Selective Hydrogenation of Acetylene over Pd-Boron Catalysts: A Density Functional Theory Study

Bo Yang, Robbie Burch, Christopher Hardacre*, P. Hu, Philip Hughes

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

22 Citations (Scopus)

Abstract

Boron-modified Pd catalysts have shown excellent performance for the selective hydrogenation of alkynes experimentally. In the current work, we investigated the hydrogenation of acetylene on boron-modified Pd(111) and Pd(211) surfaces, utilizing density functional theory calculations. The activity of acetylene hydrogenation has been studied by estimating the effective barrier of the whole process. The selectivity of ethylene formation is investigated from a comparison between the desorption and the hydrogenation of ethylene as well as comparison between the ethylene and the 1,3-butadiene formation. Formation of subsurface carbon and hydrogen on both boron-modified Pd(111) and Pd(211) surfaces has also been evaluated, since these have been reported to affect both the activity and the selectivity of acetylene hydrogenation to produce ethylene on Pd surfaces. Our results provide some important insights into the Pd B catalysts for selective hydrogenation of acetylene and also for more complex hydrogenation systems, such as stereoselective hydrogenation of longer chain alkynes and selective hydrogenation of vegetable oil.

Original languageEnglish
Pages (from-to)3664-3671
Number of pages8
JournalThe Journal of Physical Chemistry C
Volume118
Issue number7
Early online date21 Jan 2014
DOIs
Publication statusPublished - 20 Feb 2014

Keywords

  • GALLIUM INTERMETALLIC COMPOUNDS
  • INITIO MOLECULAR-DYNAMICS
  • TOTAL-ENERGY CALCULATIONS
  • AUGMENTED-WAVE METHOD
  • ETHENE-RICH STREAMS
  • PALLADIUM CATALYSTS
  • SURFACE CHARACTERIZATION
  • HETEROGENEOUS CATALYSIS
  • PD-AG/AL2O3 CATALYSTS
  • ALKYNE HYDROGENATION

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

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