Revealing the Multifunctional Electrocatalysis of Indium‐Modulated Phthalocyanine for High‐Performance Lithium‐Sulfur Batteries

The sluggish kinetics of complicated multiphase conversions and the severe shuttling effect of lithium polysulfides (LiPSs) significantly hinder the applications of Li‐S battery, which is one of the most promising candidates for the next‐generation energy storage system. Herein, a bifunctional electrocatalyst, indium phthalocyanine self‐assembled with carbon nanotubes (InPc@CNT) composite material, is proposed to promote the conversion kinetics of both reduction and oxidation processes, demonstrating a bidirectional catalytic effect on both nucleation and dissolution of Li 2 S species. The theoretical calculation shows that the unique electronic configuration of InPc@CNT is conducive to trapping soluble polysulfides in the reduction process, as well as the modulation of electron transfer dynamics also endows the dissolution of Li 2 S in the oxidation reaction, which will accelerate the effectiveness of catalytic conversion and facilitate sulfur utilization. Moreover, the InPc@CNT modified separator displays lower overpotential for polysulfide transformation, alleviating polarization of electrode during cycling. The integrated spectroscopy analysis, HRTEM, and electrochemical study reveal that the InPc@CNT acts as an efficient multifunctional catalytic center to satisfy the requirements of accelerating charging and discharging processes. Therefore, the Li–S battery with InPc@CNT‐modified separator obtains a discharge‐specific capacity of 1415 mAh g −1 at a high rate of 0.5 C. Additionally, the 2 Ah Li–S pouch cells deliver 315 Wh kg −1 and achieved 80% capacity retention after 50 cycles at 0.1 C with a high sulfur loading of 10 mg cm −2 . Our study provides a practical method to introduce bifunctional electrocatalysts for boosting the electrochemical properties of Li–S batteries.