Reconstruction of Solid Electrolyte Interphase with SrI2 Reactivates Dead Li for Durable Anode‐Free Li‐Metal Batteries

Without excess Li, anode-free Li-metal batteries (AFLMBs) have been proposed as the most likely solution to realizing highly-safe and cost-effective Li-metal batteries. Nevertheless, short cyclic life puzzles conventional AFLMBs due to anodic dead Li accumulation with a local current concentration induced by irreversible electrolyte depletion, insufficient active Li reservoir and slow Li⁺ transfer at the solid electrolyte interphase (SEI). Herein, SrI₂ is introduced into carbon paper (CP) current collector to effectively suppress dead Li through synergistic mechanisms including reversible I^- /I₃ ^- redox reaction to reactivate dead Li, dielectric SEI surface with SrF₂ and LiF to prevent electrolyte decomposition and highly ionic conductive (3.488 mS cm^-1 ) inner layer of SEI with abundant LiI to enable efficient Li⁺ transfer inside. With the SrI₂ -modified current collector, the NCM532/CP cell delivers unprecedented cyclic performances with a capacity of 129.2 mAh g^-1 after 200 cycles.