Developing
efficient adsorbent materials for iodine scavenging
is essential to mitigate the threat of radioactive iodine causing
adverse effects on human health and the environment. In this context,
we explored N-rich two-dimensional covalent organic frameworks (COFs)
with diverse functionalities for iodine capture. The pyridyl-hydroxyl-functionalized
triazine-based novel 5,5′,5″-(1,3,5-triazine-2,4,6-triyl)tris(pyridine-2-amine)
(TTPA)-COF possesses high crystallinity (crystalline domain size:
24.4 ± 0.6 nm) and high porosity (specific BET surface area:
1000 ± 90 m2 g–1). TTPA-COF exhibits
superior vapor-phase iodine adsorption (4.43 ± 0.01 g g–1) compared to analogous COF devoid of pyridinic moieties, 2,4,6-tris(4-aminophenyl)-1,3,5-triazine
(TAPT)-COF. The high iodine capture by TTPA-COF is due to the enhanced
binding affinity conferred by the extra pyridinic active sites. Furthermore,
the crucial role of long-range order in porous adsorbents has been
experimentally evidenced by comparing the performance of iodine vapor
capture of TTPA-COF with an amorphous network polymer having identical
functionalities. We have also demonstrated the high iodine scavenging
ability of TTPA-COF from the organic and aqueous phases. The mechanism
of iodine adsorption by the heteroatom-rich framework is elucidated
through FTIR, XPS, and Raman spectral analyses. The present study
highlights the need for structural tweaking of the building blocks
toward the rational construction of advanced functional porous materials
for a task-specific application.