Owing to their high Li conductivities, mechanical sinterability, and solution processability, sulfide Li argyrodites have attracted much attention as enablers in the development of high-performance all-solid-state batteries with practicability. However, solution-processable Li argyrodites have been developed only for a composition of LiPSX (X = Cl, Br, I) with insufficiently high Li conductivities (∼10 S cm). Herein, we report the highest Li conductivity of 0.54 mS cm at 30 °C (LiPGeSI) for solution-processable iodine-based Li argyrodites. A comparative investigation of three iodine-based argyrodites of unsubstituted and Ge- and Sn-substituted solution-processed LiPSI with varied heat-treatment temperature elucidates the effect of microstructural evolution on Li conductivity. Notably, local nanostructures consisting of argyrodite nanocrystallites in solution-processed LiPGeSI have been directly captured by cryogenic transmission electron microscopy, which is a first for sulfide solid electrolyte materials. Specifically, the promising electrochemical performances of all-solid-state batteries at 30 °C employing LiCoO electrodes tailored by the infiltration of LiPGeSI-ethanol solutions are successfully demonstrated.

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http://dx.doi.org/10.1021/acs.nanolett.0c01028DOI Listing

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