All-solid-state lithium-metal batteries (ASSLMBs) with sulfide electrolytes have attracted attention owing to their superior safety and high energy density. However, interfacial instability of sulfide electrolytes against Li metal still hinders their applications. Herein, F-doping is adopted to optimize the structure of LiSnPS. It is demonstrated that the LiSnPSF (LSPSF) electrolyte exhibits a high ionic conductivity of 6.4 mS cm because of F-doping, which can reduce the impurity LiSnS and generate Li vacancies. In addition, the LiPSI (LPSI) glass-ceramic interlayer is employed to enhance the interfacial stability between the sulfide electrolyte and Li metal by restraining the reduction of Sn cations, as indicated by X-ray photoelectron spectroscopy (XPS). As a result, the assembled ASSLMBs with the LPSI interlayer deliver high initial discharge capacity and remarkable cycling stability. This work provides a new design route for manufacturing high-performance ASSLMBs.
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