Tailoring-Orientated\nDeposition of Li<sub>2</sub>S\nfor Extreme Fast-Charging Lithium–Sulfur Batteries

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