Kritanan Junthod, Bunyaporn Todee, Korawit Khamphaijun, Threeraphat Chutimasakul, Tanagorn Sangtawesin, Thanchanok Ratvijitvech, Jonggol Tantirungrotechai, Utid Suriya and Thanthapatra Bunchuay*,
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引用次数: 0
Abstract
Radioactive iodine species, 129I and 131I, are volatile radioactive nuclides generated from nuclear fission processes. The exposure of these isotopes has caused severe effects on the environment as a result of the long half-life of 129I and high radiation energy of 131I. Therefore, ideal adsorbents capable of effectively adsorbing iodine from gas and solution phases have received particular attention. In this study, we applied the concept of supramolecular noncovalent interactions to design the functional polymeric adsorbents for efficient iodine removal. A series of nitrogen-functionalized hyper-crosslinked polymers (HCPs) containing hydrazine (P-Hz), azide (P-Az), and amine (P-Am) were synthesized from the reactive tosylated HCP (P-OTs) through facile organic transformations. After being characterized by Fourier transform infrared (FTIR), thermogravimetric analysis (TGA), UV–vis, scanning electron microscopy (SEM), and Brunauer–Emmett–Teller (BET) surface area analysis, iodine adsorption in the gas phase and solutions was investigated, and the results revealed that the interplay between the electron-donating ability of nitrogen functional groups of HCPs and the molecular iodine (I2) resulted in enhanced iodine adsorption compared to the nitrogen-free HCPs. Density functional theory (DFT) computational studies and UV–visible spectroscopic titrations revealed the formation of the N···I–I halogen bonding, where the electron-donating nature of nitrogen in hydrazine, azide, and amine, as well as the solvent medium, significantly governed the strength of interactions. Importantly, P-Am exhibited a high iodine adsorption capacity of 2.83 g·g–1 in the gas phase and 506.8 mg·g–1 in the hexane phase, albeit with low porosity, suggesting the importance of specific functional groups in the adsorption capacity. X-ray fluorescence (XRF) and Raman spectroscopic analysis of P-Am after iodine adsorption suggested that iodine species are stabilized on the polymer matrix in the form of polyiodides such as I3– and I5–.
期刊介绍:
ACS Applied Polymer Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics, and biology relevant to applications of polymers.
The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrates fundamental knowledge in the areas of materials, engineering, physics, bioscience, polymer science and chemistry into important polymer applications. The journal is specifically interested in work that addresses relationships among structure, processing, morphology, chemistry, properties, and function as well as work that provide insights into mechanisms critical to the performance of the polymer for applications.