Oxidative dehydrogenation of propane to propene with carbon dioxide catalyzed by PtSn/Ce<sub>1−<italic>x</italic></sub>Zr<italic><sub>x</sub>&
<p indent="0mm">The oxidative dehydrogenation of propane with carbon dioxide (CO<sub>2</sub>-ODP) is an energy-saving, efficient, and environmentally friendly process for propene production. However, the development of a high-performance catalyst is the key for its industrialization. Based on the understanding that the catalytic CO<sub>2</sub>-ODP involves the simultaneous activation of propane and CO<sub>2</sub> molecules, this work investigates the effect of oxygen defects on the catalytic performance of CO<sub>2</sub>-ODP over PtSn/Ce<sub>1−<italic>x</italic></sub>Zr<italic><sub>x</sub></italic>O<sub>2</sub> (<italic>x</italic> = 0, 0.4, 0.5, 0.7 and 1.0) from the perspective of the enhanced CO<sub>2</sub> activation. The results show that the CO<sub>2</sub>-ODP reaction catalyzed by PtSn/Ce<sub>1−<italic>x</italic></sub>Zr<italic><sub>x</sub></italic>O<sub>2</sub> follows the Mars-van-Krevelen redox mechanism. In comparison with PtSn/CeO<sub>2</sub>, the introduction of Zr leads to the formation of Ce<sub>1−<italic>x</italic></sub>Zr<italic><sub>x</sub></italic>O<sub>2</sub> solid solution in the catalyst, which increases the content of oxygen defects. As a result, the dispersion of Pt, and the ability for the adsorption and activation of CO<sub>2</sub> are increased, thus significantly enhance the catalytic performance for CO<sub>2</sub>-ODP. Among them, the PtSn/Ce<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub> catalyst shows the most oxygen defects, the highest Pt dispersion, and the best ability for the adsorption and activation of CO<sub>2</sub>, so that can supplement the consumed lattice oxygen species over the catalyst during the reaction timely, and promote the redox cycles, resulting in the highest propane conversion (31%). The analysis of the catalyst deactivation indicates that PtSn/Ce<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub> shows the best ability for the adsorption and activation of CO<sub>2</sub> to supplement the consumed lattice oxygen species, which not only maintains the redox cycles during the reaction, but also promotes the reverse Boudouard reaction and eliminates the carbon deposition, leading to the highest stability.
Authors
- Xing Ren
- Guoqing Yang
- Zhongwen Liu
Publication Details
- Journal
- Scientia Sinica Chimica
- Published
- 2024-09-14
- DOI
- https://doi.org/10.1360/ssc-2024-0111
- Primary Topic
- Catalysis and Oxidation Reactions
- Type
- article
- Field-Weighted Citation Impact
- 0.00