Issue 41, 2019

Selectivity for ethanol partial oxidation: the unique chemistry of single-atom alloy catalysts on Au, Ag, and Cu(111)

Abstract

Recently, we found that the atomic ensemble effect is the dominant effect influencing catalysis on surfaces alloyed with 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 possess unique dehydrogenation selectivity towards ethanol (EtOH) partial oxidation, using knowledge of the alloying effects from density functional theory calculations. We found that doping of a strong-binding single-atom element (e.g., Ir, Pd, Pt, and Rh) 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.

Graphical abstract: Selectivity for ethanol partial oxidation: the unique chemistry of single-atom alloy catalysts on Au, Ag, and Cu(111)

Supplementary files

Article information

Article type
Paper
Submitted
02 Mai 2019
Accepted
15 Mai 2019
First published
15 Mai 2019

J. Mater. Chem. A, 2019,7, 23868-23877

Author version available

Selectivity for ethanol partial oxidation: the unique chemistry of single-atom alloy catalysts on Au, Ag, and Cu(111)

H. Li, W. Chai and G. Henkelman, J. Mater. Chem. A, 2019, 7, 23868 DOI: 10.1039/C9TA04572D

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