University of Sussex
Browse
1.2888933.pdf (545.78 kB)

Hydrogenation of CO on a silica surface: an embedded cluster approach

Download (545.78 kB)
journal contribution
posted on 2023-06-08, 17:18 authored by T P M Goumans, C Richard A Catlow, Wendy BrownWendy Brown
The 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.

History

Publication status

  • Published

File Version

  • Published version

Journal

Journal of Chemical Physics

ISSN

0021-9606

Publisher

American Institute of Physics

Issue

13

Volume

128

Department affiliated with

  • Chemistry Publications

Full text available

  • Yes

Peer reviewed?

  • Yes

Legacy Posted Date

2014-07-22

First Open Access (FOA) Date

2014-07-22

First Compliant Deposit (FCD) Date

2014-07-22

Usage metrics

    University of Sussex (Publications)

    Categories

    No categories selected

    Exports

    RefWorks
    BibTeX
    Ref. manager
    Endnote
    DataCite
    NLM
    DC