Efficient Zeolite Electrocatalysts for Lithium‐Sulfur Batteries: Synergistic Catalysis of Co Single Atom and CoO Nanoparticles Regulated by Pore Structure

Abstract As a significant class of multiphase solid catalysts, metal‐zeolite catalysts have demonstrated excellent catalytic performance in multiphase catalysis. Herein, the regulatory mechanisms of zeolite pore structures on lithium polysulfides (LiPSs) adsorption and catalysis are investigated based on zeolites Silicalite‐1 (S‐1) and Silicalite‐2 (S‐2). Furthermore, to address the challenge that single‐site catalysts struggle to effectively mediate the complex multiphase reactions in lithium‐sulfur batteries (LSBs), a dual‐site efficient metal‐zeolite electrocatalyst, Co/S‐1, is functionally designed by stably anchoring Co single atoms (SAs) and CoO nanoparticles (CoO NPs) within the S‐1 framework. Theoretical calculations show that S‐1 with complex pores exhibits a high diffusion barrier for LiPSs, thereby suppressing shuttling and promoting sufficient contact between LiPSs and Co catalytic sites, and provides selective diffusion channels for LiPSs to increase catalytic reaction paths and enhance efficiency. When Co/S‐1 is applied as a coating on commercial polypropylene (PP) separators, LSBs exhibit excellent electrochemical performance, including a high initial capacity of 1591.83 mAh g ⁻¹ at 0.2 C, retaining 774.22 mAh g ⁻¹ after 500 cycles at 1 C. At a high sulfur loading of 5.6 mg cm ⁻² , the system achieves an initial areal capacity of 6.089 mAh cm ⁻² at 0.1 C, demonstrating significant potential for practical applications.