Coverage effects in CO dissociation on metallic cobalt nanoparticles

Bart Zijlstra, Robin Broos, Wei Chen, Heiko Oosterbeek, Ivo Filot, Emiel Hensen (Corresponding author)

Onderzoeksoutput: Bijdrage aan tijdschriftTijdschriftartikelAcademicpeer review

15 Citaten (Scopus)
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Samenvatting

The active site of CO dissociation on a cobalt nanoparticle, relevant to the Fischer-Tropsch reaction, can be computed directly using density functional theory. We investigate how the activation barrier for direct CO dissociation depends on CO coverage for step-edge and terrace cobalt sites. Whereas on terrace sites increasing coverage results in a substantial increase of the direct CO dissociation barrier, we find that this barrier is nearly independent of CO coverage for the step-edge sites on corrugated surfaces. A detailed electronic analysis shows that this difference is due to the flexibility of the adsorbed layer, minimizing Pauli repulsion during the carbon-oxygen bond dissociation reaction on the step-edge site. We constructed a simple first-principles microkinetic model that not only reproduces experimentally observed rates but also shows how migration of carbon species between step-edge and terrace sites contributes to methane formation.
Originele taal-2Engels
Pagina's (van-tot)7365-7372
Aantal pagina's8
TijdschriftACS Catalysis
Volume9
Nummer van het tijdschrift8
DOI's
StatusGepubliceerd - 2 aug 2019

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