脱氢
丙烯
丙烷
催化作用
选择性
化学
氧化还原
甲烷
无机化学
光化学
有机化学
作者
Guoqing Yang,Xing Ren,Vita A. Kondratenko,Hengbo Zhang,Evgenii V. Kondratenko,Zhong-Wen Liu
出处
期刊:Nano Research
[Springer Science+Business Media]
日期:2023-01-10
卷期号:16 (5): 6237-6250
被引量:51
标识
DOI:10.1007/s12274-022-5316-0
摘要
The oxidative dehydrogenation of propane with CO 2 (CO 2 -ODP) is a promising technology for the efficient production of propene in tandem with CO 2 reduction to CO. However, the rational design of high-performance catalysts for this green process is still challenged by limited understanding of the nature of active sites and the reaction mechanism. In this work, the effects of SnO 2 promoter on Pt/CeO 2 activity and propene selectivity in CO 2 -ODP are elucidated through varying the Sn/Pt molar ratio. When the ratio increases, propane conversion gradually decreases, while the propene selectivity increases. These dependences are explained by increasing the electron density of Pt through the promoter. The strength of this effect is determined by the Sn/Pt ratio. Owing to the electronic changes of Pt, CO 2 -ODP becomes more favorable than the undesired CO 2 reforming of propane. Sn-modified Pt—O—Ce bonds are reasonably revealed as the active sites for CO 2 -ODP occurring through a redox mechanism involving the activation of CO 2 over oxygen vacancies at Sn-modified Pt and CeO 2 boundaries. These atomic-scale understandings are important guidelines for purposeful development of high-performance Pt-based catalysts for CO 2 -ODP.
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