Smith, H., Townsend, L.T., Mohun, R. et al. (5 more authors) (2022) Cr2+ solid solution in UO2 evidenced by advanced spectroscopy. Communications Chemistry, 5. 163. ISSN 2399-3669
Abstract
Advanced Cr-doped UO2 fuels are essential for driving safe and efficient generation of nuclear energy. Although widely deployed, little is known about their fundamental chemistry, which is a critical gap for development of new fuel materials and radioactive waste management strategies. Utilising an original approach, we directly evidence the chemistry of Cr(3+)2O3–doped U(4+)O2. Advanced high-flux, high-spectral purity X-ray absorption spectroscopy (XAS), corroborated by diffraction, Raman spectroscopy and high energy resolved fluorescence detection-XAS, is used to establish that Cr2+ directly substitutes for U4+, accompanied by U5+ and oxygen vacancy charge compensation. Extension of the analysis to heat-treated simulant nuclear fuel reveals a mixed Cr2+/3+ oxidation state, with Cr in more than one physical form, explaining the substantial discrepancies that exist in the literature. Successful demonstration of this analytical advance, and the scientific underpinning it provides, opens opportunities for an expansion in the range of dopants utilised in advanced UO2 fuels.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © The Author(s) 2022. Open Access: This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
Keywords: | Ceramics; Energy science and technology; Materials science; Nuclear energy; Techniques and instrumentation |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Engineering (Sheffield) > Department of Materials Science and Engineering (Sheffield) |
Funding Information: | Funder Grant number EUROPEAN COMMISSION - HORIZON 2020 755443 ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL EP/N017374/1 ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL EP/T011424/1 Engineering and Physical Sciences Research Council EP/T011424/1 ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL EP/R006075/1 Engineering and Physical Sciences Research Council EP/V035215/1 ENGINEERING AND PHYSICAL SCIENCE RESEARCH COUNCIL EP/V035215/1 Engineering and Physical Sciences Research Council EP/R006075/1 |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 16 Nov 2022 17:12 |
Last Modified: | 05 Dec 2022 13:33 |
Status: | Published |
Publisher: | Nature Portfolio |
Refereed: | Yes |
Identification Number: | 10.1038/s42004-022-00784-3 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:193291 |