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Redox response of actinide materials to highly ionizing radiation

Tracy, Cameron L. and Lang, Maik and Pray, John M. and Zhang, Fuxiang and Popov, Dmitry and Park, Changyong and Trautmann, Christina and Bender, Markus and Severin, Daniel and Skuratov, Vladimir A. and Ewing, Rodney C. (2015):
Redox response of actinide materials to highly ionizing radiation.
In: Nature Communications, Nature Publishing Group, London, England, p. 6133, 6, ISSN 2041-1723,
[Online-Edition: http://dx.doi.org/10.1038/ncomms7133],
[Article]

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.

Item Type: Article
Erschienen: 2015
Creators: Tracy, Cameron L. and Lang, Maik and Pray, John M. and Zhang, Fuxiang and Popov, Dmitry and Park, Changyong and Trautmann, Christina and Bender, Markus and Severin, Daniel and Skuratov, Vladimir A. and Ewing, Rodney C.
Title: Redox response of actinide materials to highly ionizing radiation
Language: English
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.

Journal or Publication Title: Nature Communications
Volume: 6
Publisher: Nature Publishing Group, London, England
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Ion-Beam-Modified Materials
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences
Date Deposited: 29 Feb 2016 13:56
Official URL: http://dx.doi.org/10.1038/ncomms7133
Identification Number: doi:10.1038/ncomms7133
Funders: This work was supported as part of the Materials Science of Actinides, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0001089., HPCAT operations are supported by DOE-NNSA under Award No. DE-NA0001974 and DOE-BES under Award No. DE-FG02-99ER45775, with partial instrumentation funding by NSF., This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357., HPCAT beamtime was granted by the Cargnegie/DOE Alliance Center (CDAC).
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