Abstract
<h2>Summary</h2> The capture of radioiodine species during nuclear fuel reprocessing and nuclear accidents is crucial for nuclear safety, environmental protection, and public health. Previously reported emerging materials for iodine uptake cannot outperform commercial zeolites and active carbon under the practical dynamic scenario. Herein, we present a new design philosophy aiming at significantly enhanced specific host-guest interactions and obtain a nitrogen-rich covalent organic framework material by introducing a bipyridine group into the building block for the simultaneous capture of both iodine gas through enhanced electron-pair effect and organic iodide via the methylation reaction. These efforts give rise to not only an ultrahigh uptake capacity of 6.0 g g<sup>−1</sup> for iodine gas and a record-high value of 1.45 g g<sup>−1</sup> for methyl iodide under static sorption conditions but also, more importantly, a record-high iodine loading capability under dynamic conditions demonstrated from the breakthrough experiments.
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