Calcium substitution to improve the total ionic conductivity of the Li3/8Sr7/16Ta3/4Hf1/4O3 perovskite-type electrolyte

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dc.contributor.authorBertrand, Men_AU
dc.contributor.authorGroleau, Len_AU
dc.contributor.authorBibienne, Ten_AU
dc.contributor.authorRousselot, Sen_AU
dc.contributor.authorLiu, Xen_AU
dc.contributor.authorChi, Men_AU
dc.contributor.authorYang, FZTen_AU
dc.contributor.authorPeterson, VKen_AU
dc.contributor.authorSchmid, Sen_AU
dc.contributor.authorDollé, Men_AU
dc.date.accessioned2024-11-15T04:06:02Zen_AU
dc.date.available2024-11-15T04:06:02Zen_AU
dc.date.issued2023-11-01en_AU
dc.date.statistics2024-11-08en_AU
dc.description.abstractWe report novel calcium-substituted perovskite-type solid state electrolyte with nominal composition Li0.344Sr0.433Ca0.02Ta3/4Hf1/4O3, which we compare with Li3/8Sr7/16Ta3/4Hf1/4O3. The compounds were synthesized via solid-state reaction and studied by X-ray and neutron powder diffraction and electrochemical impedance spectroscopy. Neutron powder diffraction allowed the Li position in the structure to be accurately determined. Calcium-substituted phase showed higher Li-ion conductivity than the analogous calcium-free phase obtained with our synthesis method. High total Li-ion conductivities of 3.6 ± 1.0 × 10−4 S cm−1 (Ea = 431 meV) at 30 °C were reached for calcium-substituted phase, and both bulk and grain-boundary conductivities increased compared to that of the calcium-free phase. The same experiment was conducted on Li0.344Sr0.433Ca0.02Ta3/4Zr1/4O3 and led to the same conclusion compared to Li3/8Sr7/16Ta3/4Zr1/4O3. Elemental analysis by energy-dispersive X-ray (EDX) of Li0.344Sr0.433Ca0.02Ta3/4Hf1/4O3 showed the formation of an intermediary phase at grain boundaries, which contained essentially strontium, calcium, and oxygen. To better understand the increased bulk conductivity, neutron diffraction was performed on Li0.344Sr0.433Ca0.02Ta3/4Hf1/4O3. The results demonstrate the importance of understanding and controlling the grain boundary composition, as much as the bulk composition, to improve the total ionic conductivity of solid electrolytes. © 2023 Elsevier B.V. All rights reserved.en_AU
dc.description.sponsorshipL.G., M.B., T.B., S.R. and M.D. acknowledge the financial support from Natural Sciences and Engineering Research Council of Canada (NSERC) (project RGPIN-2015-05393 and RDCPJ 528052-18). Dr. David Lepage is acknowledged for his valuable comments, which helped us to improve the manuscript. Electron microscopy study was performed at ORNL's Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.en_AU
dc.identifier.articlenumber116324en_AU
dc.identifier.citationBertrand, M., Groleau, L., Bibienne, T., Rousselot, S., Liu, X., Chi, M., Yang, F. Z. T., Peterson, V. K., Schmid, S., & Dollé, M. (2023). Calcium substitution to improve the total ionic conductivity of the Li3/8Sr7/16Ta3/4Hf1/4O3 perovskite-type electrolyte. Solid State Ionics, 400, 116324. doi:10.1016/j.ssi.2023.116324en_AU
dc.identifier.issn0167-2738en_AU
dc.identifier.journaltitleSolid State Ionicsen_AU
dc.identifier.urihttps://doi.org/10.1016/j.ssi.2023.116324en_AU
dc.identifier.urihttps://apo.ansto.gov.au/handle/10238/15759en_AU
dc.identifier.volume400en_AU
dc.languageEnglishen_AU
dc.language.isoenen_AU
dc.publisherElsevieren_AU
dc.subjectCalciumen_AU
dc.subjectIonic conductivityen_AU
dc.subjectPerovskiteen_AU
dc.subjectElectrolytesen_AU
dc.subjectHafniumen_AU
dc.subjectTantalumen_AU
dc.subjectStrontiumen_AU
dc.subjectLithiumen_AU
dc.subjectNeutron diffractionen_AU
dc.subjectSolid state physicsen_AU
dc.subjectElectrochemistryen_AU
dc.subjectSpectroscopyen_AU
dc.titleCalcium substitution to improve the total ionic conductivity of the Li3/8Sr7/16Ta3/4Hf1/4O3 perovskite-type electrolyteen_AU
dc.typeJournal Articleen_AU
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