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Controlling Hydrocarbon (De)Hydrogenation Pathways with Bifunctional PtCu Single-Atom Alloys.

Réocreux, R; Kress, PL; Hannagan, RT; Çınar, V; Stamatakis, M; Sykes, ECH; (2020) Controlling Hydrocarbon (De)Hydrogenation Pathways with Bifunctional PtCu Single-Atom Alloys. Journal of Physical Chemistry Letters pp. 8751-8757. 10.1021/acs.jpclett.0c02455. (In press).

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Abstract

The conversions of surface-bound alkyl groups to alkanes and alkenes are important steps in many heterogeneously catalyzed reactions. On the one hand, while Pt is ubiquitous in industry because of its high activity toward C-H activation, many Pt-based catalysts tend to overbind reactive intermediates, which leads to deactivation by carbon deposition and coke formation. On the other hand, Cu binds intermediates more weakly than Pt, but activation barriers tend to be higher on Cu. We examine the reactivity of ethyl, the simplest alkyl group that can undergo hydrogenation and dehydrogenation via β-elimination, and show that isolated Pt atoms in Cu enable low-temperature hydrogenation of ethyl, unseen on Cu, while avoiding the decomposition pathways on pure Pt that lead to coking. Furthermore, we confirm the predictions of our theoretical model and experimentally demonstrate that the selectivity of ethyl (de)hydrogenation can be controlled by changing the surface coverage of hydrogen.

Type: Article
Title: Controlling Hydrocarbon (De)Hydrogenation Pathways with Bifunctional PtCu Single-Atom Alloys.
Location: United States
DOI: 10.1021/acs.jpclett.0c02455
Publisher version: https://doi.org/10.1021/acs.jpclett.0c02455
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: Hydrogen,Hydrocarbons,Platinum,Hydrogenation,Ethyl groups
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10111700
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