Synthesis and characterization of argyrodite solid electrolytes for all-solid-state Li-ion batteries

Li6PS5X (X = Cl, Br, I) argyrodites possess high ionic conductivity but with rather scattered values due to various processing conditions. In this work, Li6PS5X solid electrolytes were prepared by solid-state sintering or mechanical alloying and optimized with or without excess Li2S. Solid-state sintering prefers excess Li2S, whereas mechanical alloying prefers stoichiometric Li2S to synthesize high-purity samples with high ionic conductivity. Solid-state sintering is also more suitable than mechanical milling for high ionic conductivity. Li6PS5Cl with the highest ionic conductivity among Li6PS5X was comprehensively characterized for electrochemical performance and air stability. MoS2/Li6PS5Cl all-solid-state batteries assembled with Li6PS5Cl-coated MoS2 as cathode and with Li6PS5Cl as solid electrolyte demonstrate high capacity and good cycling stability.