Toward High Performance All‐Solid‐State Lithium Batteries with High‐Voltage Cathode Materials: Design Strategies for Solid Electrolytes, Cathode Interfaces, and Composite Electrodes

Abstract All‐solid‐state lithium batteries (ASSLBs) with nonflammable solid electrolytes (SEs) deliver greatly enhanced safety characteristics. Furthermore, ASSLBs composed of cathodes with high working voltages, such as LiCoO 2 , LiNi x Co y Mn z O 2 ( x + y + z = 1, NCM), LiNi x Co y Al z O 2 ( x + y + z = 1, NCA), LiMn x Fe y PO 4 ( x + y = 1, LMFP), and LiNi 0.5 Mn 1.5 O 4 (LNMO), and a lithium metal anode can achieve comparable or better performance compared with that of LLBs in terms of energy density. Therefore, high‐voltage ASSLBs have been regarded as the most promising next‐generation batteries. Although significant progress has been achieved in high‐voltage ASSLBs research, their development still faces multiple challenges. To facilitate further effective and target‐oriented research on high‐voltage ASSLBs, a summary of recent research progress is urgently needed. In this review, recent research progress in high‐voltage ASSLBs is summarized from the perspectives of SEs modification, interfacial challenges and their corresponding solutions for cathodes, and high‐voltage composite cathode design for practical applications. Finally, the authors’ perspectives on the state of current ASSLBs research, aiming to propose possible research directions for the future development of high‐voltage ASSLBs.