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 language | English |
|---|---|
| Pages (from-to) | 136-140 |
| Number of pages | 5 |
| Journal | ChemCatChem |
| Volume | 10 |
| Issue number | 1 |
| DOIs | |
| Publication status | Published - 9 Jan 2018 |
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Keywords
- Fischer–Tropsch
- in-situ characterization
- IR spectroscopy
- isotopic labeling
- reaction mechanisms
Cite this
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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 journal › Article › Academic › peer-review
TY - JOUR
T1 - Mechanism of carbon monoxide dissociation on a cobalt Fischer–Tropsch catalyst
AU - Chen, Wei
AU - Zijlstra, Bart
AU - Filot, Ivo A.W.
AU - Pestman, Robert
AU - Hensen, Emiel J.M.
PY - 2018/1/9
Y1 - 2018/1/9
N2 - 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.
AB - 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.
KW - Fischer–Tropsch
KW - in-situ characterization
KW - IR spectroscopy
KW - isotopic labeling
KW - reaction mechanisms
UR - http://www.scopus.com/inward/record.url?scp=85035108629&partnerID=8YFLogxK
U2 - 10.1002/cctc.201701203
DO - 10.1002/cctc.201701203
M3 - Article
C2 - 29399207
AN - SCOPUS:85035108629
VL - 10
SP - 136
EP - 140
JO - ChemCatChem
JF - ChemCatChem
SN - 1867-3899
IS - 1
ER -