A High Performing Zn‐Ion Battery Cathode Enabled by In Situ Transformation of V2O5 Atomic Layers

Developing high capacity and stable cathodes is a key to successful commercialization of aqueous Zn‐ion batteries (ZIBs). Pure layered V₂O₅ has a high theoretical capacity (585 mAh g^?1), but it suffers severe capacity decay. Pre‐inserting cations into V₂O₅ can substantially stabilize the performance, but at an expense of lowered capacity. Here we show that an atomic layer deposition derived V₂O₅ can be an excellent ZIB cathode with high capacity and exceptional cycle stability at once. We report a rapid in situ on‐site transformation of V₂O₅ atomic layers into Zn₃V₂O₇(OH)₂?2 H₂O (ZVO) nanoflake clusters, also a known Zn‐ion and proton intercalatable material. High concentration of reactive sites, strong bonding to the conductive substrate, nanosized thickness and binder‐free composition facilitate ionic transport and promote the best utilization of the active material. We also provide new insights into the V₂O₅‐dissolution mechanisms for different Zn‐salt aqueous electrolytes and their implications to the cycle stability.