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Chemisorption studies of CH{sub 3}S on Ni(111)

Journal Article · · Journal of the American Chemical Society
; ;  [1];  [2]
  1. North Carolina State Univ., Raleigh, NC (United States)
  2. Oak Ridge National Lab., TN (United States)

The chemisorption of methanethiolate on Ni(111) is treated using a many-electron embedding theory, modeling the lattice as a 28-atom, three-layer cluster with the Ni atoms fixed at the positions from the bulk. Methanethiolate binds strongly to the Ni(111) surface at both high and low symmetry sites. Calculated adsorption energies are 61 kcal/mol for an equilibrium sulfur-surface distance of 1.99 A at three-fold sites, 61 kcal/mol with a sulfur-surface distance of 2.06 A at bridge sites, and 57 kcal/mol with a sulfur-surface distance of 2.13 A at atop sites. Different equilibrium geometries are predicted for CH{sub 3}S at three-fold, bridge, and atop sites. The methanethiolate C-S axis is nearly perpendicular to the surface, inclined only about 5{degree} from the surface normal, at the three-fold site. The C-S axis is found to be tilted away from the surface normal by 45{degree} at the bridge site, and by 55{degree} at the atop site. For the C-S axis perpendicular to the surface, the calculated C-S stretching vibration is 730 cm{sup -1}, and the CH{sub 3}S-surface stretch is 281 cm{sup -1} at the three-fold site. For a 45{degree} tilt at the bridge site and a 55{degree} tilt at the atop site, the C-S stretching vibrations are 677 and 698 cm{sup -1}, respectively. 63 refs., 5 figs., 3 tabs.

Sponsoring Organization:
USDOE
OSTI ID:
102777
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 18 Vol. 116; ISSN JACSAT; ISSN 0002-7863
Country of Publication:
United States
Language:
English