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Title: Stability of surface and subsurface hydrogen on and in Au/Ni near-surface alloys

Periodic, self-consistent DFT-GGA (PW91) calculations were used to study the interaction of hydrogen atoms with the (111) surfaces of substitutional near-surface alloys (NSAs) of Au and Ni with different surface layer compositions and different arrangements of Au atoms in the surface layer. The effect of hydrogen adsorption on the surface and in the first and second subsurface layers of the NSAs was studied. Increasing the Au content in the surface layer weakens hydrogen binding on the surface, but strengthens subsurface binding, suggesting that the distribution of surface and subsurface hydrogen will be different than that on pure Ni(111). While the metal composition of the surface layer has an effect on the binding energy of hydrogen on NSA surfaces, the local composition of the binding site has a stronger effect. For example, fcc hollow sites consisting of three Ni atoms bind H nearly as strongly as on Ni(111), and fcc sites consisting of three Au atoms bind H nearly as weakly as on Au(111). Sites with one or two Au atoms show intermediate binding energies. The preference of hydrogen for three-fold Ni hollow sites alters the relative stabilities of different surface metal atom arrangements, and may provide a driving force formore » adsorbate-induced surface rearrangement.« less
 [1] ;  [1]
  1. Univ. of Wisconsin, Madison, WI (United States)
Publication Date:
Grant/Contract Number:
FG02-05ER15731; AC02-06CH11357; AC02-05CH11231
Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 640; Journal Issue: C; Journal ID: ISSN 0039-6028
Research Org:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Contributing Orgs:
EMSL, a National scientific user facility at Pacific Northwest National Laboratory (PNNL); the Center for Nanoscale Materials at Argonne National Laboratory (ANL); and the National Energy Research Scientific Computing Center (NERSC)
Country of Publication:
United States
36 MATERIALS SCIENCE; DFT; Near-surface alloys; Hydrogen; Gold; Nickel; Subsurface absorption
OSTI Identifier:
Alternate Identifier(s):
OSTI ID: 1244733