Ultrafast Tailoring Amorphous Zn_0.25V₂O₅ 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.