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Mechanism of carbon dioxide and water incorporation in Ba2TiO4: A joint computational and experimental study

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journal contribution
posted on 19.03.2018, 13:42 authored by Adam J. McSloy, Ivan Trussov, Abbey Jarvis, David J. Cooke, Peter R. Slater, Pooja GoddardPooja Goddard
© 2017 American Chemical Society. CO 2 incorporation in solids is attracting considerable interest in a range of energy-related areas. Materials degradation through CO 2 incorporation is also a critical problem with some fuel cell materials, particularly for proton conducting ceramic fuel cells. Despite this importance, the fundamental understanding of the mechanism of CO 2 incorporation is lacking. Furthermore, the growing use of lower temperature sol gel routes for the design and synthesis of new functional materials may be unwittingly introducing significant residual carbonate and hydroxyl ions into the material, and so studies such as the one reported here investigating the incorporation of carbonate and hydroxyl ions are important, to help explain how this may affect the structure and properties. This study on Ba 2 TiO 4 suggests highly unfavorable intrinsic defect formation energies but comparatively low H 2 O and CO 2 incorporation energies, in accord with experimental findings. Carbonate defects are likely to form in both pristine and undoped Ba 2 TiO 4 systems, whereas those based on H 2 O will only form in systems containing other supporting defects, such as oxygen interstitials or vacancies. However, both hydroxyl and carbonate defects will trap oxide ion defects induced through doping, and the results from both experimental and modeling studies suggest that it is primarily the presence of carbonate that is responsible for stabilizing the high temperature α′-phase at lower temperatures.


This paper recognises the use of the ’Hydra’ High Performance System at Loughborough University. Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202), this work used the ARCHER UK National Supercomputing Service (http://www.archer.ac.uk)



  • Science


  • Chemistry

Published in

Journal of Physical Chemistry C






1061 - 1069


MCSLOY, A.J. ...et al., 2018. Mechanism of carbon dioxide and water incorporation in Ba2TiO4: A joint computational and experimental study. Journal of Physical Chemistry C, 122(2), pp. 1061-1069.


© American Chemical Society (ACS)


AM (Accepted Manuscript)

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This work is made available according to the conditions of the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0) licence. Full details of this licence are available at: https://creativecommons.org/licenses/by-nc-nd/4.0/

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This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcc.7b10330