Accelerating the Development of LLZO in Solid-State Batteries Toward Commercialization: A Comprehensive Review.

Solid-state batteries (SSBs) are under development as high-priority technologies for safe and energy-dense next-generation electrochemical energy storage systems operating over a wide temperature range. Solid-state electrolytes (SSEs) exhibit high thermal stability and, in some cases, the ability to prevent dendrite growth through a physical barrier, and compatibility with the "holy grail" metallic lithium. These unique advantages of SSEs have spurred significant research interests during the last decade. Garnet-type SSEs, that is, LiLaZrO (LLZO), are intensively investigated due to their high Li-ion conductivity and exceptional chemical and electrochemical stability against lithium metal anodes. However, poor interfacial contact with cathode materials, undesirable lithium plating along grain boundaries, and moisture-induced chemical degradation greatly hinder the practical implementation of LLZO-based SSEs for SSBs. In this review, the recent advances in synthesis methods, modification strategies, corresponding mechanisms, and applications of garnet-based SSEs in SSBs are critically summarized. Furthermore, a comprehensive evaluation of the challenges and development trends of LLZO-based electrolytes in practical applications is presented to accelerate their development for high-performance SSBs.