Dehydrogenation of ethanol on an O2-4Rh/CeO2-x(1 1 1) surface: A computational study

Han Jung Li, Hui Lung Chen, Shih Feng Peng, Jia Jen Ho

Research output: Contribution to journalArticle

7 Citations (Scopus)

Abstract

We applied the periodic density-functional theory to investigate the dehydrogenation of ethanol on the O2-4Rh/CeO2-x(1 1 1) surface with an assumption that one defect site of that CeO2 surface creates an O vacancy that an excess O2 molecule replaces. Under these conditions, the adsorption energy of ethanol is calculated to be -16.08 kcal/mol. Before formation of a five-membered ring of an oxametallacyclic compound, the hydrogen atom of O-H and that of one β-carbon hydrogen of ethanol are eliminated. The dehydrogenation continues with the loss of two hydrogens from the α-carbon, at the same time, transforming to a four-membered ring species (Rh-CH2C(O)-Rh). Scission of the C-C bond occurs at this stage with a dissociation barrier 14.38 kcal/mol, forming adsorbed products CO and CH2. The ensuing steam-reforming process (CH2 + H2O) and the mechanism of the consecutive dehydrogenation are also discussed.

Original languageEnglish
Pages (from-to)141-150
Number of pages10
JournalChemical Physics
Volume359
Issue number1-3
DOIs
Publication statusPublished - 2009 May 18

Fingerprint

Dehydrogenation
dehydrogenation
Hydrogen
ethyl alcohol
Ethanol
Carbon
carbon
rings
Steam reforming
hydrogen
Carbon Monoxide
steam
Vacancies
Density functional theory
cleavage
hydrogen atoms
dissociation
density functional theory
Adsorption
Atoms

Keywords

  • 4Rh/CeO surface
  • Dehydrogenation mechanism
  • Density-functional theory calculation
  • Ethanol
  • Potential-energy surface

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Dehydrogenation of ethanol on an O2-4Rh/CeO2-x(1 1 1) surface : A computational study. / Li, Han Jung; Chen, Hui Lung; Peng, Shih Feng; Ho, Jia Jen.

In: Chemical Physics, Vol. 359, No. 1-3, 18.05.2009, p. 141-150.

Research output: Contribution to journalArticle

Li, Han Jung ; Chen, Hui Lung ; Peng, Shih Feng ; Ho, Jia Jen. / Dehydrogenation of ethanol on an O2-4Rh/CeO2-x(1 1 1) surface : A computational study. In: Chemical Physics. 2009 ; Vol. 359, No. 1-3. pp. 141-150.
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