Roldan Martinez, Alberto  ORCID: https://orcid.org/0000-0003-0353-9004 and de Leeuw, Nora H. ORCID: https://orcid.org/0000-0002-8271-0545
2019.
A density functional theory study of the hydrogenation and reduction of the thio-spinel Fe3S4{111} surface.
Physical Chemistry Chemical Physics
10.1039/C8CP06371K
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Abstract
The mineral greigite, Fe3S4, shows promising electro-reduction activity, especially towards carbon dioxide conversion to small organic molecules. We have employed density functional theory calculations with correction for the long-range dispersion forces to investigate the behavior of hydrogen on the greigite{111} surface. We have studied the adsorption, diffusion, surface reduction and associative (i.e. Volmer–Tafel mechanism) and molecular desorption of hydrogen as a function of its coverage. We found that (i) the H ad-atoms adsorb on S sites far from metallic centres in the topmost surface layer; (ii) the reduction of greigite by hydrogen is energetically unfavorable at any surface coverage; and (iii) molecular hydrogen evolution has a transition state at ∼0.5 eV above the energy of the reactants on Fe3S4{111}, which is very similar to the barrier found experimentally on Pt{111}. We have also determined the electrode potential under room conditions at which the H2 evolution reaction becomes energetically barrierless.
| Item Type: | Article |
|---|---|
| Date Type: | Published Online |
| Status: | Published |
| Schools: | Professional Services > Advanced Research Computing @ Cardiff (ARCCA) Research Institutes & Centres > Cardiff Catalysis Institute (CCI) Schools > Chemistry |
| Publisher: | Royal Society of Chemistry |
| ISSN: | 1463-9076 |
| Funders: | EPSRC |
| Date of First Compliant Deposit: | 22 January 2019 |
| Date of Acceptance: | 16 November 2018 |
| Last Modified: | 05 Aug 2024 15:17 |
| URI: | https://orca.cardiff.ac.uk/id/eprint/118611 |
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