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通过芳香杂环双功能有机结构导向剂直接合成纳米片堆叠的分级“蜂蜜棒状”MFI沸石

Direct Synthesis of Nanosheet-Stacked Hierarchical "Honey Stick-like" MFI Zeolites by an Aromatic Heterocyclic Dual-Functional Organic Structure-Directing Agent.

作者信息

Wang Risheng, Peng Zhihua, Wu Pingping, Lu Jinzhi, Rood Mark J, Sun Hongman, Zeng Jingbin, Wang Youhe, Yan Zifeng

机构信息

College of Science, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (EastChina), No. 66, Changjiang West Road Qingdao Economic & Technical Development Zone, Qingdao, 266580, Shandong, P. R. China.

Department of Civil and Environmental Engineering, University of Illinois, 205 North Mathews Avenue, Urbana, Illinois, 61801, United States.

出版信息

Chemistry. 2021 Jun 16;27(34):8694-8697. doi: 10.1002/chem.202100701. Epub 2021 May 27.

DOI:10.1002/chem.202100701
PMID:33938064
Abstract

Soft template designing is the most promising strategy for the synthesis of zeolite nanosheets. MFI nanosheets directed by soft templates (containing long-chain alkyl groups or aromatic groups as hydrophobic component) can be found frequently; however, so far, MFI nanosheets synthesized by soft templates with aromatic heterocycle groups (e. g., s-triazine groups) are rare. Herein, a nanosheet-stacked hierarchical MFI zeolite (NSHM) has been synthesized by using a triply branched s-triazine-based surfactant as a bifunctional organic structure-directing agent. On the basis of a geometrical match relationship, a formation model has been proposed. Synthesized NSHM had abundant mesopores stacked by nanosheets and exhibited a high surface area (430 m  ⋅ g ). The 1 wt% Pd/NSHM attained a significant increase in yield of cyclohexanol/cyclohexanone mixture (from 66 to 85 %) in the oxidation of cyclohexane compared with Silicalite-1 and SBA-15 as supports.

摘要

软模板设计是合成沸石纳米片最具前景的策略。由软模板(含有长链烷基或芳基作为疏水成分)导向的MFI纳米片屡见不鲜;然而,迄今为止,由带有芳杂环基团(如s-三嗪基团)的软模板合成的MFI纳米片却很罕见。在此,通过使用一种三分支的基于s-三嗪的表面活性剂作为双功能有机结构导向剂,合成了一种纳米片堆叠的分级MFI沸石(NSHM)。基于几何匹配关系,提出了一种形成模型。合成的NSHM具有由纳米片堆叠而成的丰富介孔,并表现出高比表面积(430 m²⋅g⁻¹)。与作为载体的Silicalite-1和SBA-15相比,1 wt% Pd/NSHM在环己烷氧化反应中,环己醇/环己酮混合物的产率显著提高(从66%提高到85%)。

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