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

Autor: Matthew W. Small, John J. Rehr, Joshua J. Kas, Anatoly I. Frenkel, Kristina O. Kvashnina, Moniek Tromp, Ralph G. Nuzzo
Rok vydání: 2014
Předmět:
Zdroj: ChemPhysChem. 15:1569-1572
ISSN: 1439-4235
DOI: 10.1002/cphc.201400055
Popis: 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 H2) 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.
Databáze: OpenAIRE