Ethylene hydrogenation on supported Ni, Pd and Pt nanoparticles: Catalyst activity, deactivation and the d-band model

Andrew S. Crampton, Marian D. Rötzer, Florian F. Schweinberger, Bokwon Yoon, Uzi Landman, Ueli Heiz

Research output: Contribution to journalArticlepeer-review

60 Scopus citations

Abstract

Ethylene hydrogenation catalyzed at 300 K by 1-1.5 nm nanoparticles of Ni, Pd and Pt supported on MgO(1 0 0) with a narrow size-distribution, as well as the deactivation under reaction conditions at 400 K, was investigated with pulsed molecular beam experiments. Ni nanoparticles deactivate readily at 300 K, whereas Pd particles deactivate only after pulsing at 400 K, and Pt particles were found to retain hydrogenation activity even after the 400 K heating step. The hydrogenation turnover frequency normalized to the number of particles exhibited the trend, Pt > Pd > Ni. The activity/deactivation was found to scale with the location of the particles' d-band centroid, εc, with respect to the Fermi energy of the respective metals calculated with density-functional theory. An εc closer to the Fermi level is indicative of a facile deactivation/low activity and an εc farther from the Fermi level is characteristic of higher activity/impeded deactivation. CO adsorption, probed with infrared reflection absorption spectroscopy was used to investigate the clusters before and after the reaction, and the spectral features correlated with the observed catalytic behavior.

Original languageEnglish
Pages (from-to)51-58
Number of pages8
JournalJournal of Catalysis
Volume333
DOIs
StatePublished - 1 Jan 2016
Externally publishedYes

Keywords

  • Ethylene de-/hydrogenation
  • Model catalysis
  • Nickel
  • Palladium
  • Platinum
  • d-band

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