Interface-induced lithiophilicity enhancement in graphite for advanced lithium metal anodes

Lithium metal anode (LMA) use in practical applications is hampered by issues such as dendrite growth, low coulombic efficiency (CE), and unstable solid electrolyte interphase (SEI) formation during cycling. Herein, we examine lithiophilic interfacial-gradient designs consisting of a thin metallic (Ag, Sb, Sn or Bi) layer deposited on copper (Cu) foil followed by a graphite (Gr) overlayer. The best performing engineered anode (Sb) reduced the Li nucleation overpotential and enabled stable lithium (Li) plating/stripping for up to 250 cycles at a high areal capacity of 3 mAh cm⁻² and a current density of 1 mA cm⁻². Symmetric cells demonstrated stable operation for up to 1000 h. In full-cells, the Li@Gr/Sb–Cu anode delivered specific capacities of 128.1 mAh g⁻¹vs. NMC 811 and 447.1 mAh g⁻¹versus a sulfur cathode after 200 cycles. This study unveils the ability of this interfacial strategy to enable stable Li deposition and improve long-term battery performance.