Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach

A new reactive force field to describe proton diffusion within the solid-oxide fuel cell material BaZrO3 has been derived. Using a quantum mechanical potential energy surface, the parameters of an interatomic potential model to describe hydroxyl groups within both pure and yttrium-doped BaZrO3 have...

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Main Authors: Raiteri, Paolo, Gale, Julian, Bussi, G.
Format: Journal Article
Published: IOP Publishing Ltd 2011
Subjects:
Online Access:http://hdl.handle.net/20.500.11937/4784
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author Raiteri, Paolo
Gale, Julian
Bussi, G.
author_facet Raiteri, Paolo
Gale, Julian
Bussi, G.
author_sort Raiteri, Paolo
building Curtin Institutional Repository
collection Online Access
description A new reactive force field to describe proton diffusion within the solid-oxide fuel cell material BaZrO3 has been derived. Using a quantum mechanical potential energy surface, the parameters of an interatomic potential model to describe hydroxyl groups within both pure and yttrium-doped BaZrO3 have been determined. Reactivity is then incorporated through the use of the empirical valence bond model. Molecular dynamics simulations (EVB-MD) have been performed to explore the diffusion of hydrogen using a stochastic thermostat and barostat whose equations are extended to the isostress-isothermal ensemble. In the low concentration limit, the presence of yttrium is found not to significantly influence the diffusivity of hydrogen, despite the proton having a longer residence time at oxygen adjacent to the dopant. This lack of in influence is due to the fact that trapping occurs infrequently, even when the proton diffuses through octahedra adjacent to the dopant. The activation energy for diffusion is found to be 0.42 eV, in good agreement with experimental values, though the prefactor is slightly underestimated.
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publishDate 2011
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spelling curtin-20.500.11937-47842017-09-13T16:01:58Z Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach Raiteri, Paolo Gale, Julian Bussi, G. proton diffusion A new reactive force field to describe proton diffusion within the solid-oxide fuel cell material BaZrO3 has been derived. Using a quantum mechanical potential energy surface, the parameters of an interatomic potential model to describe hydroxyl groups within both pure and yttrium-doped BaZrO3 have been determined. Reactivity is then incorporated through the use of the empirical valence bond model. Molecular dynamics simulations (EVB-MD) have been performed to explore the diffusion of hydrogen using a stochastic thermostat and barostat whose equations are extended to the isostress-isothermal ensemble. In the low concentration limit, the presence of yttrium is found not to significantly influence the diffusivity of hydrogen, despite the proton having a longer residence time at oxygen adjacent to the dopant. This lack of in influence is due to the fact that trapping occurs infrequently, even when the proton diffuses through octahedra adjacent to the dopant. The activation energy for diffusion is found to be 0.42 eV, in good agreement with experimental values, though the prefactor is slightly underestimated. 2011 Journal Article http://hdl.handle.net/20.500.11937/4784 10.1088/0953-8984/23/33/334213 IOP Publishing Ltd fulltext
spellingShingle proton diffusion
Raiteri, Paolo
Gale, Julian
Bussi, G.
Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach
title Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach
title_full Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach
title_fullStr Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach
title_full_unstemmed Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach
title_short Reactive force field simulation of proton diffusion in BaZrO3 using an empirical valence bond approach
title_sort reactive force field simulation of proton diffusion in bazro3 using an empirical valence bond approach
topic proton diffusion
url http://hdl.handle.net/20.500.11937/4784