Interfacial Engineering for High‐performance Garnet‐based Solid‐state Lithium Batteries

Abstract Solid‐state batteries represent the future of energy storage technology, offering improved safety and energy density. Garnet‐type Li7La3Zr2O12 (LLZO) solid‐state electrolytes‐based solid‐state lithium batteries (SSLBs) stand out for their appealing material properties and chemical stability. Yet, their successful deployment depends on conquering interfacial challenges. This review article primarily focuses on the advancement of interfacial engineering for LLZO‐based SSLBs. We commence with a concise introduction to solid‐state electrolytes and a discussion of the challenges tied to interfacial properties in LLZO‐based SSLBs. We deeply explore the correlations between structure and properties and the design principles vital for achieving an ideal electrode/electrolyte interface. Subsequently, we delve into the latest advancements and strategies dedicated to overcoming these challenges, with designated sections on cathode and anode interface design. In the end, we share our insights into the advancements and opportunities for interface design in realizing the full potential of LLZO‐based SSLBs, ultimately contributing to the development of safe and high‐performance energy storage solutions.