New insights into phase distribution, phase composition and disorder in Y2(Zr,Sn)2O7 ceramics from NMR spectroscopy

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dc.contributor.authorAshbrook, SEen_AU
dc.contributor.authorMitchell, MRen_AU
dc.contributor.authorSneddon, Sen_AU
dc.contributor.authorMoran, RFen_AU
dc.contributor.authorde los Reyes, Men_AU
dc.contributor.authorLumpkin, GRen_AU
dc.contributor.authorWhittle, KRen_AU
dc.date.accessioned2017-04-03T06:52:36Zen_AU
dc.date.available2017-04-03T06:52:36Zen_AU
dc.date.issued2015-03-02en_AU
dc.date.statistics2017-04-03en_AU
dc.description.abstractA combination of 89Y and 119Sn NMR spectroscopy and DFT calculations are used to investigate phase evolution, local structure and disorder in Y2Zr2−xSnxO7 ceramics, where a phase change is predicted, from pyrochlore to defect fluorite, with increasing Zr content. The ability of NMR to effectively probe materials that exhibit positional and compositional disorder provides insight into the atomic-scale structure in both ordered and disordered phases and, by exploiting the quantitative nature of the technique, we are able to determine detailed information on the composition of the phase(s) present and the average coordination number (and next-nearest neighbour environment) of the cations. In contrast to previous studies, a more complex picture of the phase variation with composition emerges, with single-phase pyrochlore found only for the Sn end member, and a single defect fluorite phase only for x = 0 to 0.6. A broad two-phase region is observed, from x = 1.8 to 0.8, but the two phases present have very different composition, with a maximum of 13% Zr incorporated into the pyrochlore phase, whereas the composition of the defect fluorite phase varies throughout. Preferential ordering of the anion vacancies in the defect fluorite phase is observed, with Sn only ever found in a six-coordinate environment, while remaining vacancies are shown to be more likely to be associated with Zr than Y. Our findings are then discussed in the light of those from previous studies, many of which utilize diffraction-based approaches, where, in most cases, a single phase of fixed composition has been assumed for the refinement procedure. The significant and surprising differences encountered demonstrate the need for complementary approaches to be considered for a detailed and accurate picture of both the long- and short-range structure of a solid to be achieved. © Royal Society of Chemistry 2017en_AU
dc.identifier.citationAshbrook, S. E., Mitchell, M. R., Sneddon, S., Moran, R. F., de los Reyes, M., Lumpkin, G. R., & Whittle, K. R. (2015). New insights into phase distribution, phase composition and disorder in Y2(Zr,Sn)2O7 ceramics from NMR spectroscopy. Physical Chemistry Chemical Physics, 17(14), 9049-9059. doi:10.1039/C4CP05827Een_AU
dc.identifier.govdoc8070en_AU
dc.identifier.issn1463-9076en_AU
dc.identifier.issue14en_AU
dc.identifier.journaltitlePhysical Chemistry Chemical Physicsen_AU
dc.identifier.pagination9049-9059en_AU
dc.identifier.urihttp://dx.doi.org/10.1039/C4CP05827Een_AU
dc.identifier.urihttp://apo.ansto.gov.au/dspace/handle/10238/8526en_AU
dc.identifier.volume17en_AU
dc.language.isoenen_AU
dc.publisherRoyal Society of Chemistryen_AU
dc.subjectSpectroscopyen_AU
dc.subjectCeramicsen_AU
dc.subjectPyrochloreen_AU
dc.subjectFluoriteen_AU
dc.subjectVariationsen_AU
dc.subjectZirconiumen_AU
dc.titleNew insights into phase distribution, phase composition and disorder in Y2(Zr,Sn)2O7 ceramics from NMR spectroscopyen_AU
dc.typeJournal Articleen_AU
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