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通过弱分子间力实现高效去除放射性碘甲烷和极性非质子有机化合物的含SuFEx弹性聚硫酸盐

SuFEx-Enabled Elastic Polysulfates for Efficient Removal of Radioactive Iodomethane and Polar Aprotic Organics through Weak Intermolecular Forces.

作者信息

Wan Haibo, Xu Qingfeng, Wu Jiacheng, Lian Cheng, Liu Honglai, Zhang Bing, He Jinghui, Chen Dongyun, Lu Jianmei

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou, Jiangsu 215123, China.

School of Chemistry and Molecular Engineering, East China University of Science and Technology, China.

出版信息

Angew Chem Int Ed Engl. 2022 Aug 15;61(33):e202208577. doi: 10.1002/anie.202208577. Epub 2022 Jul 11.

DOI:10.1002/anie.202208577
PMID:35751405
Abstract

Capturing radioactive iodomethane and its vapors is a major challenge due to its low adsorption capacity. Herein, we have developed for the first time a pyridine-entrapped elastic crosslinked polysulfate gel (pyridine/TPC-cPS) as an efficient absorbent for iodomethane capture. Each pyridine-encased TPC-cPS network cell acts as a mini-reactor for salt formation between pyridine and iodomethane. The yield reaches up to 96.65 % and traps saturated iodomethane vapor of 1.573 g g (equivalent to 18.103 g g ), which is the highest capacity reported to date. Both experiments and molecular dynamics simulations reveal that the unusual adsorption of polysulfate for polar aprotic organics can be attributed to the fact that the electrostatic interactions between the polar group (O=S=O) in the polymer backbone and the polar groups in the organic molecules fixed the solvent in the polymer matrix, while the van der Waals forces between the nonpolar groups in the polymer and molecules induced swelling.

摘要

由于碘甲烷的吸附容量低,捕获放射性碘甲烷及其蒸气是一项重大挑战。在此,我们首次开发了一种吡啶包裹的弹性交联聚硫酸盐凝胶(吡啶/TPC-cPS)作为捕获碘甲烷的高效吸收剂。每个包裹吡啶的TPC-cPS网络单元充当吡啶与碘甲烷之间形成盐的微型反应器。产率高达96.65%,可捕获1.573 gg(相当于18.103 gg)的饱和碘甲烷蒸气,这是迄今为止报道的最高容量。实验和分子动力学模拟均表明,聚硫酸盐对极性非质子有机化合物的异常吸附可归因于聚合物主链中的极性基团(O=S=O)与有机分子中的极性基团之间的静电相互作用将溶剂固定在聚合物基质中,而聚合物中的非极性基团与分子之间的范德华力导致溶胀。

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