Phase‐Transformable MOF‐Derived α‐ZnMoO₄ Cathode Featuring Oxygen Vacancies and Lattice Lubrication for Enhanced Zinc‐Ion Storage

A triclinic zinc molybdate (α‐ZnMoO 4 ) cathode was developed via the pyrolysis of Zn–Mo bimetallic metal–organic frameworks (MOFs) as sacrificial intermediates for high‐performance aqueous zinc‐ion batteries (AZIBs). After high‐temperature pyrolysis, the MOF‐derived single‐phase α‐ZnMoO 4 consists of particles approximately 4 μm in size. Notably, the structure of MOFderived α‐ZnMoO 4 transitions into a preferred α‐ZnMoO 4 ·0.8H 2 O phase with expanded lattice spacing during the initial discharge process, facilitating efficient Zn 2+ intercalation/deintercalation. This hydrated structure remains stable throughout cycling, contributing to its excellent electrochemical performance. The cathode delivers a high reversible capacity of 380 mAh g −1 at 0.05 A g −1 and retains 95% of its capacity after 500 cycles at 0.2 A g −1 . Electrochemical and structural analyses reveal that the synergistic effects of phase transformation, oxygen vacancies, and water‐mediated lattice lubrication contribute to the superior cycling stability and Zn 2+ storage kinetics of the material. These findings highlight the potential of MOF‐derived oxide cathodes and provide a strategic pathway for designing advanced materials for next‐generation AZIBs.