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

Abstract

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 Li₂S 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 Li₂S 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.

Keywords

bidirectional catalyst / indium phthalocyanine / lithium-sulfur batteries / pouch cells

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