High Performance All‐Solid‐State Lithium Batteries: Interface Regulation Mechanism

Abstract All‐solid‐state lithium batteries (ASSLBs) can overcome many problems in cathode and lithium anode, and it is a very promising safe secondary battery. However, unstable interface problems between electrolyte and electrode and within the electrolyte still restrict its commercial development. Herein, the interface problems are first revealed in ASSLBs and highlight the need to deeply explore the intrinsic failure mechanisms to solve these problems. Subsequently, the three failure mechanisms of ASSLBs: chemical, electrical, and electrochemical failure are broken down, and focus on the impact of the space charge layer problem on the cathode‐electrolyte interface. The effect of the anode physical contact problem on the anode‐electrolyte interface is discussed. Then, recent advances in ASSLBs, cathode and anode interface optimization strategies, and their corresponding electrochemical properties are discussed. Finally, the interface challenges faced by ASSLBs and feasible interface modification strategies are summarized, which provide references for subsequent studies and insights into the design of interface structures for the new generation of high‐performance ASSLBs.