Abstract
Reported is an experimental and computational investigation of the low temperature heat capacity, thermodynamic functions, and thermal conductivity of stoichiometric, polycrystalline CeO2. The experimentally measured heat capacity at T < 15 K provides an important correction to the historically accepted experimental values, and the low temperature thermal conductivity serves as the most comprehensive data set at T < 400 K available. Below 10 K, the heat capacity is observed to obey the Debye T3 law, with a Debye temperature of ΘD = 455 K. The entropy, enthalpy, and Gibbs free energy functions are obtained from the experimental heat capacity and compared with predictions from Hubbard-corrected density functional perturbation theory calculations using the Perdew, Burke, and Ernzerhof parameterization revised for solids. The thermal conductivity is determined using the Maldonado continuous measurement technique, along with laser flash analysis, and analyzed according to the Klemens-Callaway model.
| Original language | English |
|---|---|
| Article number | 044202 |
| Journal | Journal of Chemical Physics |
| Volume | 151 |
| Issue number | 4 |
| DOIs | |
| State | Published - Jul 28 2019 |
Funding
The sample preparation presented here was conducted at the Los Alamos National Laboratory under the National Nuclear Security Administration Contract No. DE-AC52-06NA25396. Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energyâ™s National Nuclear Security Administration under Contract No. DE-NA0003525. The views expressed in this article do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Low-temperature experimental work in this study was supported by The Robert A. Welch Foundation (Grant No. A-0514), Houston, TX and TAMU-NSFC (Project No. 2014-30). S.O.W. and T.D.M. acknowledge support as a Welch Postdoctoral Fellow and a Welch Predoctoral Fellow, respectively, during most of this work. T.D.M. acknowledges support as a Charles F. Squire Graduate Fellow during part of this project. D.G.N. acknowledges long term research support from TRAWF. The authors would like to thank S. Banerjee for use of the Raman Spectrometer, T. E. G. Alivio and N. A. Fleer for their help performing Raman measurements, K. D. D. Rathnayaka for help with low-temperature measurements and useful discussions, and C. C. Hays, J. H. Ross, R. E. Allen, and T. Hughbanks for useful discussions. The authors are further indebted to M. Khafizov for freely sharing the data referenced in this study. The sample preparation presented here was conducted at the Los Alamos National Laboratory under the National Nuclear Security Administration Contract No. DE-AC52-06NA25396. Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under Contract No. DE-NA0003525. The views expressed in this article do not necessarily represent the views of the U.S. Department of Energy or the United States Government. Low-temperature experimental work in this study was supported by The Robert A. Welch Foundation (Grant No. A-0514), Houston, TX and TAMU-NSFC (Project No. 2014-30). S.O.W. and T.D.M. acknowledge support as a Welch Postdoctoral Fellow and a Welch Predoctoral Fellow, respectively, during most of this work. T.D.M. acknowledges support as a Charles F. Squire Graduate Fellow during part of this project. D.G.N. acknowledges long term research support from TRAWF. The authors would like to thank S. Banerjee for use of the Raman Spectrometer, T. E. G. Alivio and N. A. Fleer for their help performing Raman measurements, K. D. D. Rathnayaka for help with low-temperature measurements and useful discussions, and C. C. Hays, J. H. Ross, R. E. Allen, and T. Hughbanks for useful discussions. The authors are further indebted to M. Khafizov for freely sharing the data referenced in this study.