Redox response of actinide materials to highly ionizing radiation

Cameron L. Tracy, Maik Lang, John M. Pray, Fuxiang Zhang, Dmitry Popov, Changyong Park, Christina Trautmann, Markus Bender, Daniel Severin, Vladimir A. Skuratov and Rodney C. Ewing ()
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Cameron L. Tracy: University of Michigan
Maik Lang: University of Tennessee
John M. Pray: University of Michigan
Fuxiang Zhang: University of Michigan
Dmitry Popov: High Pressure Collaborative Access Team (HPCAT), Geophysical Laboratory, Carnegie Institution of Washington
Changyong Park: High Pressure Collaborative Access Team (HPCAT), Geophysical Laboratory, Carnegie Institution of Washington
Christina Trautmann: GSI Helmholtzzentrum für Schwerionenforschung
Markus Bender: GSI Helmholtzzentrum für Schwerionenforschung
Daniel Severin: GSI Helmholtzzentrum für Schwerionenforschung
Vladimir A. Skuratov: Flerov Laboratory of Nuclear Reactions, Joint Institute for Nuclear Research
Rodney C. Ewing: Stanford University

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: Abstract Energetic radiation can cause dramatic changes in the physical and chemical properties of actinide materials, degrading their performance in fission-based energy systems. As advanced nuclear fuels and wasteforms are developed, fundamental understanding of the processes controlling radiation damage accumulation is necessary. Here we report oxidation state reduction of actinide and analogue elements caused by high-energy, heavy ion irradiation and demonstrate coupling of this redox behaviour with structural modifications. ThO2, in which thorium is stable only in a tetravalent state, exhibits damage accumulation processes distinct from those of multivalent cation compounds CeO2 (Ce3+ and Ce4+) and UO3 (U4+, U5+ and U6+). The radiation tolerance of these materials depends on the efficiency of this redox reaction, such that damage can be inhibited by altering grain size and cation valence variability. Thus, the redox behaviour of actinide materials is important for the design of nuclear fuels and the prediction of their performance.

Date: 2015
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DOI: 10.1038/ncomms7133

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