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100 1 _ |a Murphy, Gabriel L.
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245 _ _ |a The role of redox and structure on grain growth in Mn-doped UO2
260 _ _ |a London
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520 _ _ |a Mn-doped UO2 is considered a potential advanced nuclear fuel due to ameliorated microstructural grain growth compared to non-doped variants. However, recent experimental investigations have highlighted limitations in grain growth apparently arising from misunderstandings of its redox-structural chemistry. To resolve this, we use synchrotron X-ray diffraction and spectroscopy measurements supported by ab initio calculations to cross-examine the redox and structural chemistry of Mn-doped UO2 single crystal grains and ceramic specimens. Measurements reveal Mn enters the UO2 matrix divalently as with the additional formation of fluorite Mn+2O in the bulk material. Extended X-ray absorption near edge structure measurements unveil that during sintering, the isostructural relationship between fluorite UO2 and Mn+2O results in inadvertent interaction and subsequent incorporation of diffusing U species within MnO, rather than neighbouring UO2 grains, inhibiting grain growth. The investigation consequently highlights the significance of considering total redox-structural chemistry of main and minor phases in advanced ceramic material design.
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700 1 _ |a Rossberg, André
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700 1 _ |a Silva, Clara L.
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700 1 _ |a Amidani, Lucia
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773 _ _ |a 10.1038/s43246-024-00714-x
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