N‐Rich Tris(triazole)‐Based 2D Conjugated Metal‐Organic Framework for High Performance Aqueous Dual‐Ion Batteries

Two‐dimensional conjugated metal‐organic frameworks (2D c ‐MOFs) have emerged as promising host materials of iodine species for aqueous dual‐ion batteries (ADIBs) due to their well‐defined pore structures, abundant electrophilic active sites, and chemical functionality. Herein, we report two new tris( N ‐phenyl)triazole‐based 2D c ‐MOFs (TPT‐M‐MOF, M═Cu, Zn), in which the synergistic interaction between N‐rich sites and [MO 4 ] centers with I 3 − species is identified as the key factor responsible for significantly enhanced performance of ADIBs. Especially, TPT‐Zn‐MOF exhibits a higher specific capacity of 435 mAh g −1 at 1 A g −1 over 1000 stable cycling cycles at 5 A g −1 than its isostructural analogue TPT‐Cu‐MOF. Meanwhile, spectral characterization and theoretical calculations demonstrated that the battery performance strongly depends on the N‐rich skeleton and the coordinated metal centers. Therefore, rational design of N‐rich 2D c ‐MOFs holds great promise for advancing the development of host materials of iodine species for next‐generation ADIBs.