Cu(100) Faceted Surface for Lithiophilicity: High‐Utilization of Surface and Space of Hosts for Lithium Metal Anodes

Lithium metal anodes suffer from poor cycling stability and potential safety hazards. To alleviate the problems, Li thin film anodes prepared on current collectors (CCs) and Li‐free type of anodes involving direct Li plating on CCs have received increasing attention. Herein, we report atomic‐scale design of surface lithiophilicity of Cu CCs based on surface lattice coincidence of the bcc Li(110) and fcc Cu(100) faces as well as electrochemical achievement of Cu(100)‐preferred surfaces for smooth Li deposition with low nucleation barrier. Purposely‐designed solid‐electrolyte interphase is also created for Li anodes prepared on CCs. Not only is smooth Li planar thin film prepared, but also uniform Li plating/stripping on the skeleton of 3D CCs is achieved with high‐utilization of the surface and space of the 3D CCs. Our work demonstrates surface electrochemistry approaches to construct stable Li metal‐electrolyte interphases towards practical applications of Li anodes prepared on CCs.

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