During reactor operation, nuclear fuels are subject to extreme temperature and irradiation conditions which can significantly degrade the fuel's thermal transport properties. The reduction in thermal conductivity of the fuel as a result of irradiation-induced lattice defects is arguably the most important fuel performance metric in regard to reactor efficiency and safety. Because thorium dioxide (ThO2) is suitable as a model system for more complex materials such as UO2 and its mixed oxides, we present a theoretical investigation of thermal conductivity reduction seen in defect-bearing thorium dioxide and compare directly to experimental measurements. Phonon-mediated thermal transport of the fuel is modeled by a solution to the Boltzmann transport equation (BTE) for phonons. A cluster dynamics (CD) model for lattice defect evolution during irradiation predicts defect densities which are used as input to the BTE for modeling phonon-defect scatterings. Phonon scatterings by lattice defects include those from point defects and vacancy clusters and interstitial clusters of various sizes. The CD model is benchmarked against structural defect characterization of irradiated thorium dioxide using electron microscopy. Thermal conductivity predicted by the BTE model is compared to measured values for irradiated thorium dioxide specimens below room temperature to isolate effects of phonon-defect scattering from intrinsic 3-phonon processes, which dominate at higher temperatures. The computed conductivity values are in partial agreement at temperatures close to room temperature while slight deviations are observed at the lowest measured temperatures, suggesting that implemented phonon-defect scattering cross-section expressions may not be adequate for low temperatures. The presented work provides a necessary investigation of the influence of irradiation induced defects on fuel performance and represents a first step toward a full characterization of phonon mediated thermal transport in irradiated materials with complex defect microstructure.
Deskins, Walter Ryan, et al. "A combined theoretical-experimental investigation of thermal transport in low-dose irradiated thorium dioxide." Acta Materialia, vol. 241, no. 118379, Nov. 2022. https://doi.org/10.1016/j.actamat.2022.118379
Deskins, Walter Ryan, Mazumder, Sanjoy, Dennett, Cody A., et al., "A combined theoretical-experimental investigation of thermal transport in low-dose irradiated thorium dioxide," Acta Materialia 241, no. 118379 (2022), https://doi.org/10.1016/j.actamat.2022.118379
@article{osti_1891505,
author = {Deskins, Walter Ryan and Mazumder, Sanjoy and Dennett, Cody A. and Bawane, Kaustubh Krishna and Hua, Zilong and Ferrigno, Joshua and He, Lingfeng and Mann, J. Matthew and Khafizov, Marat and Hurley, David H and others},
title = {A combined theoretical-experimental investigation of thermal transport in low-dose irradiated thorium dioxide},
annote = {During reactor operation, nuclear fuels are subject to extreme temperature and irradiation conditions which can significantly degrade the fuel's thermal transport properties. The reduction in thermal conductivity of the fuel as a result of irradiation-induced lattice defects is arguably the most important fuel performance metric in regard to reactor efficiency and safety. Because thorium dioxide (ThO2) is suitable as a model system for more complex materials such as UO2 and its mixed oxides, we present a theoretical investigation of thermal conductivity reduction seen in defect-bearing thorium dioxide and compare directly to experimental measurements. Phonon-mediated thermal transport of the fuel is modeled by a solution to the Boltzmann transport equation (BTE) for phonons. A cluster dynamics (CD) model for lattice defect evolution during irradiation predicts defect densities which are used as input to the BTE for modeling phonon-defect scatterings. Phonon scatterings by lattice defects include those from point defects and vacancy clusters and interstitial clusters of various sizes. The CD model is benchmarked against structural defect characterization of irradiated thorium dioxide using electron microscopy. Thermal conductivity predicted by the BTE model is compared to measured values for irradiated thorium dioxide specimens below room temperature to isolate effects of phonon-defect scattering from intrinsic 3-phonon processes, which dominate at higher temperatures. The computed conductivity values are in partial agreement at temperatures close to room temperature while slight deviations are observed at the lowest measured temperatures, suggesting that implemented phonon-defect scattering cross-section expressions may not be adequate for low temperatures. The presented work provides a necessary investigation of the influence of irradiation induced defects on fuel performance and represents a first step toward a full characterization of phonon mediated thermal transport in irradiated materials with complex defect microstructure.},
doi = {10.1016/j.actamat.2022.118379},
url = {https://www.osti.gov/biblio/1891505},
journal = {Acta Materialia},
issn = {ISSN 1359-6454},
number = {118379},
volume = {241},
place = {United States},
year = {2022},
month = {11}}
Ziegler, James F.; Ziegler, M. D.; Biersack, J. P.
Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12https://doi.org/10.1016/j.nimb.2010.02.091