Halide/sulfide composite solid-state electrolyte for Li-anode based all-solid-state batteries

Abstract

Li2ZrCl6 (LZC) solid-state electrolytes (SSEs) have been recognized as a candidate halide SSEs for all-solid-state Li batteries (ASSLBs) with high energy density and safety due to its great compatibility with 4 V-class cathodes and low bill-of-material (BOM) cost. However, despite the benefits, the poor chemical/electrochemical stability of LZC against Li metal causes the deterioration of Li/LZC interface, which has a detrimental inhibition on Li+ transport in ASSLBs. Herein, we report a composite SSE combining by LZC and argyrodite buffer layer (Li6PS5Cl, LPSC) that prevent the unfavorable interaction between LZC and Li metal. The Li/LPSC-LZC-LPSC/Li symmetric cell stably cycles for over 1000 h at 0.3 mA/cm2 (0.15 mAh/cm2) and has a high critical current density (CCD) value of 2.1 mA/cm2 at 25 °C. Under high temperature (60 °C) which promotes the reaction between Li and LZC, symmetric cell fabricated with composite SSE also display stable cycling performance over 1200 h at 0.3 mAh/cm2. Especially, the Li/NCM ASSLBs fabricated with composite SSE exhibit a high initial coulombic efficiency, as well as superior cycling and rate performance. This simple and efficient strategy will be instrumental in the development of halide-based high-performance ASSLBs.