C2H2 semi-hydrogenation on the Pdshell@Mcore (M = Cu, Ag, Au) alloy catalysts: The influence of shell Pd ensemble form on the catalytic activity and selectivity. (14th December 2021)

• Record Type: Journal Article
• Authors: Qi, Yamin; Shao, Xiuxiu; Wang, Baojun; Li, Debao; Ling, Lixia; Zhang, Riguang
• Is Part Of: Chemical engineering science. Volume 245(2021)
• Publication Date: 2021-12-14
• Subjects: C2H2 semi-hydrogenation -- Pd@M catalyst -- Shell Pd ensemble -- Catalytic performance -- Electronic structure analysis; Chemical engineering -- Periodicals; Génie chimique -- Périodiques; Chemical engineering; Periodicals; Electronic journals; 660
• DOI: 10.1016/j.ces.2021.116941
• Languages: English
• ISSNs: 0009-2509

Abstract

Graphical abstract: Highlights: The catalytic performance of C2 H2 semi-hydrogenation on the Pd@M catalysts strongly depends on the shell Pd ensemble form. Pd7 @M with the Pd ensemble of dimer and trimer exhibits the best catalytic performance toward C2 H4 formation. The activity and selectivity of C2 H4 formation has a volcano curve relationship with the d -band center of Pd@M catalysts. Pd7 @M catalysts with the best catalytic performance are attributed to the moderate d -band center. Abstract: To reveal the influence of shell Pd ensemble form in the core–shell Pd@M (M = Cu, Ag, Au) catalysts on the catalytic performance of C2 H2 semi-hydrogenation, the mechanism of C2 H2 semi-hydrogenation on Pd@M catalysts with different shell Pd ensemble are fully investigated using DFT and microkinetic modeling calculations. The results show that C2 H4 selectivity and its formation activity closely depend on the shell Pd ensemble form; among Pd@Cu with different shell Pd ensemble, C2 H4 selectivity and its formation activity has a volcano curve relationship with the d -band center of Pd@Cu, in which Pd7 @Cu with the shell Pd ensemble of dimer and trimer is the best due to the moderate d -band center. The same things also occur on the Pd@Ag and Pd@Au. It is proposed that controlling the ensemble form of shell noble-metal Pd may be a good way to adjust the catalytic performance toward the selective hydrogenation of other alkynes.