A Robust Li-Intercalated Interlayer with Strong Electron Withdrawing Ability Enables Durable and High-Rate Li Metal Anode

Lithium (Li) anodes are not stable in most organic electrolytes upon cycling, which is an urgent issue in next-generation Li metal batteries (LMBs) for durable high-energy-density storage. Enhancing the Li plating uniformity is commonly believed to be decisive for stabilizing the Li metal anode. However, here it is found that prohibiting e – escape to the electrode surface for suppressing electrolyte decomposition is a more critical action than Li plating morphology control in LMB performances. A Li-intercalated interlayer, obtained through the lithiation of an orthorhombic Nb 2 O 5 precursor layer with disproportionate Nb 4+ /Nb 5+ components, is involved as the model Li protection structure with high structural integrality, fast Li + conducting channels, and, more importantly, strong e – withdrawing ability. The Li anode performance gained by this advanced interlayer significantly exceeds that by the conventional lithiophilic interlayer, particularly under limited-Li-source conditions. Our findings provide alternative guidelines for protective interlayer construction to achieve reliable and safe LMBs.