Tailoring Lithium Deposition via an SEI‐Functionalized Membrane Derived from LiF Decorated Layered Carbon Structure

Abstract Lithium (Li) metal is a key anode material for constructing next generation high energy density batteries. However, dendritic Li deposition and unstable solid electrolyte interphase (SEI) layers still prevent practical application of Li metal anodes. In this work, it is demonstrated that an uniform Li coating can be achieved in a lithium fluoride (LiF) decorated layered structure of stacked graphene (SG), leading to the formation of an SEI‐functionalized membrane that retards electron transfer by three orders of magnitude to avoid undesirable Li deposition on the top surface, and ameliorates Li + ion migration to enable uniform and dendrite‐free Li deposition beneath such an interlayer. Surface chemistry analysis and density functional theory calculations demonstrate that these beneficial features arise from the formation of C–F x surface components on the SG sheets during the Li coating process. Based on such an SEI‐functionalized membrane, stable cycling at high current densities up to 3 mA cm −2 and Li plating capacities up to 4 mAh cm −2 can be realized in LiPF 6 /carbonate electrolytes. This work elucidates the promising strategy of modifying Li plating behavior through the SEI‐functionalized carbon structure, with significantly improved cycling stability of rechargeable Li metal anodes.