Aqueous zinc-bromine batteries can fulfil the energy storage requirement for sustainable techno-scientific advancement owing to its intrinsic safety and cost-effectiveness. Nevertheless, the uncontrollable zinc dendrite growth and spontaneous shuttle effect of bromine species have prohibited their practical implementation. Herein, we develop an aqueous zinc-bromine battery integrated with the exfoliated covalent organic framework (exCOF)-bromine cathode and COF-coated zinc metal anode. As verified by experimental and theoretical investigations, exCOF with abundant functional groups exhibits strong adsorption toward Br species, therefore immobilizes Br species and facilitates bidirectional conversion of polybromide. Meanwhile, the COF artificial layer on the surface of zinc metal anode can effectively regulate zinc flux and enable the uniform Zn deposition without dendrite growth. Consequently, owing to the synergistic effect of both COF-Zn anode and Br₂-exCOF cathode, the as-assembled COF-Zn||Br₂-exCOF full cell can deliver a remarkable capacity of ∼183 mAh g^-1 (∼0.61 mAh cm^-2) after 1000 cycles with capacity retention of ∼83 % at 2 A g^-1 and high Coulombic efficiency of ∼99 %. Ultimately, this work can inspire insight into developing high-performance aqueous zinc-bromine battery systems.

由于其固有的安全性和成本效益，水系锌溴电池可以满足可持续技术科学进步的储能要求。然而，溴物种的不可控制的锌枝晶生长和自发穿梭效应阻碍了它们的实际应用。在此，我们开发了一种与剥离共价有机骨架 (exCOF)-溴正极和 COF 涂层锌金属负极集成的水系锌溴电池。实验和理论研究证实，具有丰富官能团的 exCOF 对 Br 物种表现出很强的吸附性，因此可以固定 Br 物种并促进多溴化物的双向转化。同时，锌金属阳极表面的COF人工层能有效调节锌通量，使锌沉积均匀，无枝晶生长。因此，由于 COF-Zn 阳极和 Br 的协同作用₂ -exCOF正极，组装后的COF-Zn||Br ₂ -exCOF全电池在1000次循环后可提供~183 mAh g ^-1 (~0.61 mAh cm ^-2 )的显着容量，容量保持率为~83 %在 2 A g ^-1和约 99 % 的高库仑效率下。最终，这项工作可以激发对开发高性能水性锌溴电池系统的洞察力。