Coverage effects in CO dissociation on metallic cobalt nanoparticles

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

Research output: Contribution to journalArticleAcademicpeer-review

13 Citations (Scopus)
101 Downloads (Pure)

Abstract

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.
Original languageEnglish
Pages (from-to)7365-7372
Number of pages8
JournalACS Catalysis
Volume9
Issue number8
DOIs
Publication statusPublished - 2 Aug 2019

Keywords

  • DFT
  • Fischer-Tropsch synthesis
  • activation energy
  • lateral interactions
  • microkinetic modeling

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