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通过分子膨胀构建新型超交联共轭聚合物以增强气体吸附性能。

Constructing novel hyper-crosslinked conjugated polymers through molecular expansion for enhanced gas adsorption performance.

作者信息

Shang Qigao, Cheng Yuhao, Gong Zhenpeng, Yan Ying, Han Bo, Liao Guiying, Wang Dongsheng

机构信息

Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China.

Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430074, China.

出版信息

J Hazard Mater. 2022 Mar 15;426:127850. doi: 10.1016/j.jhazmat.2021.127850. Epub 2021 Nov 20.

DOI:10.1016/j.jhazmat.2021.127850
PMID:34836684
Abstract

The porous organic polymers have been considered as effective materials for gas storage and adsorption. Herein, we synthesized highly crystalline nitrogen-rich covalent triazine frameworks (CTFs) by polycondensation for preparing the novel hyper-cross-linked conjugated polymers (HCCPs) with tunable specific surface area and pore volume through coupling Friedel-Crafts reaction, in which 1,4-Bis(chloromethyl)benzene and 4,4-Bis(chloromethyl)biphenyl as the expansion molecules were pillared between the layers of CTF-HUST. This technology not only increased the specific surface area and total pore volume of CTF-HUST by 2.56 and 4.68 times, but also greatly enhanced the utilization of adsorption sites of CTF-HUST. The HCCP2-1.25 exhibited the highest surface area (1349.29 mg) among these HCCPs and demonstrated excellent adsorption performance for ethyl acetate (1605.14 mg/g), ethanol (1371.49 mg/g), 1,2-Dichloroethane (1971.68 mg/g), benzene (1151.77 mg/g) and toluene (1024.28 mg/g) due to the multiple C-H…O, C-H…Cl, O-H…N and C-H…π interactions between volatile organic compounds (VOCs) and HCCPs framework. Moreover, CO and H storage capacities of the HCCP2-1.25 were 8.02 wt% and 1.54 wt%, 1.66 and 1.67 times higher than CTF-HUST, respectively. This study developed a simple and effective molecular expansion strategy to synthesize a series of novel high-surface-area porous polymers for potential applications in the environmental field.

摘要

多孔有机聚合物被认为是用于气体存储和吸附的有效材料。在此,我们通过缩聚反应合成了高度结晶的富氮共价三嗪框架(CTFs),通过傅克反应偶联制备具有可调比表面积和孔体积的新型超交联共轭聚合物(HCCPs),其中1,4-双(氯甲基)苯和4,4-双(氯甲基)联苯作为扩链分子被支撑在CTF-HUST层间。该技术不仅使CTF-HUST的比表面积和总孔体积分别增加了2.56倍和4.68倍,还大大提高了CTF-HUST吸附位点的利用率。在这些HCCPs中,HCCP2-1.25表现出最高的表面积(1349.29 m²/g),并对乙酸乙酯(1605.14 mg/g)、乙醇(1371.49 mg/g)、1,2-二氯乙烷(1971.68 mg/g)、苯(1151.77 mg/g)和甲苯(1024.28 mg/g)表现出优异的吸附性能,这归因于挥发性有机化合物(VOCs)与HCCPs框架之间存在多种C-H…O、C-H…Cl、O-H…N和C-H…π相互作用。此外,HCCP2-1.25的CO和H存储容量分别为8.02 wt%和1.54 wt%,分别比CTF-HUST高1.66倍和1.67倍。本研究开发了一种简单有效的分子扩链策略,以合成一系列新型高比表面积多孔聚合物,用于环境领域的潜在应用。

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