Introgression of Lone Electron Pairs into π-Conjugated Structures Resulting in Giant Electron-Rich Clusters with High Trapping Capacity for Iodine Molecules

IF 4.4 2区 化学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Yu Ji, Jinbin Huang, Chao Liu*, Cailing Ni*, Hewei Yan, Yekeh David and Yuancheng Qin*, 
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Abstract

Effective removal of radioactive iodine from fission is of great importance, whereas adsorption of iodine by porous organic polymers provides an effective adsorption method and remains an active research topic. Here, three porous organic polymers (POPs), were designed and synthesized by introducing N, S heteroatomic groups using Schiff base condensation reaction to examine their iodine adsorption ability. Excellent iodine adsorption capacity was demonstrated for the three prepared POPs, not only in the fast and reversible volatile iodine uptake of up to 510–543 wt % but also in the cyclohexane solution with high iodine adsorption capacity of 504.4, 664.6, and 537.4 mg g–1, respectively. Nitrogen and sulfur elements, as well as the π-conjugated structure of sp2 hybridization, formed huge electron-rich clusters, enticing the attraction of electron-deficient I2 molecules to form polyiodide anions (I3 and I5). On top of that, the lone pair of electrons and π-conjugation of the heteroatoms led to a high binding capacity between the adsorbent and the iodo Lewis acid molecules, contributing to a significant increase in the adsorption rate and removal efficiency of I2. In conclusion, this is a useful strategy for developing POPs to remove iodine.

Abstract Image

Abstract Image

将孤电子对引入π共轭结构,形成对碘分子具有高捕获能力的巨型富电子团簇
有效去除裂变产生的放射性碘非常重要,而多孔有机聚合物对碘的吸附提供了一种有效的吸附方法,目前仍是一个活跃的研究课题。本文利用希夫碱缩合反应,通过引入 N、S 杂原子基团,设计合成了三种多孔有机聚合物(POPs),并考察了它们的碘吸附能力。结果表明,所制备的三种持久性有机污染物都具有出色的碘吸附能力,不仅在快速、可逆的挥发性碘吸收中的吸附能力高达 510-543 wt %,而且在环己烷溶液中的吸附能力也很高,分别为 504.4、664.6 和 537.4 mg g-1。氮和硫元素以及 sp2 杂化的π-共轭结构形成了巨大的富电子团簇,吸引缺电子的 I2 分子形成聚碘阴离子(I3- 和 I5-)。此外,杂原子的孤对电子和π共轭作用使吸附剂与碘路易斯酸分子之间具有很高的结合能力,从而显著提高了对 I2 的吸附率和去除效率。总之,这是开发持久性有机污染物去除碘的一种有用策略。
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来源期刊
CiteScore
7.20
自引率
6.00%
发文量
810
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.
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