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苯乙炔在磺化碳材料上的水合作用:活性位点与本征催化活性

Hydration of phenylacetylene on sulfonated carbon materials: active site and intrinsic catalytic activity.

作者信息

Yan Pengqiang, Xie Zailai, Tian Siyuan, Li Fan, Wang Dan, Su Dang Sheng, Qi Wei

机构信息

Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences 72 Wenhua Road Shenyang 110016 P. R. China

University of Chinese Academy of Sciences Beijing 100049 P. R. China.

出版信息

RSC Adv. 2018 Nov 14;8(67):38150-38156. doi: 10.1039/c8ra07966h.

Abstract

A series of sulfonated carbon materials (sulfonated glucose-derived carbon, carbon nanotubes, activated carbon and ordered mesoporous carbon, denoted as Sglu, SCNT, SAC and SCMK, respectively) were synthesized and applied as acid catalysts in phenylacetylene (PA) hydration reactions. The sulfonic acid groups (-SOH) were identified to be the only kind of active sites and were quantified with XPS and a cation exchange process. Mechanistic studies revealed that the catalytic PA hydration reaction follows pseudo first order reaction kinetics. Sglu exhibits a higher reaction rate constant () and lower apparent activation energy ( ) in the hydration reactions than SCNT catalysts. NH-temperature programmed desorption measurement results revealed that the relatively high catalytic activity of Sglu was attributed to both the stronger acidity and larger number of -SOH active sites. This work exhibited the performance of carbon materials without any extra acidic additives in PA hydration reaction and investigated the intrinsic catalytic activity by kinetics. The present work provides the possibility for acid catalytic applications of carbon materials, which sheds light on the environmentally friendly and sustainable production strategy for aldehyde ketone compounds the catalytic alkyne hydration reactions.

摘要

合成了一系列磺化碳材料(磺化葡萄糖衍生碳、碳纳米管、活性炭和有序介孔碳,分别记为Sglu、SCNT、SAC和SCMK),并将其用作苯乙炔(PA)水合反应的酸催化剂。磺酸基团(-SOH)被确定为唯一的活性位点,并通过XPS和阳离子交换过程进行了定量。机理研究表明,催化PA水合反应遵循准一级反应动力学。在水合反应中,Sglu比SCNT催化剂表现出更高的反应速率常数()和更低的表观活化能()。NH-程序升温脱附测量结果表明,Sglu相对较高的催化活性归因于更强的酸度和更多的-SOH活性位点。这项工作展示了碳材料在PA水合反应中无需任何额外酸性添加剂的性能,并通过动力学研究了其内在催化活性。目前的工作为碳材料的酸催化应用提供了可能性,这为通过催化炔烃水合反应生产醛酮化合物的环境友好和可持续生产策略提供了思路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a473/9089823/1fd09380aeab/c8ra07966h-f1.jpg

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