Selective Lithium Deposition Through 3D Copper Collector With Lithiophilic Alloy “Skins” and Curvature Boundaries for Dendrite‐Free Lithium‐Metal Anodes

ABSTRACT Although lithium metal has been regarded as an ideal anode material for high‐energy‐density batteries, its practical applications remain hindered by many serious challenges. Three‐dimensional (3D) porous Cu current collectors demonstrate potential in ensuring uniform Li deposition. However, notable drawbacks of 3D Cu collectors—such as poor lithophilic properties, unordered interface microstructure, and insufficient surface area—still hamper their effectiveness. Herein, a 3D porous Cu skeleton with lithiophilic Cu 0.64 Zn 0.36 alloy “skins” and curvature boundaries (CuZn@Cu) is developed. In CuZn@Cu, the Cu 0.64 Zn 0.36 alloy layer endows the collector with good lithium affinity and low surface reaction activation energy, thereby promoting uniform lithium deposition. In addition, the abundant curvature boundaries in CuZn@Cu regulate the distributions of the electric field and lithium ion flux, guiding the selective nucleation and growth of lithium. Consequently, compact and dendrite‐free lithium deposition is achieved on CuZn@Cu, and the CuZn@Cu collector enables a high average Coulombic efficiency of 98.15% in 1000 cycles. The lithium symmetric cells with the CuZn@Cu exhibit a long cycle life of more than 1400 h at 1 mA cm −2 .