催化学报

催化学报 ›› 2015, Vol. 36 ›› Issue (6): 801-805.DOI: 10.1016/S1872-2067(14)60277-1

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Ce-Beta分子筛的制备及其催化性能

唐波a, 戴卫理a, 孙晓明a,b, 武光军a, 李兰冬a, 关乃佳a, Michael Hungerb   

  1. a 南开大学化学学院, 先进能源材料化学教育部重点实验室, 天津化学化工协同创新中心, 天津300071;
    b 斯图加特大学, 化学工程研究所, 德国斯图加特70550
  • 收稿日期:2014-11-04 修回日期:2014-12-04 出版日期:2015-05-21 发布日期:2015-05-21
  • 通讯作者: 戴卫理,电话/传真: (022)23500341; 电子信箱: weilidai@nankai.edu.cn
  • 基金资助:

    国家自然科学基金(21373119); 教育部创新团队(IRT13022, IRT13R30); 111计划(B12015); 德国科学基金会.

Incorporation of cerium atoms into Al-free Beta zeolite framework for catalytic application

Bo Tanga, Weili Daia, Xiaoming Suna,b, Guangjun Wua, Landong Lia, Naijia Guana, Michael Hungerb   

  1. a Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) & Key Laboratory of Advanced Energy Materials Chemistry of Ministry of Education, College of Chemistry, Nankai University, Tianjin 300071, China;
    b Institute of Chemical Technology, University of Stuttgart, 70550 Stuttgart, Germany
  • Received:2014-11-04 Revised:2014-12-04 Online:2015-05-21 Published:2015-05-21
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21373119), the Ministry of Education of China (IRT13022, IRT13R30); 111 Project (B12015), and Deutsche Forschungsgemeinschaft.

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被引次数

4

摘要：

采用简单、易重现的两步后合成法成功制备了Ce-Beta分子筛. 制备过程中, H-Beta分子筛首先经过脱铝处理得到Si-Beta分子筛, 然后再以异丙醇铈为前驱体, 通过干法浸渍的途径向Si-Beta分子筛引入Ce (IV). 利用XRD, FT-IR, UV-Vis和1H MAS NMR等对其结构进行了表征, 结果表明, Ce(IV)物种以四配位的形式成功引入Beta分子筛的骨架, Ce原子进入分子筛骨架的机理通过DRIFT光谱得以证实. 通过环氧化合物水合制备1,2-二醇反应对所制的Ce-Beta催化剂进行了催化性能评价.

关键词: Ce-Beta分子筛, 后合成, 脱铝, 开环水合, 环氧

Abstract:

Ce(IV)-containing zeolite Beta was successfully prepared by a reproducible and scalable two-step post-synthesis strategy. This consists of creating vacant T sites that are associated with silanol groups by the dealumination of the H-Beta zeolite and a subsequent dry impregnation of the resultant Si-Beta zeolite with cerium (IV) isopropoxide. XRD, FT-IR, UV-Vis and 1H MAS NMR confirmed that Ce(IV) was successfully incorporated into the Beta zeolite framework by the post-synthesis procedures and that they exist as isolated atoms with tetrahedral coordination. The mechanism of Ce incorporation into the framework of Beta zeolite was confirmed by DRIFT spectroscopy. The ring-opening hydration of epoxides to their corresponding 1,2-diols was selected as a model reaction for an evaluation of the catalytic performance of the as-synthesized Ce-Beta zeolite.

Key words: Ce-Beta zeolite, Post-synthesis, Dealumination, Ring-opening hydration, Epoxide