Ultrafast‐Loaded Nickel Sulfide on Vertical Graphene Enabled by Joule Heating for Enhanced Lithium Metal Batteries

Abstract The design and fabrication of a lithiophilic skeleton are highly important for constructing advanced Li metal anodes. In this work, a new lithiophilic skeleton is reported by planting metal sulfides (e.g., Ni₃S₂) on vertical graphene (VG) via a facile ultrafast Joule heating (UJH) method, which facilitates the homogeneous distribution of lithiophilic sites on carbon cloth (CC) supported VG substrate with firm bonding. Ni₃S₂ nanoparticles are homogeneously anchored on the optimized skeleton as CC/VG@Ni₃S₂, which ensures high conductivity and uniform deposition of Li metal with non‐dendrites. By means of systematic electrochemical characterizations, the symmetric cells coupled with CC/VG@Ni₃S₂ deliver a steady long‐term cycle within 14 mV overpotential for 1800 h (900 cycles) at 1 mA cm⁻² and 1 mAh cm⁻². Meanwhile, the designed CC/VG@Ni₃S₂‐Li||LFP full cell shows notable electrochemical performance with a capacity retention of 92.44% at 0.5 C after 500 cycles and exceptional rate performance. This novel synthesis strategy for metal sulfides on hierarchical carbon‐based materials sheds new light on the development of high‐performance lithium metal batteries (LMBs).