One-pot aprotic solvent-enabled synthesis of superionic Li-argyrodite solid electrolyte

Abstract

Li-argyrodite phase Li6PS5Cl is a promising solid electrolyte (SE) with potential applications in all-solid-state batteries (ASSBs). Conventional SE synthesis methods such as high-energy ball-milling and solid-state synthesis require a significant amount of energy. Consequently, in recent years, several studies have been conducted on developing liquid phase methods for mass-producing SEs. One such liquid phase method uses tetrahydrofuran (THF, an aprotic solvent) and ethanol (EtOH, a protic solvent) to synthesize Li6PS5Cl. However, the synthesized SE contains impurities that are generated by reactions between EtOH and PS43-. In this study, we present a novel one-pot liquid phase method for synthesizing Li6PS5Cl using THF. The synthesized SE had a high ionic conductivity (2.03 mS center dot cm(-1)) and low electronic conductivity (7.44 x 10(-8) S center dot cm(-1)). Notably, it had few impurities and was essentially composed of a single phase. Furthermore, an ASSB cell composed of LiNbO3-coated LiNi0.6Mn0.2CoO2 (NMC622)/Li6PS5Cl/Li-In, which contained the synthesized SE, exhibited a high discharge capacity of 156 mAh center dot g(-1). Therefore, the liquid phase method proposed herein can be used to synthesize SEs, and can help realize mass production and commercialization.