Advances in Inorganic Solid‐State Electrolyte/Li Interface

The increasing demand for high‐energy‐density and high‐safety energy storage devices has sparked a growing interest in all‐solid‐state lithium metal batteries (ASSLMBs). A high‐quality inorganic solid‐state electrolyte (ISE) is a fundamental requirement for ASSLMBs, and an effective ISE/Li interface is a key factor in attaining high‐performance ASSLMBs. In this Concept, we initially summarize the challenges encountered by ISE/Li interfaces and delineate four commonly employed strategies for modifying the ISE/Li interface. Then, we explore the merits and drawbacks of coatings utilized as ISE/Li interfacial phases. We also delve into the commonly employed thermal bonding and innovative cold bonding methods utilized for in situ interface preparation. Lastly, we spotlight future directions for enhancing the functionality of ISE/Li interfaces and achieving high‐performance ASSLMBs.