Engineering the pore environment of antiparallel stacked covalent organic frameworks for capture of iodine pollutants

Yinghui Xie, Qiuyu Rong, Fengyi Mao, Shiyu Wang, You Wu, Xiaolu Liu, Mengjie Hao, Zhongshan Chen, Hui Yang (), Geoffrey I. N. Waterhouse, Shengqian Ma () and Xiangke Wang ()
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Yinghui Xie: North China Electric Power University
Qiuyu Rong: North China Electric Power University
Fengyi Mao: North China Electric Power University
Shiyu Wang: North China Electric Power University
You Wu: North China Electric Power University
Xiaolu Liu: North China Electric Power University
Mengjie Hao: North China Electric Power University
Zhongshan Chen: North China Electric Power University
Hui Yang: North China Electric Power University
Geoffrey I. N. Waterhouse: The University of Auckland
Shengqian Ma: University of North Texas
Xiangke Wang: North China Electric Power University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Radioiodine capture from nuclear fuel waste and contaminated water sources is of enormous environmental importance, but remains technically challenging. Herein, we demonstrate robust covalent organic frameworks (COFs) with antiparallel stacked structures, excellent radiation resistance, and high binding affinities toward I2, CH3I, and I3− under various conditions. A neutral framework (ACOF-1) achieves a high affinity through the cooperative functions of pyridine-N and hydrazine groups from antiparallel stacking layers, resulting in a high capacity of ~2.16 g/g for I2 and ~0.74 g/g for CH3I at 25 °C under dynamic adsorption conditions. Subsequently, post-synthetic methylation of ACOF-1 converted pyridine-N sites to cationic pyridinium moieties, yielding a cationic framework (namely ACOF-1R) with enhanced capacity for triiodide ion capture from contaminated water. ACOF-1R can rapidly decontaminate iodine polluted groundwater to drinking levels with a high uptake capacity of ~4.46 g/g established through column breakthrough tests. The cooperative functions of specific binding moieties make ACOF-1 and ACOF-1R promising adsorbents for radioiodine pollutants treatment under practical conditions.

Date: 2024
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DOI: 10.1038/s41467-024-46942-0

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