Evidence To Challenge the Universality of the Horiuti-Polanyi Mechanism for Hydrogenation in Heterogeneous Catalysis: Origin and Trend of the Preference of a Non-Horiuti-Polanyi Mechanism

Bo Yang, Xue-Qing Gong, Hai-Feng Wang, Xiao-Ming Cao*, John J. Rooney, P. Hu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

72 Citations (Scopus)

Abstract

The Horiuti-Polanyi mechanism has been considered to be universal for explaining the mechanisms of hydrogenation reactions in heterogeneous catalysis for several decades. In this work, we examine this mechanism for the hydrogenation of acrolein, the simplest alpha,beta-unsaturated aldehyde, in gold-based systems as well as some other metals using extensive first-principles calculations. It is found that a non-Horiuti-Polanyi mechanism is favored in some cases. Furthermore, the physical origin and trend of this mechanism are revealed and discussed regarding the geometrical and electronic effects, which will have a significant influence on current understandings on heterogeneous catalytic hydrogenation reactions and the future catalyst design for these reactions.

Original languageEnglish
Pages (from-to)15244-15250
Number of pages7
JournalJournal of the American Chemical Society
Volume135
Issue number40
DOIs
Publication statusPublished - 09 Oct 2013

Keywords

  • DENSITY-FUNCTIONAL THEORY
  • TRANSITION-METAL SURFACES
  • INITIO MOLECULAR-DYNAMICS
  • AUGMENTED-WAVE METHOD
  • ETHENE-RICH STREAMS
  • SELECTIVE HYDROGENATION
  • ALPHA,BETA-UNSATURATED ALDEHYDES
  • CO OXIDATION
  • PALLADIUM CATALYSTS
  • PERIMETER SITES

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