以一种新型Gemini表面活性剂作为介孔模板剂通过转晶过程合成介孔 ZSM-5 分子筛

doi:10.1016/S1872-2067(14)60128-5

催化学报 ›› 2014, Vol. 35 ›› Issue (10): 1727-1739.DOI: 10.1016/S1872-2067(14)60128-5

以一种新型Gemini表面活性剂作为介孔模板剂通过转晶过程合成介孔 ZSM-5 分子筛

王全义^a,b,e, 魏迎旭^a, 徐舒涛^a, 张默之^a,e, 孟霜鹤^a, 樊栋^a,e, 齐越^a, 李金哲^a, 于政锡^a, 袁翠峪^a, 何艳丽^a, 徐庶亮^a, 陈景润^a,e, 王金棒^a, 苏宝连^b,c, 刘中民^a,d

a 中国科学院大连化学物理研究所, 洁净能源国家实验室, 辽宁大连 116023;
b 那慕尔大学无机材料化学实验室, 比利时那慕尔;
c 武汉理工大学材料复合新技术国家重点实验室, 湖北武汉 430070;
d 中国科学院大连化学物理研究所, 催化基础国家重点实验室, 辽宁大连 116023;
e 中国科学院大学, 北京 100049

收稿日期:2014-04-09 修回日期:2014-05-28 出版日期:2014-09-28 发布日期:2014-09-30
通讯作者: 魏迎旭, 苏宝连, 刘中民
基金资助:
国家自然科学基金（21273230，21273005，21103176和21103180）.

Synthesis of mesoporous ZSM-5 using a new gemini surfactant as a mesoporous directing agent：A crystallization transformation process

Quanyi Wang^a,b,e, Yingxu Wei^a, Shutao Xu^a, Mozhi Zhang^a,e, Shuanghe Meng^a, Dong Fan^a,e, Yue Qi^a, Jinzhe Li^a, Zhengxi Yu^a, Cuiyu Yuan^a, Yanli He^a, Shuliang Xu^a, Jingrun Chen^a,e, Jinbang Wang^a, baolian Su^b,c, Zhongmin Liu^a,d

a Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b Laboratory of Inorganic Materials Chemistry (CMI), University of Namur (FUNDP), 61 rue de Bruxelles, B-5000 Namur, Belgium;
c State key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei, China;
d State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
e University of Chinese Academy of Sciences, Beijing 100049, China

Received:2014-04-09 Revised:2014-05-28 Online:2014-09-28 Published:2014-09-30
Supported by:
This work was supported by the National Natural Science Foundation of China (21273230, 21273005, 21103176, 21103180).

摘要/Abstract

摘要：

将一种新型Gemini表面活性剂，丙撑基双（十八烷基二甲基氯化铵）[C₁₈H₃₇（CH₃）₂-N⁺-（CH₂）₃-N⁺-（CH₃）₂C₁₈H₃₇]Cl₂（C_18-3-18），作为介孔模板剂用于水热法合成介孔ZSM-5分子筛. 结果表明，在130 oC低温晶化即可高效合成介孔ZSM-5分子刷. C_18-3-18的加入量可影响到所合成介孔ZSM-5分子筛的相对结晶度和织构性质，它的形成遵从一个转晶过程. 在合成初期，凝胶中介孔模板剂C_18-3-18的使用导向了介孔材料的生成；随后在TPABr的模板作用下，介孔材料慢慢转晶生成具有MFI结构的介孔ZSM-5；然后所合成的介孔ZSM-5晶粒进一步长大并聚集形成块状颗粒，同时产生晶间介孔. C_18-3-18作为介孔导向剂不仅可用于合成介孔ZSM-5分子筛，也可用于其它介孔分子筛的合成中.

关键词: 介孔ZSM-5, 双模板法, Gemini型表面活性剂, 晶间介孔, 转晶过程

Abstract:

A new gemini surfactant, [C₁₈H₃₇(CH₃)₂-N⁺-(CH₂)₃-N⁺-(CH₃)₂C₁₈H₃₇]Cl₂ (C_18-3-18), has been successfully used as the mesopore directing agent in the hydrothermal synthesis of mesoporous ZSM-5 (MZSM-5). The synthesis of MZSM-5 was realized with a low temperature crystallization process at 130 ℃. The amount of C_18-3-18 used in the synthesis affected the relative crystallinity and the textural properties of the obtained MZSM-5. Detailed investigation showed that the formation of MZSM-5 followed a crystallization transformation process. The use of C_18-3-18 resulted in the formation of mesoporous material during the early stage of the synthesis, which was converted into MZSM-5 crystals templated by tetrapropylammonium bromide to form the MFI phase. As the synthesis proceeded, the MZSM-5 crystals aggregated into particles by weak interactions. This work shows that C_18-3-18 can be used as a mesopore directing agent, which could provide a route for the synthesis of other mesoporous zeolites.

Key words: Mesoporous ZSM-5, Dual-templating, Gemini surfactant, Inter-crystalline mesopore, Crystallization transformation

王全义, 魏迎旭, 徐舒涛, 张默之, 孟霜鹤, 樊栋, 齐越, 李金哲, 于政锡, 袁翠峪, 何艳丽, 徐庶亮, 陈景润, 王金棒, 苏宝连, 刘中民. 以一种新型Gemini表面活性剂作为介孔模板剂通过转晶过程合成介孔 ZSM-5 分子筛[J]. 催化学报, 2014, 35(10): 1727-1739.

Quanyi Wang, Yingxu Wei, Shutao Xu, Mozhi Zhang, Shuanghe Meng, Dong Fan, Yue Qi, Jinzhe Li, Zhengxi Yu, Cuiyu Yuan, Yanli He, Shuliang Xu, Jingrun Chen, Jinbang Wang, baolian Su, Zhongmin Liu. Synthesis of mesoporous ZSM-5 using a new gemini surfactant as a mesoporous directing agent：A crystallization transformation process[J]. Chinese Journal of Catalysis, 2014, 35(10): 1727-1739.

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以一种新型Gemini表面活性剂作为介孔模板剂通过转晶过程合成介孔 ZSM-5 分子筛

Synthesis of mesoporous ZSM-5 using a new gemini surfactant as a mesoporous directing agent：A crystallization transformation process

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