Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect

doi:10.1016/j.cjche.2020.08.006

中国化学工程学报 ›› 2021, Vol. 34 ›› Issue (6): 77-86.DOI: 10.1016/j.cjche.2020.08.006

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect

Zhibin Deng¹, Xing Ge², Wenting Zhang³, Shizhong Luo³, Jun Shen³, Fangli Jing³, Wei Chu³

1 College of Civil Aviation Safety Engineering, Civil Aviation Flight University of China, Guanghan 618307, China;
2 Sinopec Petroleum Exploration and Production Research Institute, Northwest Oilfield Branch, Urumqi 830011, China;
3 School of Chemical Engineering, Sichuan University, Chengdu 610065, China

收稿日期:2020-04-22 修回日期:2020-07-09 出版日期:2021-06-28 发布日期:2021-08-30
通讯作者: Shizhong Luo, Fangli Jing
基金资助:
We would like to acknowledge the financial supports from National Natural Science Foundation of China (No. 21603153), Science and Technology Department of Sichuan Province (No. 2016HH0026) and the Fundamental Research Funds for the Central Universities (No. YJ201544).

Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect

Zhibin Deng¹, Xing Ge², Wenting Zhang³, Shizhong Luo³, Jun Shen³, Fangli Jing³, Wei Chu³

1 College of Civil Aviation Safety Engineering, Civil Aviation Flight University of China, Guanghan 618307, China;
2 Sinopec Petroleum Exploration and Production Research Institute, Northwest Oilfield Branch, Urumqi 830011, China;
3 School of Chemical Engineering, Sichuan University, Chengdu 610065, China

Received:2020-04-22 Revised:2020-07-09 Online:2021-06-28 Published:2021-08-30
Contact: Shizhong Luo, Fangli Jing
Supported by:
We would like to acknowledge the financial supports from National Natural Science Foundation of China (No. 21603153), Science and Technology Department of Sichuan Province (No. 2016HH0026) and the Fundamental Research Funds for the Central Universities (No. YJ201544).

摘要/Abstract

摘要： SBA-15 with varied pore size from 4 to 8 nm were synthesized by tuning the temperature of hydrothermal treatment, the supports were then used to load the active phase CrO_x through a conventional impregnation method. The resulting catalysts were characterized by small/wide angle XRD, N₂ adsorption/desorption, FT-IR, TEM-EDX, XPS, TPR and CO₂-TPD to study the feature of structure, surface chemical state, redox and basicity. It was found from these results that the metal species could be well dispersed on catalysts with larger pore size. Cr⁶⁺ species could enter into the framework by substituting the Si atoms of SBA-15, and Cr³⁺ mainly exist on extra framework. Pore size had profound effects on reducibility, surface composition and basicity. Cr⁶⁺ species were necessary to activate the C-H bonds of alkanes, while the basicity played an important role in activating C-O bonds of CO₂. The best performances were achieved over the sample Cr supported on SBA-15 with a pore diameter of 7 nm in oxidative dehydrogenation of ethane in the presence of CO₂.

关键词: Ethylene, SBA-15, Pore size effect, Cr catalysts, Heterogeneous catalysis

Abstract: SBA-15 with varied pore size from 4 to 8 nm were synthesized by tuning the temperature of hydrothermal treatment, the supports were then used to load the active phase CrO_x through a conventional impregnation method. The resulting catalysts were characterized by small/wide angle XRD, N₂ adsorption/desorption, FT-IR, TEM-EDX, XPS, TPR and CO₂-TPD to study the feature of structure, surface chemical state, redox and basicity. It was found from these results that the metal species could be well dispersed on catalysts with larger pore size. Cr⁶⁺ species could enter into the framework by substituting the Si atoms of SBA-15, and Cr³⁺ mainly exist on extra framework. Pore size had profound effects on reducibility, surface composition and basicity. Cr⁶⁺ species were necessary to activate the C-H bonds of alkanes, while the basicity played an important role in activating C-O bonds of CO₂. The best performances were achieved over the sample Cr supported on SBA-15 with a pore diameter of 7 nm in oxidative dehydrogenation of ethane in the presence of CO₂.

Key words: Ethylene, SBA-15, Pore size effect, Cr catalysts, Heterogeneous catalysis

Zhibin Deng, Xing Ge, Wenting Zhang, Shizhong Luo, Jun Shen, Fangli Jing, Wei Chu. Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect[J]. 中国化学工程学报, 2021, 34(6): 77-86.

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Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect

Oxidative dehydrogenation of ethane with carbon dioxide over silica molecular sieves supported chromium oxides: Pore size effect

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