Molecular dynamics simulation of thermal transport in containing uranium, oxygen, and fission-product defects
Abstract
Uranium dioxide (UO2) is the most commonly used fuel in light-water nuclear reactors and thermal conductivity controls the removal of heat produced by fission, thereby governing fuel temperature during normal and accident conditions. The use of fuel performance codes by the industry to predict operational behavior is widespread. A primary source of uncertainty in these codes is thermal conductivity, and optimized fuel utilization may be possible if existing empirical models are replaced with models that incorporate explicit thermal-conductivity-degradation mechanisms during fuel burn up. This approach is able to represent the degradation of thermal conductivity due to each individual defect type, rather than the overall burn-up measure typically used, which is not an accurate representation of the chemical or microstructure state of the fuel that actually governs thermal conductivity and other properties. To generate a mechanistic thermal conductivity model, molecular dynamics (MD) simulations of UO2 thermal conductivity including representative uranium and oxygen defects and fission products are carried out. These calculations employ a standard Buckingham-type interatomic potential and a potential that combines the many-body embedded-atom-method potential with Morse-Buckingham pair potentials. Potential parameters for UO2+x and ZrO2 are developed for the latter potential. Physical insights from the resonant phonon-spin-scattering mechanism due tomore »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Imperial College, London (United Kingdom)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1331270
- Alternate Identifier(s):
- OSTI ID: 1329983
- Report Number(s):
- LA-UR-16-20612
Journal ID: ISSN 2331-7019; PRAHB2; TRN: US1700115
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Applied
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 4; Journal ID: ISSN 2331-7019
- Publisher:
- American Physical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS
Citation Formats
Liu, Xiang -Yang, Cooper, Michael William D., McClellan, Kenneth James, Lashley, Jason Charles, Byler, Darrin David, Bell, B. D. C., Grimes, R. W., Stanek, Christopher Richard, and Andersson, David Anders. Molecular dynamics simulation of thermal transport in UO2 containing uranium, oxygen, and fission-product defects. United States: N. p., 2016.
Web. doi:10.1103/PhysRevApplied.6.044015.
Liu, Xiang -Yang, Cooper, Michael William D., McClellan, Kenneth James, Lashley, Jason Charles, Byler, Darrin David, Bell, B. D. C., Grimes, R. W., Stanek, Christopher Richard, & Andersson, David Anders. Molecular dynamics simulation of thermal transport in UO2 containing uranium, oxygen, and fission-product defects. United States. https://doi.org/10.1103/PhysRevApplied.6.044015
Liu, Xiang -Yang, Cooper, Michael William D., McClellan, Kenneth James, Lashley, Jason Charles, Byler, Darrin David, Bell, B. D. C., Grimes, R. W., Stanek, Christopher Richard, and Andersson, David Anders. Tue .
"Molecular dynamics simulation of thermal transport in UO2 containing uranium, oxygen, and fission-product defects". United States. https://doi.org/10.1103/PhysRevApplied.6.044015. https://www.osti.gov/servlets/purl/1331270.
@article{osti_1331270,
title = {Molecular dynamics simulation of thermal transport in UO2 containing uranium, oxygen, and fission-product defects},
author = {Liu, Xiang -Yang and Cooper, Michael William D. and McClellan, Kenneth James and Lashley, Jason Charles and Byler, Darrin David and Bell, B. D. C. and Grimes, R. W. and Stanek, Christopher Richard and Andersson, David Anders},
abstractNote = {Uranium dioxide (UO2) is the most commonly used fuel in light-water nuclear reactors and thermal conductivity controls the removal of heat produced by fission, thereby governing fuel temperature during normal and accident conditions. The use of fuel performance codes by the industry to predict operational behavior is widespread. A primary source of uncertainty in these codes is thermal conductivity, and optimized fuel utilization may be possible if existing empirical models are replaced with models that incorporate explicit thermal-conductivity-degradation mechanisms during fuel burn up. This approach is able to represent the degradation of thermal conductivity due to each individual defect type, rather than the overall burn-up measure typically used, which is not an accurate representation of the chemical or microstructure state of the fuel that actually governs thermal conductivity and other properties. To generate a mechanistic thermal conductivity model, molecular dynamics (MD) simulations of UO2 thermal conductivity including representative uranium and oxygen defects and fission products are carried out. These calculations employ a standard Buckingham-type interatomic potential and a potential that combines the many-body embedded-atom-method potential with Morse-Buckingham pair potentials. Potential parameters for UO2+x and ZrO2 are developed for the latter potential. Physical insights from the resonant phonon-spin-scattering mechanism due to spins on the magnetic uranium ions are introduced into the treatment of the MD results, with the corresponding relaxation time derived from existing experimental data. High defect scattering is predicted for Xe atoms compared to that of La and Zr ions. Uranium defects reduce the thermal conductivity more than oxygen defects. For each defect and fission product, scattering parameters are derived for application in both a Callaway model and the corresponding high-temperature model typically used in fuel-performance codes. The model is validated by comparison to low-temperature experimental measurements on single-crystal hyperstoichiometric UO2+x samples and high-temperature literature data. Furthermore, this work will enable more accurate fuel-performance simulations and will extend to new fuel types and operating conditions, all of which improve the fuel economics of nuclear energy and maintain high fuel reliability and safety.},
doi = {10.1103/PhysRevApplied.6.044015},
journal = {Physical Review Applied},
number = 4,
volume = 6,
place = {United States},
year = {Tue Oct 25 00:00:00 EDT 2016},
month = {Tue Oct 25 00:00:00 EDT 2016}
}
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