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Step enhanced dehydrogenation of ethanol on Rh

Resta, Andrea LU ; Gustafson, Johan LU ; Westerström, Rasmus LU ; Mikkelsen, Anders LU ; Lundgren, Edvin LU ; Andersen, Jesper N LU ; Yang, Ming-Mei; Ma, Xiu-Fang; Bao, Xin-He and Li, Wei-Xue (2008) In Surface Science 602(18). p.3057-3063
Abstract
We have investigated the adsorption and decomposition of ethanol on the Rh(111) and Rh(5 5 3) surfaces at room temperature with special emphasis on the dehydrogenation. We use high resolution Core level photoemission and density functional theory (DFT) based simulations. A detailed analysis of the C1s core level spectra, including analysis of the vibrational fine-structure and comparison to calculated C1s binding energy shifts, shows that the ethanol decomposes into CO, ethylidyne (C2H3) methylidyne (CH), atomic C, and hydrogen. At low ethanol exposures, CH is the dominating hydrocarbon fragment on Rh(111), whereas on Rh(553) atomic C dominates over CH, indicating an enhanced dehydrogenation due to the steps present on the latter surface.... (More)
We have investigated the adsorption and decomposition of ethanol on the Rh(111) and Rh(5 5 3) surfaces at room temperature with special emphasis on the dehydrogenation. We use high resolution Core level photoemission and density functional theory (DFT) based simulations. A detailed analysis of the C1s core level spectra, including analysis of the vibrational fine-structure and comparison to calculated C1s binding energy shifts, shows that the ethanol decomposes into CO, ethylidyne (C2H3) methylidyne (CH), atomic C, and hydrogen. At low ethanol exposures, CH is the dominating hydrocarbon fragment on Rh(111), whereas on Rh(553) atomic C dominates over CH, indicating an enhanced dehydrogenation due to the steps present on the latter surface. At higher ethanol exposures we find a similar behavior of atomic C dominating over hydrocarbons on Rh(553), while on Rh(111) atomic carbon remains a minority species. Our DFT based simulations show that the enhanced dehydrogenation results from a significant lowering of the CH dissociation barrier from Rh(111) to Rh(553), as well as from the dissociation changing from endothermic on Rh(111) to exothermic on Rh(553). (C) 2008 Elsevier B.V. All rights reserved. (Less)
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author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
spectroscopy, synchrotron radiation photoelectron, photoelectron spectroscopy, Density functional calculations, soft X-ray, Photoelectron spectroscopy, Surface chemical reaction, Catalysis, Chemisorption, Rh, H, CO, C, ethylidyne, methylidyne, ethanol
in
Surface Science
volume
602
issue
18
pages
3057 - 3063
publisher
Elsevier
external identifiers
  • wos:000260550500018
  • scopus:52049099349
ISSN
0039-6028
DOI
10.1016/j.susc.2008.08.004
language
English
LU publication?
yes
id
7fa5692a-6e22-4e61-80dd-1708df931e07 (old id 1278941)
date added to LUP
2009-02-10 11:28:08
date last changed
2017-01-01 06:09:15
@article{7fa5692a-6e22-4e61-80dd-1708df931e07,
  abstract     = {We have investigated the adsorption and decomposition of ethanol on the Rh(111) and Rh(5 5 3) surfaces at room temperature with special emphasis on the dehydrogenation. We use high resolution Core level photoemission and density functional theory (DFT) based simulations. A detailed analysis of the C1s core level spectra, including analysis of the vibrational fine-structure and comparison to calculated C1s binding energy shifts, shows that the ethanol decomposes into CO, ethylidyne (C2H3) methylidyne (CH), atomic C, and hydrogen. At low ethanol exposures, CH is the dominating hydrocarbon fragment on Rh(111), whereas on Rh(553) atomic C dominates over CH, indicating an enhanced dehydrogenation due to the steps present on the latter surface. At higher ethanol exposures we find a similar behavior of atomic C dominating over hydrocarbons on Rh(553), while on Rh(111) atomic carbon remains a minority species. Our DFT based simulations show that the enhanced dehydrogenation results from a significant lowering of the CH dissociation barrier from Rh(111) to Rh(553), as well as from the dissociation changing from endothermic on Rh(111) to exothermic on Rh(553). (C) 2008 Elsevier B.V. All rights reserved.},
  author       = {Resta, Andrea and Gustafson, Johan and Westerström, Rasmus and Mikkelsen, Anders and Lundgren, Edvin and Andersen, Jesper N and Yang, Ming-Mei and Ma, Xiu-Fang and Bao, Xin-He and Li, Wei-Xue},
  issn         = {0039-6028},
  keyword      = {spectroscopy,synchrotron radiation photoelectron,photoelectron spectroscopy,Density functional calculations,soft X-ray,Photoelectron spectroscopy,Surface chemical reaction,Catalysis,Chemisorption,Rh,H,CO,C,ethylidyne,methylidyne,ethanol},
  language     = {eng},
  number       = {18},
  pages        = {3057--3063},
  publisher    = {Elsevier},
  series       = {Surface Science},
  title        = {Step enhanced dehydrogenation of ethanol on Rh},
  url          = {http://dx.doi.org/10.1016/j.susc.2008.08.004},
  volume       = {602},
  year         = {2008},
}