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 Cu 2+ 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 Zn 2+ transport along the framework channels, while the porous architecture restricts [Zn(H 2 O) 6 ] 2+ passage, accelerating desolvation and suppressing side reactions. Meanwhile, Cu 2+ 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 Zn 2+ migration. This work offers an interfacial design strategy and theoretical insight for the development of high-performance zinc-based batteries.