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 angstrom), 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.

Automated summary

The study introduces a molecular engineering strategy for MoS2 cathodes, involving the manufacturing of structure defects and O-doping to unlock the inactive basal plane and increase the interlayer spacing, leading to the production of abundant 1T-phase for enhanced Zn2+ transport. The tailored D-MoS2-O material exhibits excellent hydrophilicity and high conductivity, allowing for high-rate capability and stable performance in a wearable rechargeable Zn battery, showcasing great application potential for aqueous Zn-ion batteries.