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Volume 229, 2021
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The role of oxygenated species in the catalytic self-coupling of MeOH on O pre-covered Au(111)

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Abstract

The oxidation of alcohols plays a central role in the valorisation of biomass, in particular when performed with a non-toxic oxidant such as O2. Aerobic oxidation of methanol on gold has attracted attention lately and the main steps of its mechanism have been described experimentally. However, the exact role of O and OH on each elementary step and the effect of the interactions between adsorbates are still not completely understood. Here we investigate the mechanism of methanol oxidation to HCOOCH3 and CO2. We use Density Functional Theory (DFT) to assess the energetics of the underlying pathways, and subsequently build lattice kinetic Monte Carlo (kMC) models of increasing complexity, to elucidate the role of different oxygenates. Detailed comparisons of our simulation results with experimental temperature programmed desorption (TPD) spectra enable us to validate the mechanism and identify rate determining steps. Crucially, taking into account dispersion (van der Waals forces) and adsorbate–adsorbate lateral interactions are both important for reproducing the experimental data.

Graphical abstract: The role of oxygenated species in the catalytic self-coupling of MeOH on O pre-covered Au(111)

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Submitted
09 Dec 2019
Accepted
17 Jan 2020
First published
20 Jan 2020

This article is Open Access

Faraday Discuss., 2021,229, 251-266
Article type
Paper

The role of oxygenated species in the catalytic self-coupling of MeOH on O pre-covered Au(111)

R. Réocreux, I. Fampiou and M. Stamatakis, Faraday Discuss., 2021, 229, 251
DOI: 10.1039/C9FD00134D

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