Unraveling Energy Storage Performance and Mechanism of Metal–Organic Framework‐Derived Copper Vanadium Oxides with Tunable Composition for Aqueous Zinc‐Ion Batteries

Abstract

Achieving high‐performance aqueous zinc (Zn)‐ion batteries (AZIBs) requires stable and efficient cathode materials capable of reversible Zn‐ion intercalation. Although layered vanadium oxides possess high Zn‐ion storage capacity, their sluggish kinetics and poor conductivity present significant hurdles for further enhancing the performance of AZIBs. In response to this challenge, a dissolution‐regrowth and conversion approach is formulated using metal–organic frameworks (MOFs) as a sacrificial template, which enables the in situ creation of copper vanadium oxides (CuVOx) with porous 1D channels and distinctive nanoarchitectures. Owing to their distinctive structure, the optimized CuVOx cathode experiences a reaction involving the synergistic insertion/extraction of Zn2+, resulting in rapid Zn2+ diffusion kinetics and enhanced electrochemical activity postactivation. Specifically, the activated electrode delivers a reversible capacity of 519 mAh g−1 at 0.5 A g−1 for AZIBs. It is noteworthy that the electrode exhibits a remarkable reversible rate capacity of 220 mAh g−1 at 5 A g−1 with excellent durable cycleability, retaining 88% of its capacity even after 3000 cycles. Various ex situ testing methods endorse the reversible insertion/extraction of Zn2+ in the CuVOx cathode. This study provides a novel insight into high‐performance MOF‐derived unique structure designs for AZIB electrodes.