Molecular Engineering on MoS2 Enables Large Interlayers and Unlocked Basal Planes for High‐Performance Aqueous Zn‐Ion Storage

Aqueous Zn-storage behaviors of MoS₂ -based cathodes mainly rely on the ion-(de)intercalation at edge sites but are limited by the inactive basal plane. Herein, an in-situ molecular engineering strategy in terms of structure defects manufacturing and O-doping is proposed for MoS₂ (designated as D-MoS₂ -O) to unlock the inert basal plane, expand the interlayer spacing (from 6.2 to 9.6 Å), and produce abundant 1T-phase. The tailored D-MoS₂ -O with excellent hydrophilicity and high conductivity allows the 3D Zn²⁺ transport along both the ab plane and c-axis, thus achieving the exceptional high rate capability. Zn²⁺ diffusion through the basal plane is verified by DFT computations. As a proof of concept, the wearable quasi-solid-state rechargeable Zn battery employing the D-MoS₂ -O cathode operates stably even under severe bending conditions, showing great application prospects. This work opens a new window for designing high-performance layered cathode materials for aqueous Zn-ion batteries.