Initial Incorporation of Sulfur into the Pd(111) Surface: A Theoretical Study

Journal Article · Sun Oct 01 00:00:00 EDT 2006 · Surface Science

DOI:https://doi.org/10.1016/j.susc.2006.07.032· OSTI ID:910904

Alfonso, D R

Density functional theory is used to investigate the initial inclusion of sulfur into the subsurface interstitial sites of Pd(111) surface. Pure subsurface adsorption is found to be less energetically favorable than on-surface adsorption. The incorporation of sulfur into the metal becomes more favorable than continuous adsorption on the surface after a critical on-surface sulfur coverage. We find subsurface sulfur occupation to be energetically favorable after adsorption of more than half a monolayer on the surface. Occupation of subsurface sites induces a pronounced structural distortion of the Pd(111) surface. We find significant expansion of interplanar spacing between the uppermost surface metal layers and rearrangement of the S overlayer. The interplay between the energy cost due to structural distortion of Pd(111) and the energy gain due to bond formation for different structures is discussed.

• Research Organization: National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)
• Sponsoring Organization: USDOE - Office of Fossil Energy (FE)
• DOE Contract Number: None cited
• OSTI ID: 910904
• Report Number(s): DOE/NETL-IR-2007-009; TRN: US200802%%280
• Journal Information: Surface Science, Vol. 600, Issue 19; ISSN 0039-6028
• Publisher: Elsevier Science, Amsterdam, The Netherlands
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
ADSORPTION
ENERGY ACCOUNTING
FUNCTIONALS
INTERSTITIALS
OCCUPATIONS
SULFUR
chemisorption
density functional theory calculations
sulfur
metallic surfaces
adatoms
low index single crystal surfaces