层间模板剂导向合成新型多孔蒙脱石材料的研究

无机材料学报

层间模板剂导向合成新型多孔蒙脱石材料的研究

周春晖; 李庆伟; 葛忠华; 倪哲明; 李小年

浙江工业大学化工学院杭州 310014

收稿日期:2002-08-30 修回日期:2002-10-30 出版日期:2003-11-20 网络出版日期:2003-11-20

Synthesis of Novel Porous Silica/Montmorillonite Composites by Gallery-Template Structure-Directing Method

ZHOU Chun-Hui; LI Qing-Wei; GE Zhong-Hua; NI Zhe-Ming; LI Xiao-Nian

Laboratory of Advanced Catalyst Materials; College of Chemical Engineering; Zhejiang University of Technology; Hangzhou 310014; China

Received:2002-08-30 Revised:2002-10-30 Published:2003-11-20 Online:2003-11-20

摘要/Abstract

摘要： 采用提纯后天然蒙脱石为原料,经十六烷基三甲基溴化铵和十八烷基三甲基氯化铵改性后,分别以C8～C14中性伯胺为结构导向剂,蒙脱石/胺/正硅酸乙酯摩尔比为1:20:150,搅拌反应时间为8h,经分离、干燥、焙烧,成功制备出新型多孔氧化硅/蒙脱石复合材料.用XRD、TG、FT-IR、N_2等温吸附-脱附和酸催化烷基化探针反应等表征了其结构和性能.结果表明,合成材料具有高比表面积、大层间通道、孔径分布较窄且依据模板导向剂分子尺寸可调,其酸催化活性和选择性较普通的酸活化蒙脱石有较大的提高.

关键词: 蒙脱石, 多孔材料, 柱撑, 催化

Abstract: The purified natural montmorillonites were modified by cetyltrimethylammonium bromide (CTAB) and octadecyltrimethylammonium chloride respectively. Mixtures
of the modified montmorillonites, neutral amine and tetraethylorthosilicate (TEOS) at a molar ratio of 1:20:150 were allowed to react for 8h. The
resulting intercalates were centrifuged, dried in air and calcined at 540℃ for 4h to burn off the organic templates, a series
of novel porous silica/montmorillonites composites were successfully synthesized by the gallery-template structure-directing process. The structure
of the samples was characterized by XRD, TG, FT-IR, N₂ adsorption-desorption isotherms and acid-catalyzed alkylation probe reaction. The results show
that the samples synthesized have a narrowly pore distribution and super-gallery height, a large BET specific area. With the increasing of chain length of
neutral amine, the pore size and gallery height increase accordingly. The synthetic materials are potentially effective solid acid catalysts for the
Friedel-Crafts alkylation of catechol with tert-butyl alcohol to synthesize butyl 4-tert-butylcatechol (4-TBC). Over synthetic porous material by using CTAB
and hexylamine as template, the selectivity to 4-TBC of 78.5% and catechol conversion of 45.5% can be obtained under experimental condition.

Key words: montmorillonite, porous materials, pillaring, catalysis

中图分类号:

O643

周春晖,李庆伟,葛忠华,倪哲明,李小年. 层间模板剂导向合成新型多孔蒙脱石材料的研究[J]. 无机材料学报.

ZHOU Chun-Hui,LI Qing-Wei,GE Zhong-Hua,NI Zhe-Ming,LI Xiao-Nian. Synthesis of Novel Porous Silica/Montmorillonite Composites by Gallery-Template Structure-Directing Method[J]. Journal of Inorganic Materials.

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