Oxygen transport in off-stoichiometric uranium dioxide mediated by defect clustering dynamics

Yu, Jianguo; Bai, Xian -Ming; El-Azab, Anter; Allen, Todd R.

doi:10.1063/1.4914137

Title: Oxygen transport in off-stoichiometric uranium dioxide mediated by defect clustering dynamics

Journal Article · Thu Mar 05 00:00:00 EST 2015 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4914137· OSTI ID:1248176

Yu, Jianguo ^[1]; Bai, Xian -Ming ^[1]; El-Azab, Anter ^[2]; Allen, Todd R. ^[3]

Idaho National Lab. (INL), Idaho Falls, ID (United States)
Purdue Univ., West Lafayette, IN (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States); Univ. of Wisconsin-Madison, Madison, WI (United States)

In this study, oxygen transport is central to many properties of oxides such as stoichiometric changes, phase transformation and ionic conductivity. In this paper, we report a mechanism for oxygen transport in uranium dioxide (UO₂) in which the kinetics is mediated by defect clustering dynamics. In particular, the kinetic Monte Carlo (KMC) method has been used to investigate the kinetics of oxygen transport in UO₂ under the condition of creation and annihilation of oxygen vacancies and interstitials as well as oxygen interstitial clustering, with variable offstoichiometry and temperature conditions. It is found that in hypo-stoichiometric UO_2-x, oxygen transport is well described by the vacancy diffusion mechanism while in hyper-stoichiometric UO_2+x, oxygen interstitial cluster diffusion contributes significantly to oxygen transport kinetics, particularly at high temperatures and high off-stoichiometry levels. It is also found that diinterstitial clusters and single interstitials play dominant roles in oxygen diffusion while other larger clusters have negligible contributions. However, the formation, coalescence and dissociation of these larger clusters indirectly affects the overall oxygen diffusion due to their interactions with mono and di-interstitials, thus providing a explanation of the experimental observation of saturation or even drop of oxygen diffusivity at high off-stoichiometry.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Materials Science of Nuclear Fuel (CMSNF); Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 1248176

Alternate ID(s):: OSTI ID: 1228119

Report Number(s):: INL/JOU-14-33670; JCPSA6

Journal Information:: Journal of Chemical Physics, Vol. 142, Issue 9; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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