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用于从水中高效捕获碘的新型两性离子超交联聚合物的合成

Synthesis of a Novel Zwitterionic Hypercrosslinked Polymer for Highly Efficient Iodine Capture from Water.

作者信息

Yu Jingwen, Song Luna, Han Bingying, Hu Jiangliang, Li Zhong, Mi Jie

机构信息

State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China.

Key Laboratory of Coal Science and Technology, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China.

出版信息

Polymers (Basel). 2024 Oct 9;16(19):2846. doi: 10.3390/polym16192846.

DOI:10.3390/polym16192846
PMID:39408556
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11478924/
Abstract

Cationic porous organic polymers have a unique advantage in removing radioactive iodine from the aqueous phase because iodine molecules exist mainly in the form of iodine-containing anions. However, halogen anions will inevitably be released into water during the ion-exchange process. Herein, we reported a novel and easy-to-construct zwitterionic hypercrosslinked polymer (7AIn-PiP)-containing cationic pyridinium-type group, uncharged pyridine-type group, pyrrole-type group, and even an electron-rich phenyl group, which in synergy effectively removed 94.2% (456 nm) of I from saturated I aqueous solution within 30 min, surpassing many reported iodine adsorbents. Moreover, an I adsorption efficiency of ~95% can still be achieved after three cyclic evaluations, indicating a good recycling performance. More importantly, a unique dual 1,3-dipole was obtained and characterized by H/C NMR, HRMS, and FTIR, correlating with the structure of 7AIn-PiP. In addition, the analysis of adsorption kinetics and the characterization of I@7AIn-PiP indicate that the multiple binding sites simultaneously contribute to the high affinity towards iodine species by both physisorption and chemisorption. Furthermore, an interesting phenomenon of inducing the formation of HIO in unsaturated I aqueous solution was discovered and explained. Overall, this work is of great significance for both material and radiation protection science.

摘要

阳离子多孔有机聚合物在从水相中去除放射性碘方面具有独特优势,因为碘分子主要以含碘阴离子的形式存在。然而,在离子交换过程中,卤素阴离子不可避免地会释放到水中。在此,我们报道了一种新型且易于构建的两性离子超交联聚合物(7AIn-PiP),它含有阳离子吡啶型基团、不带电荷的吡啶型基团、吡咯型基团,甚至还有富电子苯基,这些基团协同作用,在30分钟内可有效从饱和碘水溶液中去除94.2%(456纳米)的碘,超过了许多已报道的碘吸附剂。此外,经过三次循环评估后,仍可实现约95%的碘吸附效率,表明其具有良好的循环性能。更重要的是,通过氢碳核磁共振、高分辨质谱和傅里叶变换红外光谱获得并表征了一种独特的双1,3-偶极,这与7AIn-PiP的结构相关。此外,吸附动力学分析和碘@7AIn-PiP的表征表明,多个结合位点通过物理吸附和化学吸附同时对碘物种具有高亲和力。此外,还发现并解释了在不饱和碘水溶液中诱导形成次碘酸的有趣现象。总的来说,这项工作对材料科学和辐射防护科学都具有重要意义。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/ab7981a2b138/polymers-16-02846-g011.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/f5afcc08c250/polymers-16-02846-sch003.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/ed3338218811/polymers-16-02846-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/2ac90f630089/polymers-16-02846-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/c6610ebf59ce/polymers-16-02846-sch004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/f90f0b92a7f4/polymers-16-02846-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/85ed3ee40564/polymers-16-02846-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/ab7981a2b138/polymers-16-02846-g011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/fc7572ecf710/polymers-16-02846-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/45ce54d13d5e/polymers-16-02846-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/7d3eb3eab51b/polymers-16-02846-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/475b13ae66ba/polymers-16-02846-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/0dba6c1c1159/polymers-16-02846-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/10eb53e65f58/polymers-16-02846-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/93eeb8954b4f/polymers-16-02846-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/f5afcc08c250/polymers-16-02846-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/ab1174580cc4/polymers-16-02846-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/ed3338218811/polymers-16-02846-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/2ac90f630089/polymers-16-02846-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/c6610ebf59ce/polymers-16-02846-sch004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/f90f0b92a7f4/polymers-16-02846-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/85ed3ee40564/polymers-16-02846-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ce79/11478924/ab7981a2b138/polymers-16-02846-g011.jpg

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本文引用的文献

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The paradigm for exceptional iodine capture by nonporous amorphous electron-deficient cyclophanes.无孔缺电子环番对碘的卓越捕获模式。
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Recent progress in iodine capture by macrocycles and cages.大环化合物和笼状化合物捕获碘的最新进展。
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A Cucurbit[8]uril-Based Supramolecular Framework Material for Reversible Iodine Capture in the Vapor Phase and Solution.一种基于葫芦[8]脲的超分子框架材料,用于在气相和溶液中可逆捕获碘。
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Structural Modulation of Nitrogen-Rich Covalent Organic Frameworks for Iodine Capture.用于碘捕获的富氮共价有机框架的结构调控
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Synthesis of a Triazaisotruxene-Based Porous Organic Polymer and Its Application in Iodine Capture.基于三嗪并薁的多孔有机聚合物的合成及其在碘捕获中的应用。
Molecules. 2022 Dec 9;27(24):8722. doi: 10.3390/molecules27248722.
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Multi-Functionalization Integration into the Electrospun Nanofibers Exhibiting Effective Iodine Capture from Water.多功能化集成到具有从水中有效捕获碘能力的电纺纳米纤维中。
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