Alkyne hydrogenation over Pd catalysts: A new paradigm

Detre Teschner, Elaine Vass, Michael Hävecker, Spiros Zafeiratos, Péter Schnörch, Hermann Sauer, Axel Knop-Gericke, Robert Schlögl, Mounir Chamam, Attila Wootsch, Arran S. Canning, Jonathan J. Gamman, S. David Jackson, James McGregor, Lynn F. Gladden

Research output: Contribution to journalArticle

199 Citations (Scopus)

Abstract

The hydrogenation of 1-pentyne over various palladium catalysts was studied under various conditions. In the regime of selective hydrogenation, as observed by in situ X-ray photoelectron spectroscopy, significant amounts of subsurface carbon and a Pd-C surface phase built up in the early stage of the reaction. These species inhibited the emergence of bulk-dissolved hydrogen to the surface, which is reactive but unselective. Carbon laydown was also observed by tapered element oscillating microbalance and by catalytic pulse experiments, with greater laydown occurring in the selective regime. The effect of carbon dissolution in the crystal lattice near the surface was evidenced by high-resolution transmission electron microscopy. In alkyne hydrogenation, the active phase of palladium catalysts is a Pd-C surface phase in the regime of selective hydrogenation. Because self-hydrogenation (hydrogen from dissociated pentyne) was also shown to be unselective, only surface hydrogen from the gas phase is available to generate the alkene. The issue of structure-sensitivity of alkyne hydrogenation over palladium catalysts is discussed in terms of structure-sensitive carbon deposition and carbon dissolution into the metal lattice.

Original languageEnglish
Pages (from-to)26-37
Number of pages12
JournalJournal of Catalysis
Volume242
Issue number1
DOIs
Publication statusPublished - Aug 15 2006

Keywords

  • 1-Pentyne
  • Carbon deposition
  • HRTEM
  • High-pressure XPS
  • Palladium
  • Selective hydrogenation
  • TEOM

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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  • Cite this

    Teschner, D., Vass, E., Hävecker, M., Zafeiratos, S., Schnörch, P., Sauer, H., Knop-Gericke, A., Schlögl, R., Chamam, M., Wootsch, A., Canning, A. S., Gamman, J. J., Jackson, S. D., McGregor, J., & Gladden, L. F. (2006). Alkyne hydrogenation over Pd catalysts: A new paradigm. Journal of Catalysis, 242(1), 26-37. https://doi.org/10.1016/j.jcat.2006.05.030