Li–Solid Electrolyte Interfaces/Interphases in All-Solid-State Li Batteries

Abstract The emergence of all-solid-state Li batteries (ASSLBs) represents a promising avenue to address critical concerns like safety and energy density limitations inherent in current Li-ion batteries. Solid electrolytes (SEs) show significant potential in curtailing Li dendrite intrusion, acting as natural barriers against short circuits. However, the substantial challenges at the SEs−electrode interface, particularly concerning the anode, pose significant impediments to the practical implementation of ASSLBs. This review aims to delineate the most viable strategies for overcoming anode interfacial hurdles across four distinct categories of SEs: sulfide SEs, oxide SEs, polymer SEs, and halide SEs. Initially, pivotal issues such as anode interfacial side reactions, inadequate physical contact, and Li dendrite formation are comprehensively outlined. Furthermore, effective methodologies aimed at enhancing anode interfacial stability are expounded, encompassing approaches like solid electrolyte interface (SEI) interlayer insertion, SE optimization, and the adoption of Li alloy in lieu of Li metal, each tailored to specific SE categories. Moreover, this review presents novel insights into fostering interfaces between diverse SE types and Li anodes, while also advocating perspectives and recommendations for the future advancement of ASSLBs. Graphical Abstract