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Direct synthesis of hierarchically structured MFI zeolite nanosheet assemblies with tailored activity in benzylation reaction
Microporous and Mesoporous Materials ( IF 5.2 ) Pub Date : 2018-07-10 , DOI: 10.1016/j.micromeso.2018.07.019
Baoyu Liu , Zhipeng Chen , Jiajin Huang , Huiyong Chen , Yanxiong Fang

The MFI zeolites with nanosheet assemblies morphology were prepared by a seed-assisted strategy using specially designed bolaform surfactant [C6H13-N+(CH3)2-C6H12-N+(CH3)2-(CH2)12-O-(p-C6H4)2-O-(CH2)12-N+(CH3)2-C6H12-N+(CH3)2-C6H13] [Br]4 (C6-12-diphe) as a structure-directing agent. The MFI zeolite nanosheet assemblies were composed of MFI nanosheets with randomly organized structure, exhibiting a narrow mesopore distribution. By tuning the Si/Al ratios of MFI zeolite nanosheet assemblies from 60 to 10, the morphology of resultant zeolites changed from nanosheet stacks to house-of-cards-like structures, and to nanosponges. In addition, the porosity and Brønsted acid/Lewis acid ratio exhibited a parabola-type dependence on the Si/Al ratios of obtained zeolites, indicating that meso-/microporosity and acidity of MFI nanosheet assemblies can be systematically tailored by changing the constituents of zeolites. Catalytic performance of MFI zeolite nanosheet assemblies was investigated in the benzylation of benzyl alcohol with mesitylene. The results revealed that MFI zeolite nanosheet assemblies exhibited extraordinary catalytic activity compared to conventional ZSM-5 zeolite. The conversion of benzyl alcohol and selectivity (1,3,5-trimethyl-2-benzylbenzene vs dibenzyl ether) of zeolite catalysts were linearly dependent on the Brønsted acid/Lewis acid ratio, and they exhibited a parabola-type dependence on the Sext/SBET, indicating that a balance between acidity and porosity of zeolites can be realized to modulate the catalytic properties of MFI zeolite nanosheet assemblies guided by C6-12-diphe.



中文翻译:

在苄基化反应中具有定制活性的分层结构MFI沸石纳米片组件的直接合成

具有纳米片组装形态的MFI沸石是通过晶种辅助策略使用特殊设计的硼酸盐表面活性剂[C 6 H 13 -N +(CH 32 -C 6 H 12 -N +(CH 32-(CH 2)制备的)12 -O-(pC 6 H 42 -O-(CH 212 -N +(CH 32 -C 6 H 12 -N +(CH 32 -C 6 H ^ 13 ] [BR - ] 4(C 6-12 diphe)作为结构导向剂。MFI沸石纳米片组件由具有随机组织的结构的MFI纳米片组成,表现出窄的中孔分布。通过将MFI沸石纳米片组件的Si / Al比从60调整为10,所得沸石的形态从纳米片堆叠变为类似卡片的结构,再变为纳米海绵。另外,孔隙率和布朗斯台德酸/路易斯酸比对所获得的沸石的Si / Al比表现出抛物线型依赖性,表明MFI纳米片组件的介孔/微孔和酸度可以通过改变沸石的成分来系统地调整。 。研究了MFI沸石纳米片组件的催化性能,研究了苯甲醇与均三甲苯的苄基化反应。结果表明,与传统的ZSM-5沸石相比,MFI沸石纳米片组件表现出非凡的催化活性。苯甲醇的转化率和选择性(1,3,5-三甲基-2-苄基苯相对于二苄基醚)的沸石催化剂线性地依赖于布朗斯台德酸/路易斯酸的比率,并且它们表现出对S ext / S BET的抛物线型依赖性,表明可以实现沸石的酸度和孔隙率之间的平衡来调节C 6-12-diphe指导的MFI沸石纳米片组件的催化性能。

更新日期:2018-07-10
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