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 Nb2O5 precursor layer with disproportionate Nb4+/Nb5+ 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.