Regulating triazine number in covalent organic frameworks modified separator to achieve high-energy-density performance in aqueous zinc-iodine batteries.

The development of separator by tunning the zincophilic and iodide ion-repulsive properties of covalent organic frameworks (COFs) that regulate cycle lifespan and capacity of aqueous zinc-iodine (Zn-I) batteries is one of challenges. In this work, we have shown a systematic strategic-driven investigation to elucidate the role of functional triazine properties in COF modified separator towards overall performance of aqueous Zn-I batteries. As such, three COFs with the same topology but different triazine number in their structures, have been synthesized, among which the triazine-richest framework, TAPA-TTB-COF-based separator demonstrated to be most effective to guide uniform Zn flux and simultaneously inhibit polyiodide shuttling due to the zincophilic nature and good iodide ion-repulsive capability of triazine. Consequently, the Zn||Gr@TAPA-TTB-COF@GF||Zn symmetric battery achieves a long life of more than 2100 h (5.0 mA cm) and the initial area capacity of the Zn||Gr@TAPA-TTB-COF@GF||I battery reaches up to 5.5 mAh cm (20 mA cm). After 2000 cycles, the discharge capacity can still maintain at3.0 mAh cm with a capacity decay rate of only 0.023 % per cycle. This study provides guidance for the rational design of functional COFs separators and promotes their application in high energy storage systems.