Ethanol Steam Reforming on Rh Catalysts: Theoretical and Experimental Understanding

Jia Zhang*, Ziyi Zhong, X. -M. Cao, P. Hu, Michael B. Sullivan, Luwei Chen

*Corresponding author for this work

Research output: Contribution to journalArticle

30 Citations (Scopus)

Abstract

Through combined theoretical and experimental efforts, the reaction mechanism of ethanol steam reforming on Rh catalysts was studied. The results suggest that acetaldehyde (CH3CHO) is an important reaction intermediate in the reaction on nanosized Rh catalyst. Our theoretical work suggests that the H-bond effect significantly modifies the ethanol decomposition pathway. The possible reaction pathway on Rh (211) surface is suggested as CH3CH2OH -> CH3CH2O -> CH3CHO -> CH3CO -> CH3 + CO -> CH2 + CO -> CH + CO -> C + CO, followed by the water gas shift reaction to yield H-2 and CO2. In addition, we found that the water-gas shift reaction, not the ethanol decomposition, is the bottleneck for the overall ethanol steam reforming process. The CO + OH association is considered the key step, with a sizable energy barrier of 1.31 eV. The present work first discusses the mechanisms and the water effect in ethanol steam reforming reactions on Rh catalyst from both theoretical and experimental standpoints, which may shed light on designing improved catalysts.
Original languageEnglish
Pages (from-to)448-456
Number of pages9
JournalACS Catalysis
Volume4
Issue number2
Early online date17 Dec 2013
DOIs
Publication statusPublished - Feb 2014

Keywords

  • ethanol steam reforming
  • Rh catalyst
  • reaction mechanism
  • DFT calculations
  • real-time GC/MS analysis
  • DENSITY-FUNCTIONAL THEORY
  • GAS SHIFT REACTION
  • INITIO MOLECULAR-DYNAMICS
  • HYDROGEN-PRODUCTION
  • LOW-TEMPERATURE
  • H-2 PRODUCTION
  • RH/CEO2-ZRO2 CATALYSTS
  • REACTION-MECHANISM
  • CO OXIDATION
  • FUEL-CELL

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