Halogen-free acylation of toluene over FeSBA-1 molecular sieves
Halogen-free acylation of toluene over FeSBA-1 molecular sieves
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DOI：
10.1016/j.micromeso.2006.10.014
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发表时间：
2007-03-23
影响因子：
5.2
通讯作者：
Mori, T.
中科院分区：
文献类型：
--
作者：
Vinu, A.;Krithiga, T.;Mori, T.
以十六烷基三乙基溴化铵和原硅酸四乙酯为模板剂和二氧化硅源，在强酸性介质中合成了不同铁含量的三维笼型铁取代介孔二氧化硅（FeSBA-1）。在不同n(si)/n(le)比的FeSBA-1介孔催化剂上，在液相条件下，在80-180℃的温度范围内，用乙酸酐(AA)对甲苯进行酰化，运行时间为1-6小时。对反应温度、进料比、催化剂重量和运行时间等影响反应转化率和选择性的重要因素进行了研究，并对结果进行了详细讨论。对反应条件进行了优化，所有催化运行均保持 N-AA/n(甲苯) 比率为 2，催化剂重量为 0.1 g（总反应混合物的 3.3 wt%）。研究发现催化活性受催化剂中四面体铁含量的强烈影响。在本研究中使用的催化剂中，FeSBA-1(36) 在优化的反应条件下表现出较高的甲苯转化率和对甲基苯乙酮（p-MAP）的选择性。研究还发现，所有催化剂对p-MAP的选择性始终高于in-NIAP和o-MAP，并且催化剂的活性按以下顺序变化：FeSBA1(36) > FeSBA-1(90) > FeSBA-1(120)。 (c) 2006 Elsevier Inc. 保留所有权利。
Three-dimensional cage type iron substituted mesoporous silica with different iron contents (FeSBA-1) was synthesized in a highly acidic media using cetyltriethylammonium bromide and tetraethylorthosilicate as a template and a silica source, respectively. Acylation of toluene with acetic anhydride (AA) was carried out over FeSBA-1 mesoporous catalysts with different n(si)/n(le) ratios in the temperature range 80-180 degrees C for a time-on-stream of 1-6 h under liquid phase conditions. The important factors affecting the conversion and the selectivity of the reaction, such as the reaction temperature, feed ratio, catalyst weight and time-on-stream were studied and the results are discussed in detail. The reaction conditions were optimized and the N-AA/n(Toluene) ratio of 2 and catalyst weight of 0.1 g (3.3 wt% of total reaction mixture) were maintained for all catalytic runs. It was found that the catalytic activity is strongly influenced by the amount of tetrahedral iron in the catalysts. Among the catalysts used in the present study, FeSBA-1(36) showed a high toluene conversion and selectivity to p-methylacetophenone (p-MAP) under the optimized reaction conditions. It was also found that the selectivity for p-MAP was always higher than in-NIAP and o-MAP for all the catalysts and the activity of the catalysts changes in the following order: FeSBA1(36) > FeSBA-1(90) > FeSBA-1(120). (c) 2006 Elsevier Inc. All rights reserved.