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Title: Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes

Abstract

Thermal transport in nuclear fuels used for nuclear energy applications is directly tied to performance and reliability. Uranium dioxide (UO2), one of the most important nuclear fuels, can accumulate excess oxygen atoms as interstitial defects, which significantly impacts thermal transport properties. In this study, thermal conductivities and inelastic neutron scattering (INS) measurements on UO2þx were performed at low temperatures (2–300K). The thermal conductivity of UO2þx (x¼0, 0.03, 0.04, and 0.11) is significantly suppressed compared to UO2 except near the Neel temperature TN ¼ 30.8K, where it is independent of x. INS measurements demonstrate that the heat capacities and phonon group velocities of UO2 and UO2.08 are similar, and the suppressed thermal conductivity results from smaller phonon lifetimes. These perceptions advance our understanding of thermal transport properties in advanced nuclear fuels and guide safe and economic utilization of nuclear energy.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Idaho National Lab. (INL), Idaho Falls, ID (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1878677
Alternate Identifier(s):
OSTI ID: 1875322; OSTI ID: 1923790
Report Number(s):
INL/JOU-22-66999-Rev000
Journal ID: ISSN 0003-6951; TRN: US2307540
Grant/Contract Number:  
AC05-00OR22725; the Center for Thermal Energy Transport under Irradiation; Advanced Fuel Campaign Program; AC07-05ID14517
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 121; Journal Issue: 1; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Crystallographic defects; Chemical compounds; Thermodynamic properties; Phonons; Nuclear fuel; Nuclear energy; Magnetism; Neutron scattering; Thermal conductivity; Transport properties

Citation Formats

Ma, Hao, Bryan, Matthew S., Pang, Judy W. L., Abernathy, Douglas L., Antonio, Daniel J., Gofryk, Krzysztof, and Manley, Michael E. Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes. United States: N. p., 2022. Web. doi:10.1063/5.0096655.
Ma, Hao, Bryan, Matthew S., Pang, Judy W. L., Abernathy, Douglas L., Antonio, Daniel J., Gofryk, Krzysztof, & Manley, Michael E. Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes. United States. https://doi.org/10.1063/5.0096655
Ma, Hao, Bryan, Matthew S., Pang, Judy W. L., Abernathy, Douglas L., Antonio, Daniel J., Gofryk, Krzysztof, and Manley, Michael E. Thu . "Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes". United States. https://doi.org/10.1063/5.0096655. https://www.osti.gov/servlets/purl/1878677.
@article{osti_1878677,
title = {Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes},
author = {Ma, Hao and Bryan, Matthew S. and Pang, Judy W. L. and Abernathy, Douglas L. and Antonio, Daniel J. and Gofryk, Krzysztof and Manley, Michael E.},
abstractNote = {Thermal transport in nuclear fuels used for nuclear energy applications is directly tied to performance and reliability. Uranium dioxide (UO2), one of the most important nuclear fuels, can accumulate excess oxygen atoms as interstitial defects, which significantly impacts thermal transport properties. In this study, thermal conductivities and inelastic neutron scattering (INS) measurements on UO2þx were performed at low temperatures (2–300K). The thermal conductivity of UO2þx (x¼0, 0.03, 0.04, and 0.11) is significantly suppressed compared to UO2 except near the Neel temperature TN ¼ 30.8K, where it is independent of x. INS measurements demonstrate that the heat capacities and phonon group velocities of UO2 and UO2.08 are similar, and the suppressed thermal conductivity results from smaller phonon lifetimes. These perceptions advance our understanding of thermal transport properties in advanced nuclear fuels and guide safe and economic utilization of nuclear energy.},
doi = {10.1063/5.0096655},
journal = {Applied Physics Letters},
number = 1,
volume = 121,
place = {United States},
year = {Thu Jul 07 00:00:00 EDT 2022},
month = {Thu Jul 07 00:00:00 EDT 2022}
}

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