Unveiling the Role of Cationic Pyridine Sites in Covalent Triazine Framework for Boosting Zinc-Iodine Batteries Performance.

Abstract

Rechargeable Zinc-iodine batteries (ZIBs) are gaining attention as energy storage devices due to their high energy density, low-cost, and inherent safety. However, the poor cycling performance of these batteries always arises from the severe leakage and shuttle effect of polyiodides (I3 - and I5 -). Herein, a novel cationic pyridine-rich covalent triazine framework (CCTF-TPMB) is developed to capture and confine iodine (I2) species via strong electrostatic interaction, making it an attractive host for I2 in ZIBs. The as-fabricated ZIBs with I2 loaded CCTF-TPMB (I2@CCTF-TPMB) cathode achieve a large specific capacity of 243mAhg-1 at 0.2Ag-1 and an exceptionally stable cyclic performance, retaining 93.9% of its capacity over 30000 cycles at 5Ag-1. The excellent electrochemical performance of the ZIBs can be attributed to the pyridine-rich cationic sites of CCTF-TPMB, which effectively suppress the leakage and shuttle of polyiodides, while also accelerating the conversion reaction of I2 species. Combined in situ Raman and UV-vis analysis, along with theoretical calculations, clearly reveal the critical role played by pyridine-rich cationic sites in boosting the ZIBs performances. This work opens up a promising pathway for designing advanced I2 cathode materials toward next-generation ZIBs and beyond.