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Effect of surface Pt doping on the reactivity of the Au(111) surface towards methanol dehydrogenation: a first-principles Density Functional Theory investigation
Demirtas, M.; Ustunel, H.; Toffoli, D. Effect of Surface Pt Doping on the Reactivity of Au(111) Surfaces towards Methanol Dehydrogenation: A First-Principles Density Functional Theory Investigation. Molecules2023, 28, 7928.
Demirtas, M.; Ustunel, H.; Toffoli, D. Effect of Surface Pt Doping on the Reactivity of Au(111) Surfaces towards Methanol Dehydrogenation: A First-Principles Density Functional Theory Investigation. Molecules 2023, 28, 7928.
Demirtas, M.; Ustunel, H.; Toffoli, D. Effect of Surface Pt Doping on the Reactivity of Au(111) Surfaces towards Methanol Dehydrogenation: A First-Principles Density Functional Theory Investigation. Molecules2023, 28, 7928.
Demirtas, M.; Ustunel, H.; Toffoli, D. Effect of Surface Pt Doping on the Reactivity of Au(111) Surfaces towards Methanol Dehydrogenation: A First-Principles Density Functional Theory Investigation. Molecules 2023, 28, 7928.
Abstract
The surprisingly high catalytic activity of gold has been known
to the heterogeneous catalysis community since the mid-1980s.
Significant effort has been directed towards improving the reactivity of these
surfaces towards important industrial reactions. One such strategy is
the introduction of small amounts of other metals to create Au-based
surface alloys. In this work, we investigate the synergistic effect of
Pt doping of the Au(111) surface towards decreasing the activation
barrier of the methanol dehydrogenation elementary step, within
first-principles density functional theory. To this aim we construct
several models of \ce{Pt}-doped Au(111) surfaces, including a full
\ce{Pt} overlayer and monolayer. The effect of \ce{Pt} surface doping
is then investigated via the computation of adsorption energies of the
various chemical species involved in the catalytic step, and the
estimation of activation barriers of methanol dehydrogenation. Both
electronic and strain effects induced by \ce{Pt} surface doping concur
in substantially lowering the activation energy barrier of this
important reaction elementary step. Morever, in the presence of
preadsorbed atomic oxygen, \ce{Pt} surface doping can be used to
reduce the activation energy for methanol dehydrogenation to as low as
0.1 eV.
Keywords
Density Functional Theory; Methanol dehydrogenation reaction; Nudged Elastic Band; Activation Energy; Reaction Energy
Subject
Chemistry and Materials Science, Theoretical Chemistry
Copyright:
This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
