Stabilizing Lithiophilic Sites Via Bimetallic Oxide Heterointerfaces

Abstract Designing metal oxide hosts with multiple lithophilic sites has emerged as a promising strategy to stabilize lithium (Li) metal anode for Li metal batteries (LMBs). Through lowering Li nucleation overpotentials, metal‐oxide‐derived lithiophilic frameworks can guide uniform Li deposition. However, lithiophilic sites suffer from failure upon cycling due to the structural collapse, limiting their durability for practical applications. Herein, a heterointerfacing strategy is reported to stabilize the alloy‐type lithiophilic sites of zinc. Nondurable zinc oxide is closely jointed with durable cobalt oxide, forming a unique bimetallic oxide heterointerface that possesses both favorable Li affinity and high structural integrity. The roles of individual components and the interface are both investigated. The heterostructured framework serves as a buffer layer at the anode/electrolyte interface, enabling stable regulation of Li plating and stripping. The as‐modified Li metal anode achieves high coulombic efficiency and long‐term stability in practical LMBs. This work sheds a light on designing durable lithiophilic hosts for LMBs under practical conditions.