Hyun You Kim, Habib Ullah, Zakir Ullah, Zafar A K Khattak, Muhammad Tahir, Eunji Kang, Francis Verpoort
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引用次数: 0
摘要
共价有机框架(COFs)是一类不断发展的永久性多孔有序材料,由于其奇妙的形态特征以及在气体储存、吸附和催化方面的大量应用,最近引起了越来越多的关注。然而,它们较低的水稳定性和繁琐的合成过程普遍阻碍了它们在异相催化中的应用。尽管如此,人们仍然对一种能够将二氧化碳/环氧化物偶联生成具有重要工业意义的环状碳酸盐的水稳定性异相催化体系非常感兴趣。在此,我们报告了具有超强水稳定性和热稳定性的二维钴浸渍腙连接纤维状 COFs,作为催化剂可在常压下进行二氧化碳/环氧化物偶联反应。掺杂钴(Co)的官能化 COFs 表现出优异的催化活性,具有较高的催化活性(80925)和催化时间(6466 h-1),优于已报道的用于常压下 CO2/ 环氧化物偶联反应的异相催化剂。通过密度泛函理论计算,我们发现 COF 基质中的 Co2+ 离子可催化 CO2 环加成反应。我们还证实,掺 Co 的 COF 具有出色的结构稳定性和持续的活性,可重复十次循环。
Solvent Free Ambient Pressure CO2 Cycloaddition Catalyzed by Cobalt-Impregnated 2D-Nanofibrous COFs.
Covalent organic frameworks (COFs) constitute an evolving class of permanently porous and ordered materials, and they have recently attracted increased interest due to their intriguing morphological features and numerous applications in gas storage, adsorption, and catalysis. However, their low aqueous stabilities and tedious syntheses generally hamper their use in heterogeneous catalysis. Nonetheless, a capable and water-stable heterogeneous catalytic system for coupling CO2/epoxides to generate industrially important cyclic carbonates is still of great interest. Herein, exceedingly water- and thermally stable 2D-cobalt-impregnated hydrazone-linked fibrous COFs are reported as a catalyst for CO2/epoxide coupling reactions at ambient pressure. The functionalized cobalt (Co)-doped COFs demonstrated excellent catalytic activities with the high TONs (80925) and TOFs (6466 h-1), outperforming reported heterogeneous catalysts for CO2/epoxide coupling at ambient pressure. We found that the Co2+ ions within the COF matrix catalyze CO2 cycloaddition through density functional theory calculations. We also confirmed the excellent structural stability and consistent activity of Co-doped COFs up to ten repeating cycles.
期刊介绍:
ChemSusChem
Impact Factor (2016): 7.226
Scope:
Interdisciplinary journal
Focuses on research at the interface of chemistry and sustainability
Features the best research on sustainability and energy
Areas Covered:
Chemistry
Materials Science
Chemical Engineering
Biotechnology