Dynamic Dipole‐Flipping Interlayer: Switchable Molecular‐Level Electric Field Enables Full‐Cycle Stable Zinc Anodes

ABSTRACT Nonuniform Zn 2+ flux, which triggers dendritic growth and accompanying side reactions, severely bottlenecks the practical implementation of aqueous zinc‐ion batteries. While the interfacial electric field governs Zn 2+ flux uniformity, existing modulation strategies rely on static unidirectional fields remains intrinsically decoupled from the bidirectional, field‐reversing dynamics of cyclic Zn deposition/stripping. Herein, we engineer a dynamic dipole‐flipping interlayer (DDL) on Zn anode that generates a switchable molecular‐level electric field to enable uniform Zn 2+ flux regulation during cycling. Specifically, the DDL is constructed from a rationally designed polyamide derivative featuring inherently large amide dipole moments; increased free volume and chain flexibility disrupt dense chain packing and enable rapid, reversible dipole reorientation. During Zn deposition/stripping, the amide dipoles reorient dynamically to generate polarity‐switchable interfacial molecular‑level electric fields, which direct homogeneous Zn 2+ redistribution and suppress preferential nucleation. Beyond electric‑field regulation, fluorinated segments within the DDL impart interfacial hydrophobicity and further suppress side reactions. Consequently, the DDL‐modified Zn anode cycles stably for over 3200 h at 0.5 mA cm −2 , while the Zn||MnO 2 full cell delivers 97.3% capacity retention after 1600 cycles at 1 A g −1 . This work pioneers a versatile paradigm for interfacial electric field regulation by dipole dynamics toward high‐performance aqueous metal‐based batteries.