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Structure and Dynamics of Applied Nanomaterials
Effects of Adsorbate Coverage and Bond Length Disorder on the d-Band Center in Carbon-Supported Pt Catalysts
Determination of the factors affecting the d-band center in catalysts is required for explaining 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 in 1.25 nm size Pt catalysts supported on carbon. We obtained that the decrease in adsorbate coverage at elevated temperatures is responsible for the d-band shifts towards the higher energies relative to the Fermi level while 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
M. W. Small, J. Kas, K. O. Kvashnina, J. J. Rehr, R. G. Nuzzo, M. Tromp, A. I. Frenkel
Effects of adsorbate coverage and bond length disorder on the d-band center in carbon-supported Pt catalysts
Chem. Phys. Chem. 15, 1569-1572 (2014)
