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

Réocreux, R; Fampiou, I; Stamatakis, M; (2020) The role of oxygenated species in the catalytic self-coupling of MeOH on O pre-covered Au(111). Faraday Discussions 10.1039/c9fd00134d. (In press). Green open access

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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.

Type: Article
Title: The role of oxygenated species in the catalytic self-coupling of MeOH on O pre-covered Au(111)
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/c9fd00134d
Publisher version: https://doi.org/10.1039/C9FD00134D
Language: English
Additional information: This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence (https://creativecommons.org/licenses/by-nc/3.0/).
UCL classification: UCL
UCL > Provost and Vice Provost Offices
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI: https://discovery.ucl.ac.uk/id/eprint/10090024
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