Citation: Xiangyang Ji, Yishuang Chen, Peng Zhang, Shaojia Song, Jian Liu, Weiyu Song. Boosting the first C–H bond activation of propane on rod-like V/CeO₂ catalyst by photo-assisted thermal catalysis[J]. Chinese Chemical Letters, ;2025, 36(5): 110719. doi: 10.1016/j.cclet.2024.110719 shu

Boosting the first C–H bond activation of propane on rod-like V/CeO₂ catalyst by photo-assisted thermal catalysis

Xiangyang Ji ^a ,
Yishuang Chen ^a ,
Peng Zhang ^b ,
Shaojia Song ^c ,
Jian Liu ^{a, *,} ,
Weiyu Song ^{a, *,}

a.
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China
b.
Petrochemical Research Institute, PetroChina Company Limited, Beijing 102206, China
c.
State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan 030024, China

liujian@cup.edu.cn

songwy@cup.edu.cn

Received Date: 23 October 2024
Revised Date: 2 December 2024
Accepted Date: 3 December 2024
Available Online: 3 December 2024

Figures(4)

Crystalized CeO₂ structures were typically considered potential photocatalysts due to their great capacity to alter the active sites’ size and ability to absorb light. However, the controllable fabrication of well-defined hierarchical structures of CeO₂ with high reactive facets is significant and challenging. Herein, a series of CeO₂ supports including hierarchical flower-like (F-CeO₂), ball-like (B-CeO₂), cube-like (CCeO₂), and rod-like CeO₂(R-CeO₂) supports were prepared by hydrothermal method (B-CeO₂, R-CeO₂ and CCeO₂) or ice-bath method (F-CeO₂) respectively. V atoms were selected as the active atoms and loaded on these supports. Their structure-activity relationship in photo-assisted thermal propane dehydrogenation (PTPDH) was investigated systematically. The samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N₂ adsorption-desorption isotherms, and Fourier transform infrared spectrum. Results show that R-CeO₂ support exhibits the biggest surface area thus achieving the best dispersion of VO_x species. UV–vis spectrum and photoluminescence spectrum indicate that V/F-CeO₂ has the best light adsorption property and V/R-CeO₂ has the best carrier migration capacity. The activity tests demonstrate that the V/R-CeO₂ has the largest net growth rate and the V/F-CeO₂ has the biggest relative growth ratio. Furthermore, the non-thermal effect was confirmed by the kinetic method, which lowers the propane reaction orders, selectively promoting the first C–H bond activation. The light radiation TPSR experiment confirmed this point. DFT calculations show a good linear relationship between the energy barrier and the exchanged electron number. It inspires the design of high-reactive facets for boosting the intrinsic activity of the C–H bond in photo-assisted thermal chemical processes.
- Propane dehydrogenation,
- Facet engineering,
- Photothermal effect,
- Electrons transfer,
- Reaction kinetics
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Boosting the first C–H bond activation of propane on rod-like V/CeO2 catalyst by photo-assisted thermal catalysis

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通讯作者: 陈斌, bchen63@163.com

Boosting the first C–H bond activation of propane on rod-like V/CeO₂ catalyst by photo-assisted thermal catalysis