Bilayered Vanadium Oxides Pillared by Strontium Ions and Water Molecules as Stable Cathodes for Rechargeable Zn‐Metal Batteries

Abstract Vanadium‐based compounds have attracted significant attention as cathodes for aqueous zinc metal batteries (AZMBs) because of their remarkable advantages in specific capacities. However, their low diffusion coefficient for zinc ions and structural collapse problems lead to poor rate capability and cycle stability. In this work, bilayered Sr_0.25V₂O₅·0.8H₂O (SVOH) nanowires are first reported as a highly stable cathode material for rechargeable AZMBs. The synergistic pillaring effect of strontium ions and water molecules improves the structural stability and ion transport dynamics of vanadium‐based compounds. Consequently, the SVOH cathode exhibits a high capacity of 325.6 mAh g⁻¹ at 50 mA g⁻¹, with a capacity retention rate of 72.6% relative to the maximum specific capacity at 3.0 A g⁻¹ after 3000 cycles. Significantly, a unique single‐nanowire device is utilized to demonstrate the excellent conductivity of the SVOH cathode directly. Additionally, the energy storage mechanism of zinc insertion and extraction is investigated using a variety of advanced in situ and ex situ analysis techniques. This method of ion intercalation to improve electrochemical performance will further promote the development of AZMBs in large‐scale applications.