Highly Lithiophilic Copper-Reinforced Scaffold Enables Stable Li Metal Anode

Lithium (Li) metal is regarded as one of the most prospective electrodes for next-generation rechargeable batteries. However, its widespread usage has been fettered by low coulombic efficiency (CE), poor cycling stability, and serious safety concerns, mainly arising from huge volumetric variation, inhomogeneous Li deposition, and dendrite growth during repeated Li plating/stripping cycles. Herein, we propose a facile one-pot electrospinning-derived highly lithiophilic nanocopper-reinforced three-dimensional-structured carbon nanofiber (Cu-CNF) as functional scaffold to stabilize the Li metal. The Cu-CNF scaffolded Li metal demonstrates homogeneous nanoplate-like Li deposition, enhanced CE, and ultrastable long lifespan cycling. As coupled with LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811), the cell possesses a remarkably stable high capacity retention of 93% over 300 cycles at 0.2 C. Furthermore, the cells paired with a thick LiFePO₄ (LFP) electrode (∼12 mg cm^-2) still can deliver a superior cycling performance even under the harsh conditions of an extremely low negative/positive electrode capacity (N/P) ratio (∼1.5) and lean electrolyte. Density functional theory calculations are performed to disclose the mechanism of the enhanced electrochemical performance of Cu-CNF scaffolded Li. This work provides a handy and cost-effective method to design superior performance Li metal anodes for practical applications.