Strategies Toward Stable Anode Interface for Sulfide‐Based All‐Solid‐State Lithium Metal Batteries

Abstract Sulfide‐based all‐solid‐state batteries (ASSBs) have ushered in a new era of energy storage technology, offering the tantalizing prospect of unprecedented energy density and safety. However, the poor electrode‐electrolyte interface between Li anodes and sulfide solid electrolytes has hindered its practical application. In this review, the primary focus lies in the current fundamental understanding, challenges, and optimization strategies regarding the interface chemistries between sulfide solid electrolytes and Li anode. First, an in‐depth discussion is conducted and provides a detailed summary of the interfacial challenges that exist between the Li anode and sulfide solid electrolytes. Among these challenges, poor interfacial compatibility and stability stand out as the two crucial issues. Subsequently, effective approaches are systematically explored to surmount these issues. These encompass the component optimization and structural design of the bulk anode, doping and coating strategies of the sulfide solid electrolytes, and interface design between the Li anode and sulfide solid electrolytes. Finally, the insights are present into the limitations of current studies, perspectives, and recommendations for the further development of sulfide‐based solid‐state batteries, aiming to offer a comprehensive and enlightening overview for interface engineering, which is of great significance for the integration of applicable all‐solid‐state Li metal batteries (ASSLMBs).