The Regulation of Solid Electrolyte Interphase on Composite Lithium Anodes in Solid‐State Batteries

Solid‐state lithium metal batteries (SSLMBs) with solid polymer electrolyte (SPE) are highly promising for next‐generation energy storage due to their enhanced safety and energy density. However, the stability of the solid electrolyte interphase (SEI) on the lithium metal/SPE interface is a major challenge, as continuous SEI degradation and regeneration during cycling lead to capacity fading. This article investigates the SEI formation on lithium anodes (l‐SEI) and composite lithium anodes (c‐SEI) in solid‐state lithium metal batteries. The composite anodes form a uniform Li2S‐rich inorganic SEI layer and a thinner organic SEI layer, effectively passivating the interface for enhanced cycling stability. Specifically, the full cells with c‐SEI anodes sustain over 400 cycles at 0.5 C under a high areal capacity of 2.0 mAh cm−2. Moreover, the reversible high‐loading solid‐state pouch cells exhibit exceptional safety even after curling and cutting. These findings offer valuable insights into developing composite electrodes with robust SEI for solid‐state polymer‐based lithium metal batteries.