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

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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

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

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