Recovery and Recycling of Ti Supported Bimodal Mesoporous Catalysts Prepared via Ship-in-a-bottle Method in the Epoxidation of Cyclohexene

doi:10.1016/j.cjche.2014.06.016

Chinese Journal of Chemical Engineering ›› 2014, Vol. 22 ›› Issue (8): 914-920.DOI: 10.1016/j.cjche.2014.06.016

• 第四届整体式结构化催剂与反应器国际会议专栏 • 上一篇下一篇

Recovery and Recycling of Ti Supported Bimodal Mesoporous Catalysts Prepared via Ship-in-a-bottle Method in the Epoxidation of Cyclohexene

Shiyang Bai, Xintao Hu, Jihong Sun, Bo Ren, Jinpeng Wang

Department of Chemistry and Chemical Engineering, College of Environmental & Energy Engineering, Beijing University of Technology, Beijing 100124, China

收稿日期:2014-01-03 修回日期:2014-01-16 出版日期:2014-08-28 发布日期:2014-11-04
通讯作者: Jihong Sun
基金资助:
Supported by the National Natural Science Foundation of China (21076003, 21272005), and the Funding Project for the Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of the Beijing Municipality (PHR201107104, 005000541211019/20, 005000543111517).

Recovery and Recycling of Ti Supported Bimodal Mesoporous Catalysts Prepared via Ship-in-a-bottle Method in the Epoxidation of Cyclohexene

Shiyang Bai, Xintao Hu, Jihong Sun, Bo Ren, Jinpeng Wang

Department of Chemistry and Chemical Engineering, College of Environmental & Energy Engineering, Beijing University of Technology, Beijing 100124, China

Received:2014-01-03 Revised:2014-01-16 Online:2014-08-28 Published:2014-11-04
Supported by:
Supported by the National Natural Science Foundation of China (21076003, 21272005), and the Funding Project for the Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of the Beijing Municipality (PHR201107104, 005000541211019/20, 005000543111517).

摘要/Abstract

摘要： Ti/BMMs (Ti supported bimodal mesoporous silica) catalysts have been prepared via self-assembly route combined with ship-in-a-bottle method. The recovery and recycling performances of Ti/BMMs were investigated in the epoxidation of cyclohexene. In order to the evaluate the regeneration methods and to examine the deactivation behaviors, the deactivated Ti/BMMs catalysts were washed in chloroform or calcinated at 450℃ for 6 h and then activity of the recovery catalysts were examined.Meanwhile, the structure features and surface properties of the regenerated catalysts were characterized by X-ray diffraction, N₂-sorption analysis, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, thermogravimetric analysis, UV visible spectroscopy and X-ray photoelectron spectroscopy. The results showed that the typical bimodal mesoporous structure of recycled Ti/BMMs catalysts was still maintained, and the phenomenon of Ti leaching during the catalytic process and recovery was negligible. In particular, spectroscopic observations indicated that the effects of the regeneration methods on the tetrahedrally-coordinated Ti species and catalytic deactivation were remarkable. The main reasons were related to the polarities of used solvents during recovery tests, the environment medium of adsorbed water inside mesopore channels and the deposition of bulky molecules of by-products on the mesoporous surface.

关键词: Ti/BMMs, Ship-in-a-bottle method, Recovery, Recycling, Epoxidation of cyclohexene

Abstract: Ti/BMMs (Ti supported bimodal mesoporous silica) catalysts have been prepared via self-assembly route combined with ship-in-a-bottle method. The recovery and recycling performances of Ti/BMMs were investigated in the epoxidation of cyclohexene. In order to the evaluate the regeneration methods and to examine the deactivation behaviors, the deactivated Ti/BMMs catalysts were washed in chloroform or calcinated at 450℃ for 6 h and then activity of the recovery catalysts were examined.Meanwhile, the structure features and surface properties of the regenerated catalysts were characterized by X-ray diffraction, N₂-sorption analysis, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, thermogravimetric analysis, UV visible spectroscopy and X-ray photoelectron spectroscopy. The results showed that the typical bimodal mesoporous structure of recycled Ti/BMMs catalysts was still maintained, and the phenomenon of Ti leaching during the catalytic process and recovery was negligible. In particular, spectroscopic observations indicated that the effects of the regeneration methods on the tetrahedrally-coordinated Ti species and catalytic deactivation were remarkable. The main reasons were related to the polarities of used solvents during recovery tests, the environment medium of adsorbed water inside mesopore channels and the deposition of bulky molecules of by-products on the mesoporous surface.

Key words: Ti/BMMs, Ship-in-a-bottle method, Recovery, Recycling, Epoxidation of cyclohexene

Shiyang Bai, Xintao Hu, Jihong Sun, Bo Ren, Jinpeng Wang. Recovery and Recycling of Ti Supported Bimodal Mesoporous Catalysts Prepared via Ship-in-a-bottle Method in the Epoxidation of Cyclohexene[J]. Chinese Journal of Chemical Engineering, 2014, 22(8): 914-920.

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Recovery and Recycling of Ti Supported Bimodal Mesoporous Catalysts Prepared via Ship-in-a-bottle Method in the Epoxidation of Cyclohexene

Recovery and Recycling of Ti Supported Bimodal Mesoporous Catalysts Prepared via Ship-in-a-bottle Method in the Epoxidation of Cyclohexene

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