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Lithiophilic Cu‐Li2O matrix on a Cu Collector to Stabilize Lithium Deposition for Lithium Metal Batteries

Lithium metal anode is the most ideal candidate for next‐generation energy storage system. However, the uncontrolled dendrite growth, infinite volume expansion, and undesired side reactions lead to serious safety issues and hinder their potential application. Herein, a pre‐lithiation strategy is proposed to construct a high‐lithiophilic Cu‐Li2O matrix on commercial Cu foil. The in situ‐generated Li2O promises adequate nucleation sites and strengthens solid electrolyte interphase and lateral lithium deposition. Meanwhile, the existence of 3D matrix reduces the local current density. The synergy effect of Li2O and Cu suppresses the growth of lithium dendrites. As a result, Cu‐Li2O matrix reveals an enhanced lithium plating/stripping behavior with Coulombic efficiency of 98.46% after 270 cycles. The symmetrical cell assembled by Li‐plated electrodes displays a prolonged lifespan of 1400 h. The work demonstrates a scalable and effective approach for modified current collectors toward stable Li metal anode.