Preparation and properties of sulfide solid state electrolyte Li6PS5Cl by ball milling-solid phase sintering

Li6PS5Cl (LPSC), a sulfide solid-state electrolyte with an argyrodite structure, is one of the ideal electrolyte materials for the construction of all-solid-state lithium-ion batteries.It has good development prospects because of its high ionic conductivity (>3×10-3 S·cm-1) and good stability to lithium. In this work, LPSC was prepared by the combination of high-energy ball milling and inert atmosphere solid-phase sintering, and powder X-ray diffraction, Raman spectra, and scanning electron microscopy were used to investigate the effects of the preparation process on the structure, composition, electrical properties, and ion conductivity of LPSC. The results show that the extended ball milling time is beneficial to the amorphization and subsequent sintering of the LPSC precursor powder. The increase of the sintering temperature will promote the physical purity and electrical conductivity of the prepared LPSC electrolyte, but the high sintering temperature will lead to the decomposition of LPSC. The LPSC prepared by 8 h ball milling and 500℃ sintering has the highest ion/electron conductivity ratio (2.091×105) at room temperature, with ionic conductivity up to 4.049×10-3 S·cm-1 and electronic conductivity only 1.936×10-8 S·cm-1. The 712 NCM/LPSC/In-Li all-solid-state battery prepared with this electrolyte has a first-turn discharge specific capacity of 151.3 mAh·g-1 at a charge/discharge ratio of 0.1 C, and has excellent cycling stability.