Tailoring-Orientated Deposition of Li₂S for Extreme Fast-Charging Lithium–Sulfur Batteries

Precipitation/dissolution of insulating Li₂S has long been recognized as the rate-determining step in lithium-sulfur (Li-S) batteries, which dramatically undermines sulfur utilization at elevated charging rates. Herein, we present an orientated Li₂S deposition strategy to achieve extreme fast charging (XFC, ≤15 min) through synergistic control of porosity, electronic conductivity, and anchoring sites of electrode substrate. Via magnesiothermic reduction of a zeolitic imidazolate framework, a nitrogen-doped and hierarchical porous carbon with highly graphitic phase was developed. This design effectively reduces interfacial resistance and ensures efficient sequestration of polysulfides during deposition, leading to (110)-preferred growth of Li₂S nanocrystalline between (002)-dominated graphitic layers. Our approach directs an alternative Li₂S deposition pathway to the commonly reported lateral growth and 3D thickening growth mode, ameliorating the electrode passivation. Therefore, a Li-S cell capable of charging/discharging at 5C (12 min) while maintaining excellent cycling stability (82% capacity retention) for 1000 cycles is demonstrated. Even under high S loading (8.3 mg cm^-2) and low electrolyte/sulfur ratio (3.8 mL mg^-1), the sulfur cathode still delivers a high areal capacity of >7 mAh cm^-2 for 80 cycles.