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Vapor phase condensation of methyl acetate with formaldehyde to preparing methyl acrylate over cesium supported SBA-15 catalyst

机译:铯负载SBA-15催化剂上乙酸甲酯与甲醛的气相缩合制备丙烯酸甲酯

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A cesium ion-containing catalyst, on an SBA-15 mesoporous molecular support, was prepared by the impregnation method and applied to the aldol condensation of methyl acetate with formaldehyde. The catalyst showed high catalytic activity in the condensation reaction. XRD characterization indicated that the cesium nitrate below 5 wt% loading was highly dispersed on the SBA-15 support. FT-IR and XPS results confirmed that a Si-O-Cs species was formed on the surface of the catalyst. Pyridine-IR verified that an L-acid site existed on the surface. The NH3-TPD and CO2-TPD results indicated that weak Lewis acid-base pairs were loaded on the surface, and these weak acid-base active sites might favor the aldol condensation reaction. The 5Cs/SBA-15 catalyst demonstrated the highest (48.4%)-conversion of methyl acetate reported and 95.0% selectivity for methyl acrylate. The deactivated catalyst was completely regenerated by calcination. The catalyst was regenerated nine times with a total operation time of more than 60 h, and the initial conversion of methyl acetate and the selectivity for methyl acrylate did not change. The high catalytic activity was mainly due to the suitable strength of weak acid-base properties, which were rooted in the Si-O-Cs species on the surface of the support. (C) 2014 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
机译:通过浸渍方法制备了在SBA-15中孔分子载体上的含铯离子的催化剂,并将其用于乙酸甲酯与甲醛的醛醇缩合反应。该催化剂在缩合反应中显示出高催化活性。 XRD表征表明低于5重量%负载的硝酸铯高度分散在SBA-15载体上。 FT-IR和XPS结果证实在催化剂表面上形成Si-O-Cs物质。吡啶-IR证实表面存在L-酸位点。 NH3-TPD和CO2-TPD结果表明,弱路易斯酸碱对被负载在表面上,这些弱酸碱活性位可能促进醛醇缩合反应。 5Cs / SBA-15催化剂显示出最高的乙酸甲酯转化率(48.4%),对丙烯酸甲酯的选择性为95.0%。失活的催化剂通过煅烧完全再生。催化剂再生了9次,总操作时间超过60小时,并且乙酸甲酯的初始转化率和对丙烯酸甲酯的选择性没有变化。高催化活性主要归因于弱酸碱性质的适当强度,弱酸碱性质源于载体表面的Si-O-Cs物种。 (C)2014韩国工业和工程化学学会。由Elsevier B.V.发布。保留所有权利。

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