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Title: Theoretical investigation of thermodynamic stability and mobility of the oxygen vacancy in ThO 2 –UO 2 solid solutions

Abstract

The thermodynamic stability and the migration energy barriers of oxygen vacancies in ThO 2 –UO 2 solid solutions are investigated by density functional theory calculations. In pure ThO 2, the formation energy of oxygen vacancy is 7.58 eV and 1.46 eV under O rich and O poor conditions, respectively, while its migration energy barrier is 1.97 eV. The addition of UO 2 into ThO 2 significantly decreases the energetics of formation and migration of the oxygen vacancy. Among the range of UO 2-ThO 2 solid solutions studied in this work, UO 2 exhibits the lowest formation energy (5.99 eV and -0.13 eV under O rich and O poor conditions, respectively) and Th 0.25U0 .75O 2 exhibits the lowest migration energy barrier (~ 1 eV). Moreover, by considering chemical potential, the phase diagram of oxygen vacancy as a function of both temperature and oxygen partial pressure is shown, which could help to gain experimental control over oxygen vacancy concentration.

Authors:
 [1];  [1];  [2];  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. of Tennessee, Knoxville, TN (United States). Department of Materials Science and Engineering
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1163592
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 16; Journal Issue: 46; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thoria; Urania; Oxygen Vacancy

Citation Formats

Liu, B., Aidhy, D. S., Zhang, Y., and Weber, W. J. Theoretical investigation of thermodynamic stability and mobility of the oxygen vacancy in ThO2 –UO2 solid solutions. United States: N. p., 2014. Web. doi:10.1039/C4CP03660C.
Liu, B., Aidhy, D. S., Zhang, Y., & Weber, W. J. Theoretical investigation of thermodynamic stability and mobility of the oxygen vacancy in ThO2 –UO2 solid solutions. United States. doi:10.1039/C4CP03660C.
Liu, B., Aidhy, D. S., Zhang, Y., and Weber, W. J. Thu . "Theoretical investigation of thermodynamic stability and mobility of the oxygen vacancy in ThO2 –UO2 solid solutions". United States. doi:10.1039/C4CP03660C. https://www.osti.gov/servlets/purl/1163592.
@article{osti_1163592,
title = {Theoretical investigation of thermodynamic stability and mobility of the oxygen vacancy in ThO2 –UO2 solid solutions},
author = {Liu, B. and Aidhy, D. S. and Zhang, Y. and Weber, W. J.},
abstractNote = {The thermodynamic stability and the migration energy barriers of oxygen vacancies in ThO2 –UO2 solid solutions are investigated by density functional theory calculations. In pure ThO2, the formation energy of oxygen vacancy is 7.58 eV and 1.46 eV under O rich and O poor conditions, respectively, while its migration energy barrier is 1.97 eV. The addition of UO2 into ThO2 significantly decreases the energetics of formation and migration of the oxygen vacancy. Among the range of UO2-ThO2 solid solutions studied in this work, UO2 exhibits the lowest formation energy (5.99 eV and -0.13 eV under O rich and O poor conditions, respectively) and Th0.25U0.75O2 exhibits the lowest migration energy barrier (~ 1 eV). Moreover, by considering chemical potential, the phase diagram of oxygen vacancy as a function of both temperature and oxygen partial pressure is shown, which could help to gain experimental control over oxygen vacancy concentration.},
doi = {10.1039/C4CP03660C},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 46,
volume = 16,
place = {United States},
year = {Thu Oct 16 00:00:00 EDT 2014},
month = {Thu Oct 16 00:00:00 EDT 2014}
}

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