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Issue 1, 2017
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Characteristics of chemical bonding of pentavalent uranium in La-doped UO2

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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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Publication details

The article was received on 21 Sep 2016, accepted on 15 Nov 2016 and first published on 15 Nov 2016


Article type: Communication
DOI: 10.1039/C6CC07684J
Citation: 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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