Ultrafast Tailoring Amorphous ZnVO with Precision-Engineered Artificial Atomic-Layer 1T'-MoS Cathode Electrolyte Interphase for Advanced Aqueous Zinc-Ion Batteries.

Vanadium (V)-based oxides as cathode materials for aqueous zinc-ion batteries (AZIBs) still encounter challenges such as sluggish Zn diffusion kinetics and V-dissolution, thus leading to severe capacity fading and limited life span. Here, we designed an ultrafast and facile colloidal chemical synthesis strategy based on crystalline ZnVO (c-ZVO) to successfully prepare a-ZVO@MoS core@shell heterostructures, where atomic-layer MoS uniformly coats on the surface of amorphous a-ZVO. The tailored amorphous structure of a-ZVO provides more isotropic pathways and active sites for Zn, thus significantly enhancing the Zn diffusion kinetics during charge-discharge processes. Meanwhile, as an efficient artificial cathode electrolyte interphase, the precision-engineered atomic-layer MoS with semi-metallic 1T' phase not only contributes to improved electron transport but also effectively inhibits the V-dissolution of a-ZVO. Therefore, the prepared a-ZVO@MoS and conceptually validated a-VO@MoS derived from commercial c-VO exhibit excellent cycling stability at an ultralow current density (0.05 A g) while maintaining good rate capability and capacity retention. This research achievement provides a new effective strategy for various amorphous cathode designs for AZIBs with superior performance.