Dehydrogenation of Propane to Propylene by a Pd/Cu Single-Atom Catalyst: Insight from First-Principles Calculations
2015 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 119, no 2, 1016-1023 p.Article in journal (Refereed) Published
The catalytic properties of the single-Pd-doped Cu55 nanoparticle toward propane dehydrogenation have been systemically investigated by first-principles calculations, and the possible reaction mechanisms and effects of the single and multiple Pd doping on the catalytic activity have been discussed. Calculations reveal that the low-energy catalytic conversion of propane to propylene by the Pd/Cu single-atom catalyst comprises the initial crucial C–H bond breaking at either the methyl or methylene group, the facile diffusion of detached H atoms on the Cu surface, and the subsequent C–H bond dissociation activation of the adsorbed propyl species. The single-Pd-doped Cu55 nanoparticle shows remarkable activity toward C–H bond activation, and the presence of relatively inactive Cu surface is beneficial for the coupling and desorption of detached H atoms and can reduce side reactions such as deep dehydrogenation and C–C bond breaking. The single-Pd-doped Cu55 cluster bears good balance between the maximum use of the noble metal and the activity, and it may serve as a promising single-atom catalyst toward selective dehydrogenation of propane.
Place, publisher, year, edition, pages
2015. Vol. 119, no 2, 1016-1023 p.
Atoms, Calculations, Catalyst activity, Catalysts, Chemical activation, Dehydrogenation, Nanoparticles, Precious metals, Propane, Propylene, C-H bond dissociation, Catalytic conversion, Catalytic properties, CH-bond activation, Dehydrogenation of propanes, First-principles calculation, Propane dehydrogenation, Reaction mechanism
IdentifiersURN: urn:nbn:se:kth:diva-159882DOI: 10.1021/jp508625bISI: 000348094000017ScopusID: 2-s2.0-84949115465OAI: oai:DiVA.org:kth-159882DiVA: diva2:787517
QC 201502112015-02-102015-02-102015-03-09Bibliographically approved