Tuning the Electronic Configuration of MoMn Bimetallic–Nitrogen–Carbon Catalysts for Advanced Lithium–Sulfur Batteries

ABSTRACT Lithium–sulfur (Li–S) batteries are widely recognized as a promising future energy storage solution, primarily due to their high theoretical energy density and low cost. However, their commercial implementation remains hindered by severe polysulfide shuttling and sluggish redox kinetics. Herein, we introduce a synergistic bicatalytic strategy by constructing bimetallic catalysts, where Mo and Mn active centers are embedded within an N‐doped carbon matrix (MoMn–NC). Combined theoretical and experimental analyses demonstrate that Mo incorporation precisely regulates the local electronic configuration of Mn–NC active sites, which boosts electron transfer from both Mn and Mo to LiPSs and shifts the d –band center closer to the Fermi level. Such intermetallic coupling modulates the charge environment of the active sites, enabling bimetallic centers to strongly immobilize polysulfides and accelerate sulfur conversion, thus suppressing the shuttling effect and preventing electrode passivation. Consequently, the MoMn–NC electrocatalytic membranes enable Li–S batteries to achieve prolonged durability exceeding 1000 cycles, superior rate capability up to 5 C, and a remarkable areal capacity of 6.9 mAh cm ⁻² under high sulfur loading (7.1 mg cm ⁻² ) and lean electrolyte dosage (5 µL mg ⁻¹ ) at 0.2 C. These findings showcase the pivotal role of electronic structure modulation in bimetallic–nitrogen–carbon catalysts for pragmatic Li–S battery techniques.