Synergistic Interaction of Strongly Polar Zinc Selenide and Highly Conductive Carbon Nanoframeworks Accelerates Redox Kinetics of Polysulfides

Lithium-sulfur batteries (LSBs) have become strong competitors in secondary battery systems because of their superior theoretical capacity and energy density. However, due to the serious shuttle effect of soluble long-chain lithium polysulfides (LiPSs) and the slow solid-solid reaction kinetics, LSBs face some specific challenges, such as a short cycle life and low rate performance. The introduction of selenide/carbon composites derived from zeolite imidazolate frameworks (ZIFs) into separator coatings is a direct and effective solution to the aforementioned problems. Here, a zinc selenide/carbon catalyst material (ZnSe@C) was constructed and employed to modify commercial polypropylene (PP) separators to accelerate the conversion of intermediates. The highly polar ZnSe effectively fixes the active material on the cathode side by transferring electrons between elements with LiPSs and improves the utilization rate of sulfur. Concurrently, the highly conductive carbon nanoskeleton generated following the pyrolysis of ZIF-8 ensures the rapid transfer of charges during the catalytic reaction. The prepared ZnSe@C has a large specific surface area (250.07 m² g^-1) and mesoporous ratio (78.03%), which not only enhances adsorption and catalysis but also promotes the penetration of the electrolyte and the transport of Li⁺. Based on this, ZnSe@C/PP separator cells exhibit a low average capacity decay rate of 0.051% per cycle after 500 cycles at 1 C.