Robust Imidazopyridinium Covalent Organic Framework as Efficient Iodine Capturing Materials in Gaseous and Aqueous Environment

Abstract The development of a high‐performing adsorbent that can capture both iodine vapor from volatile nuclear waste and traces of iodine species from water is an important challenge, especially in industrially relevant process conditions. This study introduces novel imidazopyridinium‐based covalent organic frameworks (COFs) through post‐modification of a picolinaldehyde‐based imine COF. These COFs demonstrate excellent iodine adsorption capacity, adsorption kinetics, and a high stability/recyclability in both vapor and water phases. Notably, one imidazopyridinium COF exhibits gaseous iodine uptake of 21 wt.% under dynamic adsorption conditions at 150 °C and a relative humidity of 50%, surpassing the performance of the currently used silver‐based zeolite adsorbents (Ag@MOR (17wt.%)). Additionally, the same imidazopyridinium COFs can efficiently remove iodine species at a low concentration from aqueous solution. Seawater containing triiodide ions treated under dynamic flow‐through conditions resulted in decreased concentrations down to the ppb level. The adsorption mechanisms for iodine and polyiodide species are elucidated for the imine COF and imidazopyridinium COFs; involving halogen bonding, hydrogen bonding, and charge‐transfer complexes.