Selective propylene epoxidation in liquid phase using highly dispersed Nb catalysts incorporated in mesoporous silicates

doi:10.1016/j.cjche.2018.03.001

Chinese Journal of Chemical Engineering ›› 2018, Vol. 26 ›› Issue (6): 1278-1284.DOI: 10.1016/j.cjche.2018.03.001

Selective propylene epoxidation in liquid phase using highly dispersed Nb catalysts incorporated in mesoporous silicates

Wenjuan Yan¹, Yuhui Wu¹, Xiang Feng¹, Chaohe Yang¹, Xin Jin¹, Jian Shen²

1 State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Qingdao 266580, China;
2 Department of Environmental Science and Engineering, Xiangtan University, Xiangtan 411105, China

收稿日期:2017-11-30 修回日期:2018-03-05 出版日期:2018-06-28 发布日期:2018-08-03
通讯作者: Chaohe Yang,E-mail address:yangch@upc.edu.cn;Jian Shen,E-mail address:js_xtuhzy@xtu.edu.cn
基金资助:
Supported by the China Postdoctoral Science Foundation (2017 M612374), the Natural Science Foundation of Shandong Province (ZR2017BB007), the Postdoctoral Research Funding of Shandong Province (201703016), the Qingdao Postdoctoral Research Funding (BY20170210), the Fundamental Research Funding of Qingdao (17-1-1-67-jch, 17-1-1-80-jch), the Fundamental Research Funds for the Central Universities (18CX02145A, 17CX02017A), the New Faculty Start-up Funding from China University of Petroleum (YJ201601058) and the Natural Science Foundation of China (21606254).

Selective propylene epoxidation in liquid phase using highly dispersed Nb catalysts incorporated in mesoporous silicates

Wenjuan Yan¹, Yuhui Wu¹, Xiang Feng¹, Chaohe Yang¹, Xin Jin¹, Jian Shen²

1 State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Qingdao 266580, China;
2 Department of Environmental Science and Engineering, Xiangtan University, Xiangtan 411105, China

Received:2017-11-30 Revised:2018-03-05 Online:2018-06-28 Published:2018-08-03
Contact: Chaohe Yang,E-mail address:yangch@upc.edu.cn;Jian Shen,E-mail address:js_xtuhzy@xtu.edu.cn
Supported by:
Supported by the China Postdoctoral Science Foundation (2017 M612374), the Natural Science Foundation of Shandong Province (ZR2017BB007), the Postdoctoral Research Funding of Shandong Province (201703016), the Qingdao Postdoctoral Research Funding (BY20170210), the Fundamental Research Funding of Qingdao (17-1-1-67-jch, 17-1-1-80-jch), the Fundamental Research Funds for the Central Universities (18CX02145A, 17CX02017A), the New Faculty Start-up Funding from China University of Petroleum (YJ201601058) and the Natural Science Foundation of China (21606254).

摘要/Abstract

摘要： Selective propylene epoxidation to propylene oxide (PO) with hydrogen peroxide (H₂O₂) was carried out in a catalytic semi-batch reactor. High propylene epoxidation activity (44 h^-1) was observed over Nb based mesoporous silicate materials Nb-TUD-1 under mild operating conditions. The physical and chemical properties of the Nb based silicates characterized using BET, FTIR, TPD, TEM and UV-Vis revealed that the site isolation and surface acidity are crucial for PO production. Catalyst synthesis methods were investigated for their effects on PO productivity, PO selectivity and H₂O₂ utilization efficiency. It is found that Nb-TUD-1 material synthesized by the sol-gel method is more active and selective than impregnated materials for liquid phase propylene epoxidation. Surface characterization confirms that thus synthesized Nb-TUD-1 catalysts have more Lewis acidity and less Bronsted acidity compared to the catalysts by impregnation.

关键词: Propylene, Epoxidation, Propylene oxide, TUD-1, Niobium, mesoporous materials

Abstract: Selective propylene epoxidation to propylene oxide (PO) with hydrogen peroxide (H₂O₂) was carried out in a catalytic semi-batch reactor. High propylene epoxidation activity (44 h^-1) was observed over Nb based mesoporous silicate materials Nb-TUD-1 under mild operating conditions. The physical and chemical properties of the Nb based silicates characterized using BET, FTIR, TPD, TEM and UV-Vis revealed that the site isolation and surface acidity are crucial for PO production. Catalyst synthesis methods were investigated for their effects on PO productivity, PO selectivity and H₂O₂ utilization efficiency. It is found that Nb-TUD-1 material synthesized by the sol-gel method is more active and selective than impregnated materials for liquid phase propylene epoxidation. Surface characterization confirms that thus synthesized Nb-TUD-1 catalysts have more Lewis acidity and less Bronsted acidity compared to the catalysts by impregnation.

Key words: Propylene, Epoxidation, Propylene oxide, TUD-1, Niobium, mesoporous materials

Wenjuan Yan, Yuhui Wu, Xiang Feng, Chaohe Yang, Xin Jin, Jian Shen. Selective propylene epoxidation in liquid phase using highly dispersed Nb catalysts incorporated in mesoporous silicates[J]. Chinese Journal of Chemical Engineering, 2018, 26(6): 1278-1284.

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Selective propylene epoxidation in liquid phase using highly dispersed Nb catalysts incorporated in mesoporous silicates

Selective propylene epoxidation in liquid phase using highly dispersed Nb catalysts incorporated in mesoporous silicates

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