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 , 11 (20) pp. 8751-8757. 10.1021/acs.jpclett.0c02455.

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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.

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