Dynamic Integrated Interface for Synergistic Li + Redox‐Diffusion in Low‐Temperature Lithium Metal Batteries

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ABSTRACT Practical application of lithium metal batteries (LMBs) is severely hindered by nonuniform lithium (Li) nucleation during the charging process. Low‐temperature conditions further substantially elevate the barrier for Li + reduction, leading to uncontrolled dendritic growth. Herein, we propose a “synergistic Li + redox‐diffusion” regulation mechanism to reduce the kinetic barrier for Li + reduction, and the integrated intermetallic (Ag‐Sn‐Ag 3 Sn, abbreviated ASA) layer is self‐reductively constructed on the Li metal, in which Ag provides abundant nucleation sites to guide uniform Li deposition, Sn acts as an electron redistribution center to enable directional interfacial charge transfer, and Ag 3 Sn features a low diffusion barrier (0.75 eV) that accelerates Li + migration. As a result, the ASA@Cu electrode exhibits a Li deposition rate of 6.65 ng s −1 by electrochemical quartz crystal microbalance (EQCM) measurements during the nucleation stage, which is ∼19.6% higher than that of bare Cu. Application of ASA@Li into the symmetric cell achieves a long lifespan of 2500 h at a high current density of 10 mA cm −2 , and the NCM811||ASA@Li full cell achieves high capacity retention of 86.1% after 100 cycles at −20°C and 0.2 C. This work provides fundamental insights into synergistically regulating Li + reduction kinetics for low‐temperature LMBs.

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