2p hybridization. The analysis of the experimental data within the framework of the Anderson impurity model (AIM) indicates a significant change in the characteristics and degree of covalency for the chemical bonding in the U(V) subsystem of UO2 as compared to undoped UO2, which is a Mott–Hubbard system. The results are also supported by AIM calculations of X-ray photoelectron and optical absorption data.

Graphical abstract: Characteristics of chemical bonding of pentavalent uranium in La-doped UO2

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Article information

DOI
https://doi.org/10.1039/C6CC07684J
Article type
Communication
Submitted
21 Sep 2016
Accepted
15 Nov 2016
First published
15 Nov 2016

Chem. Commun., 2017,53, 115-118

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Characteristics of chemical bonding of pentavalent uranium in La-doped UO2

S. M. Butorin, K. O. Kvashnina, D. Prieur, M. Rivenet and P. M. Martin, Chem. Commun., 2017, 53, 115 DOI: 10.1039/C6CC07684J

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