Investigation of oxygen self-diffusion in PuO2 by combining molecular dynamics with thermodynamic calculations

Saltas, V.; Chroneos, A.; Cooper, Michael William D.; Fitzpatrick, M. E.; Vallianatos, F.

doi:10.1039/C6RA24575G

Title: Investigation of oxygen self-diffusion in PuO₂ by combining molecular dynamics with thermodynamic calculations

Journal Article · Fri Jan 01 00:00:00 EST 2016 · RSC Advances

DOI:https://doi.org/10.1039/C6RA24575G· OSTI ID:1331292

Saltas, V. ^[1]; Chroneos, A. ^[2]; Cooper, Michael William D. ^[3]; Fitzpatrick, M. E. ^[4]; Vallianatos, F. ^[1]

Technological Educational Institute of Crete (Greece); UNESCO Chair on Solid Earth Physics and Geohazards Risk Reduction (Greece)
Imperial College, London (United Kingdom); Coventry Univ., Coventry (United Kingdom)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Coventry Univ., Coventry (United Kingdom)

In the present work, the defect properties of oxygen self-diffusion in PuO₂ are investigated over a wide temperature (300–1900 K) and pressure (0–10 GPa) range, by combining molecular dynamics simulations and thermodynamic calculations. Based on the well-established cBΩ thermodynamic model which connects the activation Gibbs free energy of diffusion with the bulk elastic and expansion properties, various point defect parameters such as activation enthalpy, activation entropy, and activation volume were calculated as a function of T and P. Molecular dynamics calculations provided the necessary bulk properties for the proper implementation of the thermodynamic model, in the lack of any relevant experimental data. The estimated compressibility and the thermal expansion coefficient of activation volume are found to be more than one order of magnitude greater than the corresponding values of the bulk plutonia. As a result, the diffusion mechanism is discussed in the context of the temperature and pressure dependence of the activation volume.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1331292

Report Number(s):: LA-UR-16-28070; RSCACL

Journal Information:: RSC Advances, Vol. 6, Issue 105; ISSN 2046-2069

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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