Oxygen‐Doped MoS2 with Expanded Interlayer Spacing for Rapid and Stable Polysulfide Conversion

Abstract Lithium–sulfur batteries face challenges such as the polysulfide shuttle effect and sluggish redox kinetics, leading to poor sulfur utilization and limited cyclic stability. Herein, an oxygen‐doped engineering approach is presented to achieve pillar‐free interlayer extension of MoS 2 (E‐MoS 2 ) for lithium polysulfide conversion. E‐MoS 2 features expanded interlayer spacing (from 0.63 to 0.95 nm), improved conductivity, and an optimized Mo d band center, which collectively enhances polysulfide conversion efficiency. Consequently, cathodes with E‐MoS 2 deliver a capacity of 638 mAh g −1 after 600 cycles at 2 C (0.046% decay/cycle) and an areal capacity of 12.0 mAh cm −2 under practical conditions (12 mg cm −2 S loading, E/S = 4 µL mg −1 ). This work highlights interlayer engineering as a key strategy for optimizing MoS 2 catalysts in conversion‐type batteries.