A Metal–Organic Framework as a Multifunctional Ionic Sieve Membrane for Long‐Life Aqueous Zinc–Iodide Batteries

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The introduction of the redox couple of triiodide/iodide (I₃ ⁻ /I⁻ ) into aqueous rechargeable zinc batteries is a promising energy-storage resource owing to its safety and cost-effectiveness. Nevertheless, the limited lifespan of zinc-iodine (Zn-I₂ ) batteries is currently far from satisfactory owing to the uncontrolled shuttling of triiodide and unfavorable side-reactions on the Zn anode. Herein, space-resolution Raman and micro-IR spectroscopies reveal that the Zn anode suffers from corrosion induced by both water and iodine species. Then, a metal-organic framework (MOF) is exploited as an ionic sieve membrane to simultaneously resolve these problems for Zn-I₂ batteries. The multifunctional MOF membrane, first, suppresses the shuttling of I₃ ⁻ and restrains related parasitic side-reaction on the Zn anode. Furthermore, by regulating the electrolyte solvation structure, the MOF channels construct a unique electrolyte structure (more aggregative ion associations than in saturated electrolyte). With the concurrent improvement on both the iodine cathode and the Zn anode, Zn-I₂ batteries achieve an ultralong lifespan (>6000 cycles), high capacity retention (84.6%), and high reversibility (Coulombic efficiency: 99.65%). This work not only systematically reveals the parasitic influence of free water and iodine species to the Zn anode, but also provides an efficient strategy to develop long-life aqueous Zn-I₂ batteries.