Deconvoluting Cr states in Cr-doped UO2 nuclear fuels via bulk and single crystal spectroscopic studies

Gabriel L. Murphy (), Robert Gericke, Sara Gilson, Elena F. Bazarkina, André Rossberg, Peter Kaden, Robert Thümmler, Martina Klinkenberg, Maximilian Henkes, Philip Kegler, Volodymyr Svitlyk, Julien Marquardt, Theresa Lender, Christoph Hennig, Kristina O. Kvashnina and Nina Huittinen ()
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Gabriel L. Murphy: Forschungszentrum Jülich GmbH
Robert Gericke: Helmholtz-Zentrum Dresden-Rossendorf
Sara Gilson: Helmholtz-Zentrum Dresden-Rossendorf
Elena F. Bazarkina: Helmholtz-Zentrum Dresden-Rossendorf
André Rossberg: Helmholtz-Zentrum Dresden-Rossendorf
Peter Kaden: Helmholtz-Zentrum Dresden-Rossendorf
Robert Thümmler: Forschungszentrum Jülich GmbH
Martina Klinkenberg: Forschungszentrum Jülich GmbH
Maximilian Henkes: Forschungszentrum Jülich GmbH
Philip Kegler: Forschungszentrum Jülich GmbH
Volodymyr Svitlyk: Helmholtz-Zentrum Dresden-Rossendorf
Julien Marquardt: Goethe-Universität Frankfurt
Theresa Lender: RWTH Aachen University
Christoph Hennig: Helmholtz-Zentrum Dresden-Rossendorf
Kristina O. Kvashnina: Helmholtz-Zentrum Dresden-Rossendorf
Nina Huittinen: Helmholtz-Zentrum Dresden-Rossendorf

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Cr-doped UO2 is a leading accident tolerant nuclear fuel where the complexity of Cr chemical states in the bulk material has prevented acquisition of an unequivocal understanding of the redox chemistry and mechanism for incorporation of Cr in the UO2 matrix. To resolve this, we have used electron paramagnetic resonance, high energy resolution fluorescence detection X-ray absorption near energy structure and extended X-ray absorption fine structure spectroscopic measurements to examine Cr-doped UO2 single crystal grains and bulk material. Ambient condition measurements of the single crystal grains, which have been mechanically extracted from bulk material, indicated Cr is incorporated substitutionally for U+4 in the fluorite lattice as Cr+3 with formation of additional oxygen vacancies. Bulk material measurements reveal the complexity of Cr states, where metallic Cr (Cr0) and oxide related Cr+2 and Cr+32O3 were identified and attributed to grain boundary species and precipitates, with concurrent (Cr+3xU+41-x)O2-0.5x lattice matrix incorporation. The deconvolution of chemical states via crystal vs. powder measurements enables the understanding of discrepancies in literature whilst providing valuable direction for safe continued use of Cr-doped UO2 fuels for nuclear energy generation.

Date: 2023
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DOI: 10.1038/s41467-023-38109-0

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