高等学校化学学报 ›› 2021, Vol. 42 ›› Issue (1): 74.doi: 10.7503/cjcu20200461

所属专题: 分子筛功能材料 2021年,42卷,第1期

• 综合评述 • 上一篇    下一篇

等级孔分子筛的可控合成、 扩散研究及催化应用

邹润1,董霄1,矫义来2,Carmine D'AGOSTINO1,闫文付3,范晓雷1   

  1. 1.Department of Chemical Engineering and Analytical Science, School of Engineering, the University of Manchester, Manchester M13 9PL, United Kingdom
    2.中国科学院沈阳金属研究所, 沈阳材料科学国家研究中心, 沈阳 110016
    3.吉林大学化学学院, 无机合成与制备化学国家重点实验室, 长春 130012
  • 收稿日期:2020-07-16 出版日期:2021-01-10 发布日期:2021-01-12
  • 基金资助:
    欧盟“地平线2020”研究与创新基金(872102);国家留学基金委基金(201906740020);高等学校学科创新引智计划项目(B17020);国家自然科学基金(批准号(U1967215);21835002, 21621001)、 英国工程与自然科学研究理事会基金(EP/S019138/1);辽宁省自然科学基金(2018010047-301);国家重点研发计划项目(SQ2019YFE011366)

Controllable Synthesis, Diffusion Study and Catalysis of Hierarchical Zeolites

ZOU Run1, DONG Xiao1, JIAO Yilai2, Carmine D'AGOSTINO1, YAN Wenfu3, FAN Xiaolei1()   

  1. 1.Department of Chemical Engineering and Analytical Science,School of Engineering,the University of Manchester,M13 9PL,United Kingdom
    2.Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China
    3.State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,College of Chemistry,Jilin University,Changchun 130012,China
  • Received:2020-07-16 Online:2021-01-10 Published:2021-01-12
  • Contact: FAN Xiaolei E-mail:xiaolei.fan@manchester.ac.uk
  • Supported by:
    This paper is supported by the European Union’s Horizon 2020 Research and Innovation Programme(872102);the China Scholarship Council-The University of Manchester Joint Scholarship(201906740020);the Programme of Introducing Talents of Discipline to Universities of China(B17020);the National Natural Science Foundation of China(U1967215);the EPSRC New Investigator Award(EP/S019138/1);the Natural Science Foundation of Liaoning Province, China(2018010047-301);the National Key Research and Development Program of China(SQ2019YFE011366)

摘要:

等级孔分子筛是一类具有两种或多种以特定形式排布的孔结构的分子筛材料. 多层等级的孔结构使得分子筛孔道内的分子扩散得到显著改善, 进而提升了其在吸附和非均相催化等领域的应用性能. 等级孔分子筛的制备策略通常有两种, 即“自上而下”后处理法(如对母样分子筛进行脱铝、 脱硅产生介孔)和“自下而上”合成法(如软模板、 硬模板法). 本文主要对近20年来等级孔分子筛的合成方法进行了梳理, 并着重介绍了具有较高应用潜力的“自上而下”制备法. 鉴于合成等级孔分子筛的主要目的是提高分子的晶内扩散, 对近年来客体分子在等级孔分子筛内扩散的实验研究也进行了简要综述. 此外, 本文还综合评述了等级孔分子筛与传统分子筛在催化应用中的对比, 以展示前者在提升催化性能方面(如活性、 选择性等)的独特优势.

关键词: 等级孔分子筛, 后处理, 扩散, 脉冲梯度场核磁共振, 催化

Abstract:

Hierarchical zeolites refer to zeolitic materials having bi-/multi-modal interconnective pores arranged in order of certain ranks, which improve the molecular diffusion within their frameworks, and hence the performance in their applications such as adsorption and heterogeneous catalysis. Hierarchical zeolites are commonly produced via the top-down post-synthetic treatments(such as dealumination and/or desilication) of pre-synthesized zeolites(i.e. the parent zeolites) and the bottom-up synthesis-by-design methods(such as soft/hard templating). This review presents the recent advances(mainly post 2000) in the strategies of making hierarchical zeolites, with the emphasis on the top-down approaches due to their relatively high practicality. Since hierarchical zeolites are proposed to improve intracrystalline diffusion, experimental studies of guest molecules diffusion in hierarchical zeolites are also reviewed. Additionally, catalytic applications of hierarchical zeolites, in comparison with the conventional microporous pristine zeolites, are also commented to highlight the advantages of hierarchical zeolites to improve catalysis.

Key words: Hierarchical zeolite, Post-synthetic treatment, Diffusion, Pulsed-field gradient nuclear magnetic resonance(PFG NMR), Catalysis

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