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Tantalum‐doped lithium lanthanum zirconate garnet (Li7−
x La3Zr2−x Tax O12[LLZTO]) has received interest as a solid electrolyte for solid‐state lithium batteries due to its good electrochemical properties and ionic conductivity. However, the source of discrepancies for reported values of ionic conductivity in nominally or nearly equivalent compositions of LLZTO is not completely clear. Herein, synthesis‐related factors that may contribute to the differences in performance of garnet electrolytes are systematically characterized. The conductivity of samples with composition Li6.4La3Zr1.4Ta0.6O12prepared by various methods including solid‐state reaction (SSR), combustion, and molten salt synthesis is compared. Varying levels of elemental inhomogeneity, comprising a variation in Ta and Zr content on the level of individual LLZTO particles, are identified. The elemental inhomogeneity is found to be largely preserved even after high‐temperature sintering and correlated with reduced ionic conductivity. It is shown that the various synthesis and processing‐related variables in each of the preparation methods play a role in these compositional variations, and that even LLZTO synthesized via conventional, high‐temperature SSR can exhibit substantial variability in local composition. However, by improving reagent mixing and using LLZTO powder with low agglomeration and small particle size distribution, the compositional uniformity, and hence, ionic conductivity, of sintered garnet electrolytes can be improved. -
null (Ed.)Lithium conducting garnets are attractive solid electrolytes for solid-state lithium batteries but are difficult to process, generally requiring high reaction and sintering temperatures with long durations. In this work, we demonstrate a synthetic route to obtain Ta-doped garnet (Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 ) utilizing La- and Ta-doped lanthanum zirconate (La 2.4 Zr 1.12 Ta 0.48 O 7.04 ) pyrochlore nanocrystals as quasi-single-source precursors. Via molten salt synthesis (MSS) in a highly basic flux, the pyrochlore nanocrystals transform to Li-garnet at reaction temperatures as low as 400 °C. We also show that the pyrochlore-to-garnet conversion can take place in one step using reactive sintering, resulting in densified garnet ceramics with high ionic conductivity (0.53 mS cm −1 at 21 °C) and relative density (up to 94.7%). This approach opens new avenues for lower temperature synthesis of lithium garnets using a quasi-single-source precursor and provides an alternative route to highly dense garnet solid electrolytes without requiring advanced sintering processes.more » « less
