Evaluation of polymorphism and charge transport in a BaO–CaO–Ta2O5 perovskite phase diagram using TOF-neutron and synchrotron X-ray diffraction, the bond-valence method and impedance spectroscopy

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dc.contributor.authorSingh, Ken_AU
dc.contributor.authorYang, Hen_AU
dc.contributor.authorZhang, Zen_AU
dc.contributor.authorAvdeev, Men_AU
dc.contributor.authorHuq, Ashfiaen_AU
dc.contributor.authorWu, DYen_AU
dc.contributor.authorLee, JJen_AU
dc.contributor.authorKan, WHen_AU
dc.contributor.authorThangadurai, Ven_AU
dc.date.accessioned2024-02-23T05:03:23Zen_AU
dc.date.available2024-02-23T05:03:23Zen_AU
dc.date.issued2022-10-26en_AU
dc.date.statistics2024-02-23en_AU
dc.description.abstractAmong the alkaline earth-based perovskite oxides, the Ba-based perovskites have superior chemical stability and tunable electrical/catalytic property via chemical substitution/doping. One of the best-known examples is Ba3Ca1.18Nb1.82O8.73 as a ceramic proton conductor for all-solid-state steam electrolysis and solid oxide fuel cells (SOFCs). Structural ordering variation is often driven by chemical composition, which directly correlates with their chemical/physical properties. In the present work, we develop a comprehensive functional perovskite-type phase diagram for the Ba–Ca–Ta–O quaternary system Ba3Ca1+xTa2−xO9−3x/2 (0 ≤ x ≤ 0.36) with a wide chemical composition between 1000 and 1550 °C, coupled with theoretical calculations to investigate the cation ordering in supercells. Furthermore, the impact of cation clustering on the diffusion pathways of O2− ions was evaluated as a case study. Experimentally, precise cation ordering and other structural features are quantitively determined by TOF-neutron and synchrotron X-ray diffraction analyses. This work provides a comprehensive evaluation of some potential applications of the Ba–Ca–Ta–O quaternary system. The electrochemical impedance data were also systematically studied by impedance spectroscopy genetic programming (ISGP). The electrical conductivity was found to increase from x = 0 to x = 0.27 and then decrease for the end member when x = 0.36 due to a decrease in mobile charge carrier concentration. Interestingly, in dry air, the electrical conductivity was found to increase from x = 0 to x = 0.36. However, only Ba3Ca1.18Ta1.82O8.73 (BCT18) and Ba3Ca1.27Ta1.73O8.595 (BCT27) were found to show an increasing trend in conductivity in humid atmospheres, and this indicates that the clustering effect was pO2 dependent. © Royal Society of Chemistry 2024en_AU
dc.description.sponsorshipW. H. K. acknowledges the very helpful discussion with Dr Kirill Okhotnikov about the Supercell program. We thank Drs Bohang Song and Melanie Kirkham at ORNL for assistance with neutron measurement. The POWGEN beamline at ORNL was sponsored by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy. W. H. K. appreciates the beamtime in ECHIDNA granted by the Australian Centre for Neutron Scattering (ACNS) in ANSTO. The Natural Sciences and Engineering Research Council of Canada (NSERC) has supported this work through Discovery Grants to V. T. (Award number RGPIN-2016-03853). V. T. and K. S. also acknowledge funding from the Canada First Research Excellence Fund (CFREF) at the University of Calgary. This work was also supported by the National Natural Science Foundation of China (11805034, U1930102 and 21704105) and Natural Science Foundation of Guangdong Province (2017A030313021).en_AU
dc.identifier.citationSingh, K., Yang, H., Zhang, Z., Avdeev, M., Huq, A., Wu, D.-Y., Lee, J.-J., Kan, W. H., & Thangadurai, V. (2022). Evaluation of polymorphism and charge transport in a BaO–CaO–Ta2O5 perovskite phase diagram using TOF-neutron and synchrotron X-ray diffraction, the bond-valence method and impedance spectroscopy [10.1039/D2TA02725A]. Journal of Materials Chemistry A, 10(41), 22257-22270. doi:10.1039/D2TA02725Aen_AU
dc.identifier.issn2050-7488en_AU
dc.identifier.issn2050-7496en_AU
dc.identifier.issue41en_AU
dc.identifier.journaltitleJournal of Materials Chemistry Aen_AU
dc.identifier.pagination22257-22270en_AU
dc.identifier.urihttp://dx.doi.org/10.1039/d2ta02725aen_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15430en_AU
dc.identifier.volume10en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherRoyal Society of Chemistry (RSC)en_AU
dc.subjectCharge transporten_AU
dc.subjectPerovskiteen_AU
dc.subjectPhase diagramsen_AU
dc.subjectNeutron diffractionen_AU
dc.subjectX-ray diffractionen_AU
dc.subjectSynchrotronsen_AU
dc.subjectValenceen_AU
dc.subjectSpectroscopyen_AU
dc.subjectOxidesen_AU
dc.titleEvaluation of polymorphism and charge transport in a BaO–CaO–Ta2O5 perovskite phase diagram using TOF-neutron and synchrotron X-ray diffraction, the bond-valence method and impedance spectroscopyen_AU
dc.typeJournal Articleen_AU
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