2D-on-2D Mott–Schottky 1T-MoS₂ Heterostructure with Rich Defects and an Expanded Interlayer for Enhanced Zn-Storage

Layered transition metal dichalcogenides, especially MoS2, have great potential as cathodes for aqueous zinc ion batteries (AZIBs) due to their flexible interlayer structural characteristics. However, the unsatisfactory diffusion efficiency of Zn2+ in pristine MoS2 severely restricts its application. Herein, a strategy of interfacial heterostructure construction and surface defect fabrication is employed to introduce metallic VS2 with matchable formation energies into MoS2 (designated as HD-MVS), thereby exposing active interfaces, increasing the 1T-phase proportion, and expanding interlayer spacing. The GITT, rate-scan CV, and multiple ex situ characterizations confirm that HD-MVS possesses a rapid and reversible Zn2+ insertion/extraction ability. Therefore, HD-MVS exhibits satisfactory rate performance (265 mA h g–1 at 0.1 A g–1 and 116 mA h g–1 at 6.0 A g–1), long cycle durability (92.47% capacity retention over 5000 cycles at 1.0 A g–1), and stable flexible electrochemistry (91.68% capacity retention after 2000 cycles under 180°), providing assistance for the widespread application of AZIBs in the future.