The efficient metal- and halogen-free polymer catalyst for the intensification on CO2 cycloaddition

IF 4.7 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2024-10-23 DOI:10.1016/j.apcata.2024.119996

引用次数: 0

Abstract

An environmentally friendly polymer catalyst (PAS) was synthesized via inverse emulsion polymerization using acrylic acid (AA) and 1-vinyl imidazole (VI) as monomers. The excellent catalytic activity of PAS was attributed to the synergistic effects of the carboxyl groups (-COOH) as hydrogen bond donors and N-heterocyclic carbene (NHCs) as electron donor, as well as the swelling properties of the polymer, which can enrich the substrate into the polymer network, increasing the contact between the substrate and active sites. Characterization results from thermogravimetric (TG) analysis and small-angle X-ray scattering (SAXS) showed that the excessive imidazole addition disrupted the polymer's chain-like structure, significantly reducing its swelling properties. And, the catalytic performance is influenced by both the amount of imidazole in PAS and the swelling properties of the polymer. Finally, the reaction mechanism of the CO₂ cycloaddition reaction catalyzed by PAS was proposed and validated through density functional theory (DFT) calculations.

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用于强化 CO2 环化反应的高效无卤金属聚合物催化剂

以丙烯酸（AA）和 1-乙烯基咪唑（VI）为单体，通过反向乳液聚合合成了一种环境友好型聚合物催化剂（PAS）。羧基（-COOH）作为氢键供体，N-杂环碳烯（NHC）作为电子供体，两者的协同作用以及聚合物的溶胀特性使底物富集到聚合物网络中，增加了底物与活性位点的接触，从而使 PAS 具有优异的催化活性。热重（TG）分析和小角 X 射线散射（SAXS）表征结果表明，咪唑的过量添加破坏了聚合物的链状结构，显著降低了其溶胀性能。此外，催化性能还受到 PAS 中咪唑含量和聚合物溶胀性能的影响。最后，通过密度泛函理论（DFT）计算，提出并验证了 PAS 催化 CO2 环加成反应的反应机理。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.