A DFT and KMC based study on the mechanism of the water gas shift reaction on the Pd(100) surface
| Autor: | Arunabhiram Chutia, Michail Stamatakis, C. Richard A. Catlow, Adam Thetford |
|---|---|
| Rok vydání: | 2020 |
| Předmět: |
Materials science
Diffusion General Physics and Astronomy 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Redox Water-gas shift reaction Transition state 0104 chemical sciences Adsorption Chemical physics F100 Chemistry Molecule Density functional theory Kinetic Monte Carlo Physical and Theoretical Chemistry 0210 nano-technology |
| Zdroj: | Physical chemistry chemical physics : PCCP. 22(6) |
| ISSN: | 1463-9084 1463-9076 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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