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A DFT and KMC based study on the mechanism of the water gas shift reaction on the Pd(100) surface

Chutia, A; Thetford, A; Stamatakis, M; Catlow, CRA; (2020) A DFT and KMC based study on the mechanism of the water gas shift reaction on the Pd(100) surface. Physical Chemistry Chemical Physics , 22 (6) pp. 3620-3632. 10.1039/C9CP05476F. Green open access

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Abstract

We present a combined density functional theory (DFT) and Kinetic Monte Carlo (KMC) study of the water gas shift (WGS) reaction on the Pd(100) surface. We propose a mechanism comprising both the redox and the associative pathways for the WGS within a single framework, which consists of seven core elementary steps, which in turn involve splitting of a water molecule followed by the production of an H-atom and an OH-species on the Pd(100) surface. In the following steps, these intermediates then recombine with each other and with CO leading to the evolution of CO2, and H2. Seven other elementary steps, involving the diffusion and adsorption of the surface intermediate species are also considered for a complete description of the mechanism. The geometrical and electronic properties of each of the reactants, products, and the transition states of the core elementary steps are presented. We also discuss the analysis of Bader charges and spin densities for the reactants, transition states and the products of these elementary steps. Our study indicates that the WGS reaction progresses simultaneously via the direct oxidation and the carboxyl paths on the Pd(100) surface.

Type: Article
Title: A DFT and KMC based study on the mechanism of the water gas shift reaction on the Pd(100) surface
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/C9CP05476F
Publisher version: https://doi.org/10.1039/C9CP05476F
Language: English
Additional information: This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (http://creativecommons.org/licenses/by/3.0/).
UCL classification: UCL
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
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10090027
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