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

机译：苯乙炔在磺化碳材料上的水合：活性位和固有催化活性

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摘要

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 (–SO _(3) H) 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 ( k ) and lower apparent activation energy ( E _(a) ) in the hydration reactions than SCNT catalysts. NH _(3) -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 –SO _(3) H 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 via the catalytic alkyne hydration reactions.
机译：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，分别表示为Sglu，SCNT，SAC和SCMK），并用作苯乙炔（PA）水合反应中的酸催化剂。磺酸基团（–SO _（3）H）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水合反应遵循伪一级反应动力学。 Sglu在水合反应中比SCNT催化剂具有更高的反应速率常数（k）和更低的表观活化能（E _（a））。 NH _（3）-温度程序解吸测量结果表明，Sglu较高的催化活性归因于较强的酸度和大量的–SO _（3）H活性位。这项工作展示了在PA水合反应中不含任何酸性添加剂的碳材料的性能，并通过动力学研究了固有的催化活性。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的醛酮化合物的环保和可持续生产策略提供了启示。

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