Scalable copper current collectors with precisely engineered lithiophilic alloy “skins” for durable lithium-metal batteries†

Abstract

Depositing a uniform lithium metal layer on a highly conductive current collector (CC) is essential for the development of next-generation Li metal batteries (LMBs). However, poor cycling stability, low Coulombic efficiency, and the potential safety hazards associated with Li dendrite growth remain major obstacles to their commercialization. Herein, a lithiophilic copper–zinc (Cu_0.64Zn_0.36) alloy “skin” is fabricated on commercial Cu CCs for LMBs using an adjustable and scalable ultrafast high-temperature (UHT) Joule heating method. The Cu_0.64Zn_0.36 alloy exhibits strong lithiophilicity, facilitating uniform nucleation and growth of Li metal on its surface, thereby enabling dendrite-free deposition. Density functional theory (DFT) and molecular dynamics (MD) simulations further convincingly support the experimental results. Benefiting from these enhancements, this modified Cu CC demonstrates excellent long-term stability in both LillCu half-cells and full-batteries paired with LiFePO₄ or LiNi_0.9Co_0.05Mn_0.05O₂ cathodes. More importantly, the versatile UHT method can be extended to develop various metal-“skin”-coated CCs, offering an ingenious strategy for creating composite lithiophilic materials. This work presents a viable pathway for the batch production of advanced Cu CCs for high-performance Li anodes, laying a significant foundation for the practical application of high-energy-density LMBs.