Defect‐Modulate Nanoalloy Catalysts Enable Efficient Catalytic Conversion in Lithium–Sulfur Batteries

To address critical issues in lithium–sulfur batteries, such as slow polysulfide conversion kinetics and shuttle effects, we designed and synthesized a high‐performance nanoalloy catalyst through a defect reconstruction strategy, aiming to enhance the electrochemical performance of batteries. The coexistence of Ni, Co, and Mn first led to the formation of a metastable (Ni 1/3 Co 1/3 Mn 1/3 ) 3 ZnC@C precursor. Subsequent thermal treatment induced Zn volatilization and vacancy formation, thereby driving the synergistic reconstruction of the three metal components into a defect‐rich alloy resembling the A 3 B 7 structure. Electrochemical performance testing revealed that the A 3 B 7 @C‐based lithium–sulfur battery exhibited an initial specific capacity of 1278 mAh g −1 at 0.1C and maintained a reversible capacity of 665 mAh g −1 at the high rate of 3C. After 100 cycles, the capacity retention rate was 81.4%. Additionally, this catalyst exhibits a lower polarization voltage (0.34 V) and reduced charge–transfer impedance. Its Tafel slope (44.9 mV dec −1 ) indicates an effective reduction in the activation energy for polysulfide conversion, thereby accelerating reaction kinetics. This study optimizes the exposure and electronic properties of catalytically active sites through the synergistic effects of defect regulation and alloy reconstruction, providing new insights for designing high‐performance lithium–sulfur batteries.