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Oxidation behaviour of U3Si2: An experimental and first principles investigation

Abstract

Uranium-containing metallic systems such as U3Si2 are potential Accident Tolerant Fuel (ATF) for Light Water Reactors (LWRs) and the next generation of nuclear reactors. Its oxidation behaviour, especially in oxygen and water-enriched environments, plays a critical role in determining its applicability in commercial reactors. In this work, we have investigated the oxidative behaviour of U3Si2 experimentally and by theoretical computation. The appearance of oxide signatures has been established from X-ray diffraction (XRD) and Raman spectroscopic techniques after oxidation of the solid U3Si2 sample in synthetic air (oxygen and nitrogen). We have also studied the changes in electronic structure as well as the energetics of oxygen interactions on U3Si2 surfaces using first-principles calculations in the Density Functional Theory (DFT) formalism. Detailed charge transfer and bond length analyses revealed the preferential formation of mixed oxides of UO2 and SiO2 on the U3Si2 {001} surface as well as UO2 alone on the U3Si2 {110} and {111} surfaces. Formation of peroxo (O22-) state confirmed the dissociation of molecular oxygen before U3Si2 oxidation. Core experimental analyses of the oxidized U3Si2 samples have revealed the formation of higher oxides from Raman spectroscopy and XRD techniques. This work is introduced to further a better understanding of the oxidation of U-Si metallic fuel compounds.

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Publication details

The article was received on 21 Oct 2017, accepted on 12 Jan 2018 and first published on 12 Jan 2018


Article type: Paper
DOI: 10.1039/C7CP07154J
Citation: Phys. Chem. Chem. Phys., 2018, Accepted Manuscript
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    Oxidation behaviour of U3Si2: An experimental and first principles investigation

    E. E. Jossou, U. Eduok, N. Y. Dzade, B. Szpunar and Jerzy.A Szpunar, Phys. Chem. Chem. Phys., 2018, Accepted Manuscript , DOI: 10.1039/C7CP07154J

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