Effect of long- and short-range disorder on the oxygen ionic conductivity of Tm2(Ti2–xTmx)O7–x/2 “stuffed” pyrochlores

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dc.contributor.authorMullens, BGen_AU
dc.contributor.authorZhang, Zen_AU
dc.contributor.authorAvdeev, Men_AU
dc.contributor.authorBrand, HEAen_AU
dc.contributor.authorCowie, BCCen_AU
dc.contributor.authorMúzquiz, MSen_AU
dc.contributor.authorKennedy, BJen_AU
dc.date.accessioned2021-09-13T22:27:57Zen_AU
dc.date.available2021-09-13T22:27:57Zen_AU
dc.date.issued2021-03-10en_AU
dc.date.statistics2021-09-07en_AU
dc.description.abstractThe long-range average and short-range local structures in the Tm2(Ti2–xTmx)O7–x/2 (x = 0.00–0.67) series were studied using a combination of diffraction and spectroscopic techniques. The long-range average structure, established from synchrotron X-ray and neutron powder diffraction data, shows the development of multiphase regions from x = 0.134 and the formation of antisite cation disorder from x = 0.402. The crystal field splitting of the Ti4+ ions, as derived from the Ti L3-edge X-ray absorption near-edge structure (XANES) spectroscopy, decreases gradually from 2.17 to 1.92 eV with increasing Tm3+ content (x), reflecting the increase in coordination number from 6 to predominantly 7. This is consistent with a gradual evolution of the short-range local disorder from x = 0.00 to 0.67. These results suggest that local disorder develops gradually throughout the entire composition range, whereas changes in the long-range disorder occur more suddenly. Electrochemical impedance spectroscopic results show an increase in oxygen ionic conductivity at 1000 °C, by a factor of 4 upon doping at x = 0.268. This suggests that inducing small amounts of disorder into the pyrochlore structure, by stuffing, may lead to applications of this material as a solid electrolyte in solid-oxide fuel cells. © 2021 American Chemical Societyen_AU
dc.identifier.citationMullens, B. G., Zhang, Z., Avdeev, M., Brand, H. E. A., Cowie, B. C. C., Múzquiz, M. S., & Kennedy, B. J. (2021). Effect of long- and short-range disorder on the oxygen ionic conductivity of Tm2(Ti2–xTmx)O7–x/2 “stuffed” pyrochlores. Inorganic Chemistry, 60(7), 4517–4530. doi:10.1021/acs.inorgchem.0c03363en_AU
dc.identifier.issn1520-510Xen_AU
dc.identifier.issue7en_AU
dc.identifier.journaltitleInorganic Chemistryen_AU
dc.identifier.pagination4517-4530en_AU
dc.identifier.urihttps://doi.org/10.1021/acs.inorgchem.0c03363en_AU
dc.identifier.urihttps://apo.ansto.gov.au/dspace/handle/10238/11685en_AU
dc.identifier.volume60en_AU
dc.language.isoenen_AU
dc.publisherAmerican Chemical Societyen_AU
dc.subjectNeutron diffractionen_AU
dc.subjectX-ray diffractionen_AU
dc.subjectCrystal fielden_AU
dc.subjectElectrochemistryen_AU
dc.subjectImpedanceen_AU
dc.subjectPyrochloreen_AU
dc.titleEffect of long- and short-range disorder on the oxygen ionic conductivity of Tm2(Ti2–xTmx)O7–x/2 “stuffed” pyrochloresen_AU
dc.typeJournal Articleen_AU
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