Dendrites‐Free Lithium Metal Anode Enabled by Synergistic Surface Structural Engineering

Abstract Lithium (Li) metal with high specific capacity and low redox potential is widely considered as a potential anode for lithium‐ion batteries (LIBs) with high energy density. However, the catastrophic dendrites growth, “dead Li” formation, and surface passivation hinder its practical application. Herein, a selective artificial solid electrolyte interphase (SEI) layer (Li₂S_x, x = 1, 2) protection strategy is adopted, where the tip sites passivation and the uniform Li nucleation in grooves are well combined, which enables reversible Li stripping/plating with high storage capacity and robust electrode framework. The grooves derived patterned array Li with selective Li₂S_x artificial SEI (LS@A‐Li) exhibit over 1800 h cycling life at 1.0 mA cm^–2/1.0 mAh cm^–2 and over 600 h even under 5.0 mA cm^–2/10.0 mAh cm^–2. The application feasibility of such LS@A‐Li is also confirmed by coupling with commercial LiFePO₄ and LiNi_0.5Co_0.2Mn_0.3O₂ (NCM523) in the full batteries. This work paves way for the large‐scale application of Li metal anode in lithium‐metal batteries with a facile and efficient fabrication process.