Co/MoN Invigorated Bilateral Kinetics Modulation for Advanced Lithium–Sulfur Batteries

Abstract Sluggish sulfur redox kinetics and Li‐dendrite growth are the main bottlenecks for lithium–sulfur (Li–S) batteries. Separator modification serves as a dual‐purpose approach to address both of these challenges. In this study, the Co/MoN composite is rationally designed and applied as the modifier to modulate the electrochemical kinetics on both sides of the sulfur cathode and lithium anode. Benefiting from its adsorption‐catalysis function, the decorated separators (Co/MoN@PP) not only effectively inhibit polysulfides (LiPSs) shuttle and accelerate their electrochemical conversion but also boost Li + flux, realizing uniform Li plating/stripping. The accelerated LiPSs conversion kinetics and excellent sulfur redox reversibility triggered by Co/MoN modified separators are evidenced by performance, in‐situ Raman detection and theoretical calculations. The batteries with Co/MoN@PP achieve a high initial discharge capacity of 1570 mAh g −1 at 0.2 C with a low decay rate of 0.39%, uniform Li + transportation at 1 mA cm −2 over 800 h. Moreover, the areal capacity of 4.62 mAh cm −2 is achieved under high mass loadings of 4.92 mg cm −2 . This study provides a feasible strategy for the rational utilization of the synergistic effect of composite with multifunctional microdomains to solve the problems of Li anode and S cathode toward long‐cycling Li–S batteries.