Ultrafast Tailoring Amorphous Zn0.25V2O5 with Precision‐Engineered Artificial Atomic‐Layer 1T′‐MoS2 Cathode Electrolyte Interphase for Advanced Aqueous Zinc‐Ion Batteries

Abstract Vanadium (V)‐based oxides as cathode materials for aqueous zinc‐ion batteries (AZIBs) still encounter challenges such as sluggish Zn 2+ 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 Zn 0.25 V 2 O 5 ( c‐ ZVO) to successfully prepare a‐ ZVO@MoS 2 core@shell heterostructures, where atomic‐layer MoS 2 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 2+ , thus significantly enhancing the Zn 2+ diffusion kinetics during charge–discharge processes. Meanwhile, as an efficient artificial cathode electrolyte interphase, the precision‐engineered atomic‐layer MoS 2 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 2 and conceptually validated a‐ V 2 O 5 @MoS 2 derived from commercial c‐ V 2 O 5 exhibit excellent cycling stability at an ultralow current density (0.05 A g −1 ) 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.