Interfacial Electronic Coupling‐Activated 2H‐MoS 2 for Enhanced Sulfur Conversion Kinetics in Lithium–Sulfur Batteries

ABSTRACT Interfacial electronic coupling has emerged as an effective strategy to regulate the electronic structure of sulfur hosts and enhance their catalytic activity toward lithium polysulfides conversion in lithium–sulfur batteries. However, using atomically dispersed metal sites as local electronic regulators to modulate interfacial charge redistribution and electronically activate thermodynamically stable 2H‐MoS 2 remains insufficiently understood. Herein, a 2D heterostructure was constructed by coupling stable 2H‐MoS 2 with Co single‐atom‐anchored reduced graphene oxide (MoS 2 ‐Co‐rGO). Experimental characterizations and theoretical calculations reveal that the Co single atoms regulate the electronic state of the rGO substrate and strengthen interfacial charge redistribution, thereby reconstructing the local electronic environment of adjacent Mo centers and electronically activating 2H‐MoS 2 . The electronically reconstructed MoS 2 exhibits enhanced interactions with lithium polysulfides, accelerated interfacial charge‐transfer kinetics, and facilitated Li 2 S nucleation/decomposition. Consequently, the MoS 2 ‐Co‐rGO/S cathode delivers a high specific capacity of 1328 mAh g −1 at 0.2 C and a low‐capacity decay rate of 0.042% per cycle over 800 cycles at 2 C. Moreover, an Ah‐level pouch cell achieves a capacity of 14 Ah and a gravimetric energy density of 474 Wh kg −1 . This work provides a single‐atom‐regulated interfacial electronic‐reconstruction strategy for activating stable 2H‐MoS 2 toward high‐energy‐density lithium–sulfur batteries.