Discriminating the Role of Surface Hydride and Hydroxyl for Acetylene Semihydrogenation over Ceria through In Situ Neutron and Infrared Spectroscopy

Ceria has been used as a hydrogenation catalyst especially in selective alkyne hydrogenation, but the reaction mechanism regarding the role of different surface hydrogen species remains unclear. In this work, we utilized in situ neutron and infrared vibration spectroscopy to show the catalytic role...

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Veröffentlicht in:ACS catalysis 2020-05, Vol.10 (9), p.5278-5287
Hauptverfasser: Moon, Jisue, Cheng, Yongqiang, Daemen, Luke L, Li, Meijun, Polo-Garzon, Felipe, Ramirez-Cuesta, Anibal J, Wu, Zili
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Sprache:eng
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Zusammenfassung:Ceria has been used as a hydrogenation catalyst especially in selective alkyne hydrogenation, but the reaction mechanism regarding the role of different surface hydrogen species remains unclear. In this work, we utilized in situ neutron and infrared vibration spectroscopy to show the catalytic role of cerium hydride (Ce–H) and hydroxyl (OH) groups in acetylene hydrogenation over ceria surfaces with different degree of reduction. In situ inelastic neutron scattering spectroscopy (INS) proved that not only Ce–H but also surface atomic hydrogen species on the reduced ceria surface can participate in acetylene semihydrogenation. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results implied that bridging OH groups both on the oxidized and reduced ceria are active in the selective hydrogenation of acetylene. It appears that surface Ce–H is more reactive than the coexisting OH species on the reduced ceria surface, but over-reduction of ceria also results in strongly bound species that may lead to catalyst deactivation. These spectroscopic results clearly explain the reaction mechanism including not only the surface chemistry but also the nature of the active hydrogen species for selective hydrogenation over ceria, providing insights into the design of more active and stable ceria-based catalysts for hydrogenation reactions.
ISSN:2155-5435
2155-5435
DOI:10.1021/acscatal.0c00808