Confining Iodine into Metal‐Organic Framework Derived Metal‐Nitrogen‐Carbon for Long‐Life Aqueous Zinc‐Iodine Batteries

Abstract Aqueous zinc–iodine batteries (AZIBs) are highly appealing for energy requirements owing to their safety, cost‐effectiveness, and scalability. However, the inadequate redox kinetics and severe shuttling effect of polyiodide ions impede their commercial viability. Herein, several Zn‐MOF‐derived porous carbon materials are designed, and the further preparation of iron–doped porous carbon (Fe–N–C, M9) with varied Fe doping contents is optimized based on a facile self‐assembly/carbonization approach. M9, with atomic Fe coordinated to nitrogen atoms, is employed as an efficient cathode host for AZIBs. Functional modifications of porous carbon hosts involving the doping species and levels are investigated. The adsorption tests, in situ Raman spectroscopy, and in situ UV–vis results demonstrate the adsorption capability and charge‐discharge mechanism for the iodine species. Furthermore, experimental findings and theoretical analyses have proven that the redox conversion of iodine is enhanced through a physicochemical confinement effect. This study offers basic principles for the strategic design of single‐atom dispersed carbon as an iodine host for high‐performance AZIBs. Flexible soft–pack battery and wearable microbattery applications also have implications for future long‐life aqueous battery designs.