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 ca...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.展开更多
基金the National Natural Science Foundation of China(No.21636006)the Fundamental Research Funds for the Central Universities(No.GK201901001).G.Q.Y.acknowledges support from the China Scholarship Council.
文摘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.
