Electrocatalytic MOF‐Carbon Bridged Network Accelerates Li ⁺ ‐Solvents Desolvation for High Li ⁺ Diffusion toward Rapid Sulfur Redox Kinetics

Lithium-sulfur batteries are famous for high energy density but prevented by shuttling effect and sluggish electrochemical conversion kinetics due to the high energy barriers of Li+ transport across the electrode/electrolyte interface. Herein, the Li+-solvents dissociation kinetics is catalyzed and stimulated by designing a carbon bridged metal-organic framework (MOF@CC), aimed at realizing increased bare Li+ transport for the rapid conversion kinetics of sulfur species. Theoretical simulations and spectroscopic results demonstrate that the bridged MOF@CC well grants a special transport channel for accelerating Li+ benefited from aggregated anion/cation clusters. Moreover, the C-N bridge between -NH2 ligand in MOF and carbon shell enhances electron exchange, and thus promotes polysulfide catalytic efficiency and hinder polysulfide aggregation and accumulation. With the MOF@CC-modified separators, the assembled Li/S batteries deliver a reversible capability of 1063 mAh g(-1) at 0.5 C, a capacity retention of 88% after 100 cycles, and a high-rate performance of 765 mAh g(-1) at 5 C. Moreover, the large areal pouch cell with 100 mu m Li foil and lean electrolyte is capable of stabilizing 855 mAh g(-1) after 70 cycles. These results well demonstrate the efficiency of catalyzing desolvation for fast Li+ transport kinetics and the conversion of polysulfides.