Enhancing Sulfur Redox Conversion of Active Iron Sites by Modulation of Electronic Density for Advanced Lithium-Sulfur Battery

Despite lithium-sulfur (Li-S) batteries possessing ultrahigh energy density as great promising energy storage devices, the suppressing shuttle effect and improving sulfur redox reaction (SROR) are vital for their practical application. Developing high-activity electrocatalysts for enhancing the SROR kinetics is a major challenge for the application of Li-S batteries. Herein, single-molecule iron phthalocyanine species are anchored on the N and P dual-doped porous carbon nanosheets (Fe-NPPC) via axial Fe-N coordination to optimize the electronic structure of active centers. The Fe-NPPC can promote the catalytic conversion of polysulfides by modulation of the electronic density in active moieties, endowing the Li-S battery with a high reversible capacity of 1023 mAh g⁻¹ at 1 C as well as an ultralow capacity decay of 0.035% per cycle over 1500 cycles. Even with a high sulfur loading of 7.1 mg cm⁻², the Li-S battery delivers a high areal capacity of 4.8 mAh cm⁻² after 150 cycles at 0.2 C. With further increasing the sulfur loading to 9.2 mg cm⁻², an excellent areal capacity of up to 9.3 mAh cm⁻² is obtained at 0.1 C.