SCI和EI收录∣中国化工学会会刊

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. 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. 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: 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 CrOx 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 CrOx 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