The development of covalent organic polymers (COPs) to remove iodine in vapor and from solutions is highly desirable for the sustainable production of nuclear energy. Herein, we reported the successful synthesis of ionic COPs (iCOPs) via a post-synthesis functionalization approach. Subsequently, magnetically responsive iCOPs (IMF-COP-Fe) were obtained using a simple double-solvent reduction method to facilitate separation. It was noteworthy that IMF-COP-Fe could rapidly achieve solid-liquid separation under the influence of an external magnetic field, with a magnetic recovery rate of 91.89%. The rational design endowed IMF-COP-Fe with affinity sites for both iodine in vapor and from solutions. Experimental findings demonstrated that the adsorption capacity of IMF-COP-Fe towards iodine vapor was 2.46 g g–1 at 75°C. Concurrently, the iodine removal rate of IMF-COP-Fe in 700 mg L–1 iodine-cyclohexane solution attained 80.56%. Even after four adsorption-desorption experiments, it still maintained good adsorption performance. Furthermore, the maximum adsorption capacity of IMF-COP-Fe for iodide ions was found to be 109.9 mg g–1. The present study proposes original concepts for the rational molecular design materials for simultaneous removal various forms of radioactive iodine.

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