咪唑基介孔有机硅材料固载磷钼酸催化剂的制备及烯烃环氧化性能

doi:10.1016/S1872-2067(14)60025-5

催化学报 ›› 2014, Vol. 35 ›› Issue (4): 532-539.DOI: 10.1016/S1872-2067(14)60025-5

咪唑基介孔有机硅材料固载磷钼酸催化剂的制备及烯烃环氧化性能

王静^a,b, 邹永存^c, 孙渝^b, Mximilin Hemgeserg^b, Dirk Shffner^b, 高洪成^a, 宋晓静^a, 张文祥^a, 贾明君^a, Werner R. Thiel^b

a 吉林大学化学学院, 理论化学计算国家重点实验室, 吉林长春130021;
b 凯泽斯劳滕工业大学化学系, 凯泽斯劳滕67663, 德国;
c 吉林大学化学学院, 无机合成与制备化学国家重点实验室, 吉林长春130012

收稿日期:2013-11-14 修回日期:2014-01-02 出版日期:2014-03-20 发布日期:2014-03-21
通讯作者: 贾明君，Werner R. Thiel
基金资助:
中国国家留学基金管理委员会；国家自然科学基金（21173100）.

Electrostatic immobilization of phosphomolybdic acid on imidazolium-based mesoporous organosilicas for catalytic olefin epoxidation

Jing Wang^a,b, Yongcun Zou^c, Yu Sun^b, Maximilian Hemgesberg^b, Dirk Schaffner^b, Hongcheng Gao^a, Xiaojing Song^a, Wenxiang Zhang^a, Mingjun Jia^a, Werner R. Thiel^b

a State Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry, Jilin University, Changchun 130021, Jilin, China;
b Faculty of Chemisity, Technical University of Kaiserslautern, Erwin-Schroedinger-Str., Building 54, Kaiserslautern 67663, Germany;
c State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, Jilin, China

Received:2013-11-14 Revised:2014-01-02 Online:2014-03-20 Published:2014-03-21
Supported by:
This work was supported by the China Scholarship Council and the National Natural Science Foundation of China (21173100).

摘要/Abstract

摘要：

以含有咪唑阳离子的周期性介孔有机硅（PMO-ILs）材料为载体，制备了一类固载化磷钼酸（PMA）多相催化材料（PMA@PMO-ILs），并采用N₂吸附-脱附实验、X射线衍射、原子吸收光谱、差热-热重分析、红外光谱、紫外光谱及固体核磁共振技术研究了材料的结构及物理化学性质. 结果表明，磷钼酸通过静电相互作用被成功固载到PMO-ILs载体表面和孔道中，且在制备过程中磷钼酸及载体基本结构均未发生变化. 反应结果表明，PMA@PMO-ILs材料在以叔丁基过氧化氢为氧化剂的环辛烯环氧化反应中表现出一定的催化活性和很高的选择性. 中断实验结果表明，催化剂的主要活性中心在反应过程中未发生明显流失，且催化剂经多次循环使用后活性及选择性基本保持不变. PMO-ILs中大量的咪唑阳离子能有效稳定磷钼酸阴离子，使该催化材料表现出良好的稳定性.

关键词: 多金属氧酸盐, 介孔有机硅, 咪唑阳离子, 静电相互作用, 环氧化, 多相催化

Abstract:

Polyoxometalate-based heterogeneous materials were prepared by the immobilization of 12-phosphomolybdic acid (PMA) on periodic mesoporous organosilicas containing embedded imidazolium cations (PMO-ILs). The resulting hybrid materials (PMA@PMO-ILs) were characterized by N₂ adsorption-desorption, powder X-ray diffraction, atomic adsorption spectroscopy, thermogravimetric and differential thermal analyses, Fourier transform infrared spectroscopy, ultraviolet-visible diffuse reflectance spectroscopy, and solid-state cross-polarization magic angle spinning nuclear magnetic resonance. PMA was electrostatically immobilized on the surface and in the channels of PMO-ILs. The PMO-IL support and PMA structures were retained during the preparation processes. The catalytic properties of the PMA@PMO-ILs were evaluated for the liquid-phase epoxidation of cyclooctene. PMA@PMO-ILs were catalytically active, with nearly 100% selectivity to cyclooctene epoxide using tert-butyl hydroperoxide as the oxidant. The catalysts could be reused four times without obvious loss of activity or selectivity under identical reaction conditions. Imidazolium cations in the PMO-IL framework improved the stability and recyclability of the PMA immobilized catalysts.

Key words: Polyoxometalate, Mesoporous organosilica, Imidazolium cation, Electrostatic interaction, Epoxidation, Heterogeneous catalysis

王静, 邹永存, 孙渝, Mximilin Hemgeserg, Dirk Shffner, 高洪成, 宋晓静, 张文祥, 贾明君, Werner R. Thiel. 咪唑基介孔有机硅材料固载磷钼酸催化剂的制备及烯烃环氧化性能[J]. 催化学报, 2014, 35(4): 532-539.

Jing Wang, Yongcun Zou, Yu Sun, Maximilian Hemgesberg, Dirk Schaffner, Hongcheng Gao, Xiaojing Song, Wenxiang Zhang, Mingjun Jia, Werner R. Thiel. Electrostatic immobilization of phosphomolybdic acid on imidazolium-based mesoporous organosilicas for catalytic olefin epoxidation[J]. Chinese Journal of Catalysis, 2014, 35(4): 532-539.

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咪唑基介孔有机硅材料固载磷钼酸催化剂的制备及烯烃环氧化性能

Electrostatic immobilization of phosphomolybdic acid on imidazolium-based mesoporous organosilicas for catalytic olefin epoxidation

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