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化学进展 2015, Vol. 27 Issue (8): 1002-1013 DOI: 10.7536/PC150150 前一篇   后一篇

• 综述与评论 •

纳米薄层分子筛的合成与应用

闵媛媛, 尚蕴山, 宋宇, 李国栋, 巩雁军*   

  1. 中国石油大学(北京)化学工程学院 重质油国家重点实验室 CNPC 催化重点实验室 北京 102249
  • 收稿日期:2015-01-01 修回日期:2015-03-01 出版日期:2015-08-15 发布日期:2015-06-05
  • 通讯作者: 巩雁军 E-mail:gongyj@cup.edu.cn
  • 基金资助:
    国家重点基础研究发展计划(973)项目(No. 2012CB215002)和国家自然科学基金项目(No. 21176255, 21276278)资助
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The Synthesis of Nanosheets Zeolite and Its Catalytic Application

Min Yuanyuan, Shang Yunshan, Song Yu, Li Guodong, Gong Yanjun*   

  1. State Key Laboratory of Heavy Oil Processing, Key Laboratory of Catalysis, China National Petroleum Corporation, College of Chemistry Engineering, China University of Petroleum-Beijing, Beijing 102249, China
  • Received:2015-01-01 Revised:2015-03-01 Online:2015-08-15 Published:2015-06-05
  • Supported by:
    The work was supported by the State Key Development Program for Basic Research of China (No. 2012CB215002) and the National Natural Science Foundation of China (No. 21176255, 21276278).
纳米薄层分子筛(nanosheets zeolite)由于其独特的准二维结构,具有有序的微孔-介孔特征、适宜的表面酸性和良好的扩散性能,已成为分子筛控制合成及其应用研究中标志性的研究热点之一。该类分子筛在合成中采用不同双头或者多头季铵盐(碱)表面活性剂作结构导向剂,所得的纳米薄层分子筛具有晶面二维生长趋向和可控薄层交错形貌,在吸附、催化应用等多方面展现出独特的应用潜力。本文系统总结了季铵盐类表面活性剂对纳米薄层分子筛合成、物化性质的影响以及此类分子筛催化应用研究方面的最新进展,着重介绍了MFI结构的纳米薄层分子筛对甲醇转化制烃、贝克曼重排、异构化、烯烃环氧化等重要催化反应中的优势。最后对这种结构新颖的纳米薄层分子筛在合成和其他应用领域方面未来的研究方向进行了展望。
关键词： 纳米薄层, ZSM-5分子筛, 季铵盐, 催化应用
Nanosheets zeolite is a brand new type of pseudo 2-dimensional zeolite, possessing distinctive growth trend in the (010) crystal surface and hierarchical micro-mesoporous texture, which has triggered an immense interest in the development of nanosheets and its application. The specific morphology can be obtained and dominantly controlled by using multi-quaternary ammonium surfactants as the structure directing agent. Due to its predominant micro-mesoporous property, optimized surface acidity and lower restriction of the diffusion of macro-molecule with respect to conventional bulk zeolite, nanosheets zeolite has tremendous application potential in adsorption and catalysis fields. This review summarizes the advances in the synthesis and the characterization of ZSM-5 zeolite nanosheets with novel morphology. Furthermore, nanosheets zeolite exhibits premium advantages in many applications. Some different reactions that MFI nanosheets zeolite has been applied to are discussed in detail, including methanol conversion to hydrocarbons and macro-molecules involved reaction, i.e. Beckman rearragement reactions. Additionally, newly developed metal-modified nanosheets zeolite has been applied to isomerization, hydroxylation reaction and the epoxidation of olefins etc. Although nanosheets zeolite possesses a large number of strong points compared with conventional zeolite, there is still a long way to go for MFI nanosheets zeolite in improving the synthesis in a more facile/economical way as well as expanding the applications. The outlook section cast great expectation on nanosheets for enlightening the innovative design of other materials.

Contents
1 Introduction
2 Synthesis of nanosheets zeolites by quaternary ammoniums
2.1 MFI nanosheets zeolite
2.2 Nanosheets zeolite with two different framework intergrown
2.3 Hierarchical zeolite with other kinds of topologies
3 Properties of MFI nanosheets zeolite
3.1 2-Dimensional growth orientation
3.2 Ordered mesoporosity
3.3 Acid properties
3.4 Adsorption properties
4 Application of MFI nanosheet zeolite
4.1 Methanol conversion to hydrocarbons
4.2 Beckman rearrangement reaction
4.3 Applications over the metal-modified MFI nanosheets
5 Conclusion and outlook

Key words: nanosheets, ZSM-5 zeolite, quaternary ammonium, catalytic application

中图分类号: 

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摘要

纳米薄层分子筛的合成与应用