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Soft-templating synthesis of hierarchical mordenite as high-performance catalyst for cyclic acetals production via acetylation of glycerol and benzaldehyde
Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2024-03-26 , DOI: 10.1016/j.micromeso.2024.113111
Jiang-Tian Gong , Taghrid S. Alomar , Najla AlMasoud , Ludovica Pace , Aurelie Vicente , Pedro Maireles-Torres , Joon Ching Juan , Zeinhom M. El-Bahy , Svetlana Mintova , Eng-Poh Ng

Highly active hierarchical mordenite zeolite with micro/mesoporosity (TM-) for selective synthesis of cyclic acetals acetylation reaction is reported. The hierarchical zeolite is synthesized using soft-templating approach with variations in octadecyltrimethoxysilane (OTMS/AlO ratio, = 0.2, 0.3 and 0.4) in precursor hydrogels. The results reveal that OTMS not only creates secondary mesoporosity in zeolite framework (larger mesopore volume, external surface area, average pore diameter), but also influences the crystallization process, altering the crystal morphology, crystallinity and Si/Al ratios. Among TM- zeolites prepared, TM-0.3 hierarchical mordenite has the optimum OTMS amount incorporated while further increasing the OTMS amount leads to the formation of ANA/GIS intergrowth. Thanks to the accessible hierarchical porosity, reduced acidity and morphological effects, the TM-0.3 hierarchical mordenite exhibits excellent catalytic performance (84.1% conversion, TOF = 0.087 s, 61.5% dioxolane selectivity) in acetylation of glycerol and benzaldehyde (160 °C, 20 min) better than pristine mordenite. The catalyst is reusable for five runs with minimal loss of activity (TOF = 0.087 → 0.084 s), making it a promising catalyst for chemical productions involving bulky molecules. In addition, comparative catalytic tests with classical homogeneous and heterogeneous catalysts, including HSO, HCl, CHCOOH, H–Y, H-LTL, Na-X, Na-A, were performed.

中文翻译:

软模板合成分级丝光沸石作为甘油和苯甲醛乙酰化生产环状缩醛的高性能催化剂

报道了具有微孔/中孔(TM-)的高活性分级丝光沸石,用于选择性合成环状缩醛乙酰化反应。使用软模板方法合成分级沸石,并在前体水凝胶中改变十八烷基三甲氧基硅烷(OTMS/Al2O比= 0.2、0.3和0.4)。结果表明,OTMS不仅在沸石骨架中产生次生介孔(更大的介孔体积、外表面积、平均孔径),而且影响结晶过程,改变晶体形态、结晶度和Si/Al比。在制备的TM-沸石中,TM-0.3分级丝光沸石具有最佳的OTMS掺入量,而进一步增加OTMS掺入量导致ANA/GIS共生的形成。由于具有可达到的分级孔隙率、降低的酸度和形态效应,TM-0.3分级丝光沸石在甘油和苯甲醛的乙酰化(160°C,20)中表现出优异的催化性能(84.1%转化率,TOF = 0.087s,61.5%二氧戊环选择性)分钟)优于原始丝光沸石。该催化剂可重复使用五次,活性损失最小(TOF = 0.087 → 0.084 s),使其成为涉及大分子的化学生产的有前景的催化剂。此外,还对经典的均相和非均相催化剂(包括 HSO、HCl、CHCOOH、H-Y、H-LTL、Na-X、Na-A)进行了催化对比测试。
更新日期:2024-03-26
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