Inter‐molecular Channel Gated Ion Migration for High Performance Zinc‐ion Batteries

ABSTRACT Aqueous zinc‐ion batteries (AZIBs) are plagued by dendrite growth and parasitic side reactions, which severely hinder their stable operation. Inspired by carrier proteins, amphiphilic surfactants are introduced as ion channel mediators. During zinc deposition, the cationic surfactants preferentially adsorb onto the zinc surface through their headgroups and self‐assemble into ordered ion channels, thereby guiding dense and uniform Zn 2+ flux. The ion channeling capability of cationic surfactants with various alkyl chain lengths is systematically investigated. Decyltrimethylammonium chloride, possessing the optimal chain length, is subsequently selected to construct efficient ion channels. Its moderate alkyl length enables the formation of stable ion channels that regulate the electric double layer (EDL) environment and promote directional zinc deposition. Benefiting from the ion‐regulating strategy, Zn||Cu asymmetric cells achieve an average Coulombic efficiency as high as 99.58% over 3000 cycles. Meanwhile, Zn||Zn symmetric cells operate stably for over 800 h under harsh conditions of 10 mA cm −2 with 10 mAh cm −2 . The assembled Zn||VO 2 pouch cell demonstrates impressive cycling stability over 300 cycles. This work provides a new perspective on surfactant‐enabled dendrite suppression and offers a low‐cost and highly effective solution for the practical development of AZIBs.