Comparison of Pd and Pd4S based catalysts for partial hydrogenation of external and internal butynes

Yanan Liu, Yinwen Li, James Anderson, Junting Feng, Antonio Guerrero-Ruiz, Inmaculada Rodríguez-Ramos, Alan J McCue* (Corresponding Author), Dianqing Li (Corresponding Author)

*Corresponding author for this work

Research output: Contribution to journalArticle

Abstract

The partial hydrogenation of but-1-yne and but-2-yne was studied with a view to probing the difference between external and internal alkynes. Catalysts with Pd and Pd4S active phases were prepared on a carbon nanofiber support. Over the simple Pd catalyst over-hydrogenation was common which restricted alkene selectivity greatly – 25–35% depending on temperature. In contrast, the Pd4S active phase offered exceptional alkene selectivity (maximum of 92–93% alkene selectivity for both the external and internal alkyne). DFT calculations were subsequently used to rationalise this difference in product selectivity – sulfur appears to change the geometry of the active site in Pd4S and create a surface which favours alkene desorption relative to over-hydrogenation. This work further emphases the potential of palladium sulfide phases as an alternative to purely metallic palladium catalysts for partial alkyne hydrogenation.
Original languageEnglish
Pages (from-to)51-59
Number of pages9
JournalJournal of Catalysis
Volume383
Early online date25 Jan 2020
DOIs
Publication statusPublished - Mar 2020

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Keywords

  • partial hydrogenation
  • palladium sulfide
  • metal sulfide
  • but-1-yne
  • but-2-yne
  • butene
  • GALLIUM INTERMETALLIC COMPOUNDS
  • ACETYLENE
  • PERFORMANCE
  • But-2-yne
  • 1-BUTYNE
  • ALKYNES
  • SELECTIVE HYDROGENATION
  • PROPYNE
  • PHASE HYDROGENATION
  • 1,3-BUTADIENE
  • Metal sulfide
  • Palladium sulfide
  • Partial hydrogenation
  • But-1-yne
  • Butene
  • PALLADIUM SULFIDE

Cite this

Liu, Y., Li, Y., Anderson, J., Feng, J., Guerrero-Ruiz, A., Rodríguez-Ramos, I., ... Li, D. (2020). Comparison of Pd and Pd4S based catalysts for partial hydrogenation of external and internal butynes. Journal of Catalysis, 383, 51-59. https://doi.org/10.1016/j.jcat.2020.01.010