Selectivity for Ethanol Partial Oxidation: The Unique Chemistry of Single-Atom Alloy Catalysts on Au, Ag, and Cu(111)
Recently, we found that the atomic ensemble effect is the dominant effect influencing catalysis on surfaces alloyed by strong- and weak-binding elements, determining the activity and selectivity of many reactions on the alloy surface. In this study we design single-atom alloys that possesses unique dehydrogenation selectivity towards ethanol (EtOH) partial oxidation, using knowledge of these alloying effects from density functional theory calculations. We found that strong-binding single-atom element (e.g., Ir, Pd, Pt, and Rh) doped into weak-binding inert close-packed substrates (e.g., Au, Ag, and Cu) leads to a highly active and selective initial dehydrogenation at the α-C-H site of adsorbed EtOH. We show that many of these stable single-atom alloy surfaces not only have tunable hydrogen binding, which allows for facile hydrogen desorption, but are also resistant to carbon-coking. More importantly, we show that a rational design of the ensemble geometry can tune the selectivity of a catalytic reaction.
- This article is part of the themed collection: Journal of Materials Chemistry A Emerging Investigators