Effects of Adsorbate Coverage and Bond-Length Disorder on the d-Band Center of Carbon-Supported Pt Catalysts

Matthew W. Small, Joshua J. Kas, Kristina O. Kvashnina, John J. Rehr*, Ralph G. Nuzzo, Moniek Tromp, Anatoly I. Frenkel

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

14 Citations (Scopus)

Abstract

Determination of the factors that affect the d-band center of catalysts is required to explain their catalytic properties. Resonant inelastic X-ray scattering (RIXS) enables direct imaging of electronic transitions in the d-band of Pt catalysts in real time and in realistic environmental conditions. Through a combination of in situ, temperature-resolved RIXS measurements and theoretical simulations we isolated and quantified the effects of bond-length disorder and adsorbate coverage (CO and H-2) on the d-band center of 1.25 nm size Pt catalysts supported on carbon. We found that the decrease in adsorbate coverage at elevated temperatures is responsible for the d band shifts towards higher energies relative to the Fermi level, whereas the effect of the increase in bond-length disorder on the d-band center is negligible. Although these results were obtained for a specific case of non-interacting support and weak temperature dependence of the metal-metal bond length in a model catalyst, this work can be extended to a broad range of real catalysts.

Original languageEnglish
Pages (from-to)1569-1572
Number of pages4
JournalChemphyschem
Volume15
Issue number8
DOIs
Publication statusPublished - 6-Jun-2014
Externally publishedYes

Keywords

  • catalysis
  • nanoparticles
  • platinum
  • resonant inelastic X-ray scattering
  • X-ray absorption spectroscopy
  • METAL-SURFACES
  • ELECTRONIC-STRUCTURE
  • OXYGEN REDUCTION
  • CO
  • REACTIVITY
  • ADSORPTION
  • STRAIN
  • EXAFS

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