Mechanism of carbon monoxide dissociation on a cobalt Fischer–Tropsch catalyst

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Abstract

The way in which the triple bond in CO dissociates, a key reaction step in the Fischer–Tropsch (FT) reaction, is a subject of intense debate. Direct CO dissociation on a Co catalyst was probed by 12C16O/13C18O scrambling in the absence and presence of H2. The initial scrambling rate without H2 was significantly higher than the rate of CO consumption under CO hydrogenation conditions, which indicated that the surface contained sites sufficiently reactive to dissociate CO without the assistance of H atoms. Only a small fraction of the surface was involved in CO scrambling. The minor influence of CO scrambling and CO residence time on the partial pressure of H2 showed that CO dissociation was not affected by the presence of H2. The positive H2 reaction order was correlated to the fact that the hydrogenation of adsorbed C and O atoms was slower than CO dissociation. Temperature-programmed in situ IR spectroscopy underpinned the conclusion that CO dissociation does not require H atoms.

Original languageEnglish
Pages (from-to)136-140
Number of pages5
JournalChemCatChem
Volume10
Issue number1
DOIs
Publication statusPublished - 9 Jan 2018

Fingerprint

Carbon Monoxide
Cobalt
Carbon monoxide
carbon monoxide
cobalt
dissociation
catalysts
Catalysts
Atoms
Hydrogenation
hydrogenation
atoms
Partial pressure
partial pressure
Infrared spectroscopy
spectroscopy
Temperature
temperature

Keywords

  • Fischer–Tropsch
  • in-situ characterization
  • IR spectroscopy
  • isotopic labeling
  • reaction mechanisms

Cite this

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title = "Mechanism of carbon monoxide dissociation on a cobalt Fischer–Tropsch catalyst",
abstract = "The way in which the triple bond in CO dissociates, a key reaction step in the Fischer–Tropsch (FT) reaction, is a subject of intense debate. Direct CO dissociation on a Co catalyst was probed by 12C16O/13C18O scrambling in the absence and presence of H2. The initial scrambling rate without H2 was significantly higher than the rate of CO consumption under CO hydrogenation conditions, which indicated that the surface contained sites sufficiently reactive to dissociate CO without the assistance of H atoms. Only a small fraction of the surface was involved in CO scrambling. The minor influence of CO scrambling and CO residence time on the partial pressure of H2 showed that CO dissociation was not affected by the presence of H2. The positive H2 reaction order was correlated to the fact that the hydrogenation of adsorbed C and O atoms was slower than CO dissociation. Temperature-programmed in situ IR spectroscopy underpinned the conclusion that CO dissociation does not require H atoms.",
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Mechanism of carbon monoxide dissociation on a cobalt Fischer–Tropsch catalyst. / Chen, Wei; Zijlstra, Bart; Filot, Ivo A.W.; Pestman, Robert; Hensen, Emiel J.M.

In: ChemCatChem, Vol. 10, No. 1, 09.01.2018, p. 136-140.

Research output: Contribution to journalArticleAcademicpeer-review

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