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Hydrogenation of CO on a silica surface: an embedded cluster approach
journal contribution
posted on 2023-06-08, 17:18 authored by T P M Goumans, C Richard A Catlow, Wendy BrownWendy BrownThe sequential addition of H atoms to CO adsorbed on a siliceous edingtonite surface is studied with an embedded cluster approach, using density functional theory for the quantum mechanical (QM) cluster and a molecular force field for the molecular mechanical (MM) cluster. With this setup, calculated QM/MM adsorption energies are in agreement with previous calculations employing periodic boundary conditions. The catalytic effect of the siliceous edingtonite (100) surface on CO hydrogenation is assessed because of its relevance to astrochemistry. While adsorption of CO on a silanol group on the hydroxylated surface did not reduce the activation energy for the reaction with a H atom, a negatively charged defect on the surface is found to reduce the gas phase barriers for the hydrogenation of both CO and H2C = O. The embedded cluster approach is shown to be a useful and flexible tool for studying reactions on (semi-)ionic surfaces and specific defects thereon. The methodology presented here could easily be applied to study reactions on silica surfaces that are of relevance to other scientific areas, such as biotoxicity of silica dust and geochemistry.
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Publication status
- Published
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- Published version
Journal
Journal of Chemical PhysicsISSN
0021-9606Publisher
American Institute of PhysicsExternal DOI
Issue
13Volume
128Department affiliated with
- Chemistry Publications
Full text available
- Yes
Peer reviewed?
- Yes
Legacy Posted Date
2014-07-22First Open Access (FOA) Date
2014-07-22First Compliant Deposit (FCD) Date
2014-07-22Usage metrics
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