Achieving Stable\nOrientational Zinc Deposition for\nReversible Zinc Anode through Supramolecular Anchoring Mechanism

Aqueous zinc-ion batteries have been impeded by the hydrogen\nevolution\nreaction (HER), uncontrolled zinc dendrites, and side reactions on\nthe Zn anode. In this work, a Zn–polyphenol supramolecular\nnetwork is rationally designed for stabilizing Zn anodes (ZPN@Zn)\neven at high current density. Theoretical calculations and experiments\nshow that the zinc–polyphenol supramolecular layer effectively\ninhibits the hydrogen evolution reaction by capturing water molecules\nthrough strong hydrogen bonding networks while also facilitating the\nrapid replenishment of Zn<sup>2+</sup> ions at the interface through\nsupramolecular anchoring. Additionally, it results in preferential\ndeposition of Zn on the (002) plane, thereby contributing to nondendritic\nand highly reversible Zn plating/stripping behaviors even under high\nrates. Concomitantly, the ZPN@Zn achieves superior stability of nearly\n1200 h at a high current density of 20 mA cm<sup>–2</sup> and\nmaintains a high CE efficiency of 99.86% after 3000 cycles at 1 mAh\ncm<sup>–2</sup> and 5 mA cm<sup>–2</sup>. Remarkably,\nthe full cell assembled with ZPN@Zn and NaV<sub>3</sub>O<sub>8</sub> (NVO) endures 25 000 cycles at 20 A g<sup>–1</sup>, achieving an impressive performance for the realization of dendrite-free\nZn anodes by supramolecular modulation.