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dc.contributor.authorHeywood, Stephen
dc.contributor.authorLessmeier, Matt
dc.contributor.authorDriscoll, David
dc.contributor.authorSofie, Stephen
dc.identifier.citationHeywood S, LessmeierM, Driscoll D, Sofie S. Tailoring solid-statesynthesis routes for high confidence production ofphase pure, low impedance Al-LLZO. J Am CeramSoc. 2023;1–11.
dc.descriptionThis is the peer reviewed version of the following article: [Tailoring solid‐state synthesis routes for high confidence production of phase pure, low impedance Al‐LLZO. Journal of the American Ceramic Society (2023)], which has been published in final form at This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions:
dc.description.abstractLithium lanthanum zirconium oxide (LLZO) garnet is a solid-state lithium ion conducting electrolyte promising all-solid-state batteries (ASSB) with high charge rates and good energy density due to its chemical stability against lithium metal anodes. LLZO has a high room temperature Li ion conductivity of ∼0.1–1 mS/cm in its cubic phase, but the stability of the cubic phase and ionic conductivity are highly sensitive to lithium stoichiometry. Stabilizing agents such as aluminum oxide and excess lithium are needed to preserve the cubic phase and compensate for lithium volatility. With the range of the end LLZO products spanning powders, porous membranes to dense membranes combined with sintering/calcination that often exceeds 1000°C, it is challenging to maintain an ideal lithium content given its high volatility from a single base powder. This study was designed to elucidate the sensitivities of aluminum doped LLZO powder synthesis and processing along its path to being utilized in a ceramic-manufacturing optimized ASSB. By utilizing thermogravimetric analysis in conjunction with in situ X-ray diffraction analysis of solid-state LLZO synthesis, it was discovered that the sensitivity of the LLZO cubic phase to lithium volatility can be reduced via early incorporation of excess lithium carbonate during initial phase formation in direct combination with controlled surface-to-volume ratios of the powders. Isostatically pressed powders of our LLZO sintered at 1100°C for 2 h showed RT ionic conductivity of 0.3–0.4 mS/cm measured via electrochemical impedance spectroscopy, and an improvement in microstructural uniformity with lowered porosity. The improved suppression of lithium volatilization has important implications for the scalable production of LLZO powders and assembly of ASSBs.en_US
dc.rightscopyright Wiley 2023en_US
dc.subjectionic conductivityen_US
dc.subjectlithium oxideen_US
dc.titleTailoring solid‐state synthesis routes for high confidence production of phase pure, low impedance Al‐LLZOen_US
mus.citation.journaltitleJournal of the American Ceramic Societyen_US
mus.relation.collegeCollege of Engineeringen_US
mus.relation.departmentMechanical & Industrial Engineering.en_US
mus.relation.universityMontana State University - Bozemanen_US

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