@article{4354f0732f6040edade9335080fe9729,
title = "Structural dynamics of Schottky and Frenkel defects in CeO2: a density-functional theory study",
abstract = "Cerium dioxide CeO 2 (ceria) is an important material in catalysis and energy applications. The intrinsic Frenkel and Schottky defects can impact a wide range of material properties including the oxygen storage capacity, the redox cycle, and the ionic and thermal transport. Here, we study the impact of Frenkel and Schottky defects on the structural dynamics and thermal properties of ceria using density functional theory. The phonon contributions to the free energy are found to reduce the defect formation free energies at elevated temperature. The phonon dispersions of defective CeO 2 show significant broadening of the main branches compared to stoichiometric ceria. Phonon modes associated with the defects are identifiable in the infrared spectra through characteristic shoulders on the main features of the stoichiometric fluorite structure.",
keywords = "structural dynamics, thermal conductivity, nuclear fuel, cerium dioxide, defects, density functional theory (DFT)",
author = "Thomas Smith and Samuel Moxon and Tse, {Joshua S} and Skelton, {Jonathan M} and Cooke, {David J} and Gillie, {Lisa J} and {Da silva}, {E Lora} and Harker, {Robert M} and Storr, {Mark T} and Parker, {Stephen C} and Marco Molinari",
note = "Funding Information: T S and M M acknowledge the University of Huddersfield EPSRC-DTP 2018-19 (EP/R513234/1) for funding. J M S is supported by a UK Research and Innovation Future Leaders Fellowship (MR/T043121/1) and previously held a University of Manchester Presidential Fellowship. E L d S acknowledges the Network of Extreme Conditions Laboratories (NECL), financed by FCT and co-financed by NORTE 2020, through the Portugal 2020 and FEDER programmes. Simulations were performed on the ARCHER and ARCHER2 UK national supercomputing services via our membership of the UK HEC Materials Chemistry Consortium (MCC), which is funded by the UK Engineering and Physical Sciences Research Council (EPSRC EP/L000202, EP/R029431). Analysis was performed using the Orion computing facility at the University of Huddersfield (UoH). We would like to acknowledge computing time granted through the EU PRACE DECI-16 Project 16DECI0044/SDAnOx. To the extent that this paper relies on the contribution of RMH/MTS, then copyright in said contribution rests with the {\textcopyright}British Crown Copyright 2020/AWE. Funding Information: T S and M M acknowledge the University of Huddersfield EPSRC-DTP 2018–19 (EP/R513234/1) for funding. J M S is supported by a UK Research and Innovation Future Leaders Fellowship (MR/T043121/1) and previously held a University of Manchester Presidential Fellowship. E L d S acknowledges the Network of Extreme Conditions Laboratories (NECL), financed by FCT and co-financed by NORTE 2020, through the Portugal 2020 and FEDER programmes. Simulations were performed on the ARCHER and ARCHER2 UK national supercomputing services via our membership of the UK HEC Materials Chemistry Consortium (MCC), which is funded by the UK Engineering and Physical Sciences Research Council (EPSRC EP/L000202, EP/R029431). Analysis was performed using the Orion computing facility at the University of Huddersfield (UoH). We would like to acknowledge computing time granted through the EU PRACE DECI-16 Project 16DECI0044/SDAnO . To the extent that this paper relies on the contribution of RMH/MTS, then copyright in said contribution rests with the {\textcopyright}British Crown Copyright 2020/AWE. x Publisher Copyright: {\textcopyright} 2023 The Author(s). Published by IOP Publishing Ltd.",
year = "2023",
month = apr,
day = "1",
doi = "10.1088/2515-7655/acbb29",
language = "English",
volume = "5",
journal = "JPhys Energy",
issn = "2515-7655",
publisher = "Institute of Physics Publishing Ltd.",
number = "2",
}