Zhendong Hao, Jiadong Tang, Shihai Cao, Wenyao Zhang, Huimin Yin, Wenjie Li, Yu Xiang Fu, Yinghao Li, Qianqian Zhang, Mingyue Zheng, Yuntong Sun, Jong‐Min Lee
Aqueous energy storage and conversion systems (AESCS) offer a cost-effective and safe alternative to conventional energy storage technologies. Among their key components, separators with high ionic selectivity are crucial for maximizing the energy output and ensuring long-term stability. Covalent organic frameworks, a class of nanoporous materials with tunable functional groups, are promising candidates for AESCS. Herein, we design and synthesize TP-4KT, which is coated onto a commercial glass fiber separator (TP-4KT@GF) to realize ion selectivity. The performance of TP-4KT@GF is evaluated in two representative AESCS: concentration cells and aqueous zinc-ion batteries (AZIBs). The modified separator achieves a high cation transference number (0.71) and a power density of 33.18 W m –2 in concentration cells, while effectively suppressing dendrite formation and improving electrochemical stability in AZIBs. This study provides valuable insights into the development of functional ion-sieving separators for next-generation energy storage and conversion technologies.