Synthesis of “all-in-one” hypercrosslinked organic polymers: experimental and kinetic models for CO2 chemical fixation and iodine adsorption†

IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Sustainable Energy & Fuels Pub Date : 2024-08-23 DOI:10.1039/D4SE01033G
Xuanbo Liu, Yongjing Hao, Xiuli Yan, Yuhang Zhang, Xionglei Wang, Zheng Zhu, Jiajia Yang, Shuangshuo Li, Tao Chang and Shenjun Qin
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Abstract

A series of “all-in-one” hypercrosslinked polymers (HCPOH-Cn) have been synthesized by Friedel–Crafts alkylation of phenols tethered with adjustable alkyl chains and the quaternization reaction of N,N-dimethylethylenediamine in one-pot in the presence of dibromomethylbenzene as the crosslinking and ammonium agent. After characterization, the polymers were implemented for sustainable CO2 conversion and iodine adsorption. The experimental results showed that HCPOH-C12 can effectively catalyze the CO2 cycloaddition reaction, and an excellent yield of 94% was confirmed after optimizing the conditions. The outstanding activity is attributed to the lower activation energy (69.52 kJ mol−1). The polymer of HCPOH-C12 exhibits excellent substrate adaptability and recyclability, and a possible catalytic mechanism has been proposed. Furthermore, HCPOH-C0 has showcased an impressive adsorption capacity for iodine, with the process aligning well with second-order adsorption kinetics and conforming to Langmuir adsorption isotherms. Iodine adsorption on HCPOH-C0 is characterized as a spontaneous and endothermic process, indicative of an increase in the disorder at the solid–liquid interface during the adsorption phase.

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一体化 "超交联有机聚合物的合成:二氧化碳化学固定和碘吸附的实验和动力学模型
在二溴甲基苯作为交联剂和铵剂的存在下,通过对以可调烷基链为系链的苯酚进行弗里德尔-卡夫烷基化反应,以及对 N,N-二甲基乙二胺进行季铵化反应,我们合成了一系列 "一体化 "超交联聚合物(HCPOH-Cn)。经过表征后,聚合物被用于可持续的二氧化碳转化和碘吸附。实验结果表明,HCPOH-C12 能有效催化 CO2 环加成反应,在优化条件后,产率高达 94%。其出色的活性归功于较低的活化能(69.52 kJ mol-1)。HCPOH-C12 聚合物具有出色的底物适应性和可回收性,并提出了一种可能的催化机理。此外,HCPOH-C0 还显示出惊人的碘吸附能力,其吸附过程与二阶吸附动力学非常吻合,并符合朗缪尔吸附等温线。HCPOH-C0 对碘的吸附是一个自发的内热过程,表明在吸附阶段固液界面的无序性增加。
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来源期刊
Sustainable Energy & Fuels
Sustainable Energy & Fuels Energy-Energy Engineering and Power Technology
CiteScore
10.00
自引率
3.60%
发文量
394
期刊介绍: Sustainable Energy & Fuels will publish research that contributes to the development of sustainable energy technologies with a particular emphasis on new and next-generation technologies.
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