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 [MO₄] centers with I₃ ^- 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.