Theoretical analysis of hydrogen chemisorption on Pd(111), Re(0001) and PdML/Re(0001), ReML/Pd(111) pseudomorphic overlayers

Venkataraman Pallassana, Matthew Neurock, Lars Bruno Hansen, Bjørk Hammer, Jens Kehlet Nørskov

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Abstract

Gradient-corrected density-functional theory (DFT-GGA) periodic slab calculations have been used to analyze the binding of atomic hydrogen on monometallic Pd(111), Re(0001), and bimetallic Pd-mL/Re(0001) [pseudomorphic monolayer of Pd(111) on Re(0001)] and Re-ML/Pd(111) surfaces. The computed binding energies of atomic hydrogen adsorbed in the fee hollow site, at 100% surface coverage, on the Pd(111), Re(0001), Pd-ML/Re(0001), and Re-ML/Pd(111) surfaces, are -2.66, -2.82, -2.25, and -2.78 eV, respectively. Formal chemisorption theory was used to correlate the predicted binding energy with the location of the d-band center of the bare metal surfaces, using a model developed by Hammer and N phi rskov. The DFT-computed adsorption energies were also analyzed on the basis of the density of states (DOS) at the Fermi level for the clean metal surfaces. The results indicate a clear correlation between the d-band center of the surface metal atoms and the hydrogen chemisorption energy. The further the d-band center is from the Fermi level, the weaker is the chemisorption bond of atomic hydrogen on the surface. Although the DOS at the Fermi level may be related to the location of the d-band, it does not appear to provide an independent parameter for assessing surface reactivity. The weak chemisorption of hydrogen on the Pd-ML/Re(0001) surface relates to substantial lowering of the d-band center of Pd, when it is pseudomorphically deposited as a monolayer on a Re substrate. [S0163-1829(99)00331-2].
Original languageEnglish
JournalPhysical Review B
Volume60
Issue number8
Pages (from-to)6146-6154
ISSN2469-9950
DOIs
Publication statusPublished - 1999

Bibliographical note

Copyright (1999) by the American Physical Society.

Keywords

  • ELECTRONIC-STRUCTURE
  • METAL-SURFACES
  • TOTAL-ENERGY CALCULATIONS
  • DENSITY-FUNCTIONAL METHOD
  • DISSOCIATIVE ADSORPTION
  • PALLADIUM
  • H-2
  • REACTIVITY
  • WORK FUNCTION
  • BIMETALLIC SURFACES

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