Multiple-Synergistic Interfacial Layer Enabled by a Porous Aromatic Framework for Dendrite-Free Zinc Deposition in Ultrastable Zinc-Ion Batteries

The uncontrolled growth of dendritic zinc remains a major challenge hindering the practical deployment of zinc-ion batteries (ZIBs), highlighting the need for dendrite-free zinc anodes. Herein, we construct a porous aromatic framework, Cu@PAF-STB, rich in hydroxyl (−OH) groups and anchored with Cu2+ ions, as an artificial interfacial layer on the zinc anode. This layer enables uniform zinc deposition through a multiple-synergistic mechanism, significantly enhancing cycling stability. Specifically, the abundant −OH functional groups facilitate directional Zn2+ transport along the framework channels, while the porous architecture restricts [Zn(H2O)6]2+ passage, accelerating desolvation and suppressing side reactions. Meanwhile, Cu2+ ions induce in situ formation of a Zn–Cu alloy, providing a stable and zincophilic interface that promotes uniform nucleation and the growth of zinc. Consequently, symmetric cells exhibit an ultralong cycling life exceeding 6600 h, and full cells retain a high reversible capacity of 111 mAh·g–1 after 1000 cycles at 3.0 A·g–1. Theoretical evaluation further confirms, at the atomic scale, the cooperative role of each component in lowering the desolvation energy barrier and optimizing Zn2+ migration. This work offers an interfacial design strategy and theoretical insight for the development of high-performance zinc-based batteries.