Partial oxidation of ethanol on vanadia catalysts on supporting oxides with different redox properties compared to propane

نویسندگان

  • Benjamin Beck
  • Manuel Harth
  • Neil G. Hamilton
  • Carlos Carrero
  • John J. Uhlrich
  • Annette Trunschke
  • Shamil Shaikhutdinov
  • Helmut Schubert
  • Hans-Joachim Freund
  • Robert Schlögl
  • Joachim Sauer
  • Reinhard Schomäcker
چکیده

The influence of the support material of vanadia catalysts on the reaction rate, activation energies, and defect formation enthalpies was investigated for the oxidative dehydrogenation of ethanol and propane. Characterization by infrared absorption–reflection spectroscopy (IRAS), Raman and UV–vis spectroscopy verifies a high dispersion of vanadia for powder and thin-film model catalysts. The support effect of ceria, alumina, titania, and zirconia is reflected in activation energy, oxidative dehydrogenation (ODH) rate, and temperature-programmed reductions (TPR) for both catalyst systems, ethanol and propane. Impendence spectroscopy and density functional theory (DFT) calculations were used to determine the defect formation enthalpy of the vanadyl oxygen double bond, providing the scaling parameter for a Bell– Evans–Polanyi relationship. On the basis of a Mars–van-Krevelen mechanism, an energy profile for the oxidative dehydrogenation is proposed. 2012 Elsevier Inc. All rights reserved.

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تاریخ انتشار 2012