Tailoring-Orientated Deposition of Li<sub>2</sub>S for Extreme Fast-Charging Lithium–Sulfur Batteries
Jeong‐Hoon Yu, Jeong‐Hoon Yu, Byong‐June Lee, Shiyuan Zhou, Jong Hun Sung, Chen Zhao, Cheol-Hwan Shin, Bo Yu, Gui‐Liang Xu, Khalil Amine, Jong‐Sung Yu, Jong‐Sung Yu
Abstract
Precipitation/dissolution of insulating Li 2 S 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 Li 2 S 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 Li 2 S nanocrystalline between (002)-dominated graphitic layers. Our approach directs an alternative Li 2 S 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.