Dynamic Regulation for the Well‐Distribution of Electrons and Zn ²⁺ Ions Achieving Uniform Zn Redox in Ah‐Scale Pouch Cells

Abstract Uneven distribution of the electric field and zinc ion (Zn ²⁺ ), and crosstalk effects all lead to irreversible redox of Zn, eventually accelerating the failure of various Zn‐metal energy storage devices, especially Ah‐scale pouch batteries. This study pioneers a strategy to dynamically regulate electrons and Zn ²⁺ ions for uniform Zn redox, in which a series of additive molecules with varying electron delocalized spaces is designed to verify this dynamic regulation mechanism. Due to the large electron delocalized space, the additives with delocalized π‐bonds and ‒COOH form a stable molecular layer for the Zn anode. This layer can effectively prevent side reactions and dynamically regulate the arrangement of electrons and Zn ²⁺ ions by driving electrons to flow among conjugated atoms and functional groups, ultimately evening out the electric field and reaction sites of Zn ²⁺ ions during the Zn redox process. Thanks to this dynamic regulation, the Ah‐scale Zn//I ₂ pouch cell exhibits a high capacity of 1.473 Ah (188.7 Wh kg ⁻¹ ) at 2 mA cm ⁻² and outstanding rate performance. This dynamic regulation also presents great compatibility with Zn‐manganese pouch cells and Zn‐bromine cells. This work deepens the understanding of the regulation mechanism for highly reversible Ah‐scale AZIBs.