Periodic DFT calculations were used to study the creation of Schottky defects on
MO2(110) rutile surface where M = Ti or Sn. These defects were oxygen
vacancies: a bridging oxygen atom was removed from the surface creating an F°S
center and re-adsorbed on a vicinal site. The re-adsorption permitted compensation
of a part of the energy cost required for the removal. Durng this process, the
stoichiometry and the atomic oxidation states remained those of the perfect surface. The energy cost for such a defect was found to be almost 5 times lower for
TiO2(110) than for SnO2(110). The effect of hydrogen co-adsorption was then
analyzed. The hydrogenated surface was considered to involve one hydrogen atom
binding to a bridging oxygen atom and reducing the metal-oxide surface. The
Schottky process then became the displacement of a hydroxyl ion which desorbed
and re-adsorbed on surface titanium just as the basic species did. This coadsorption
did not affect the energy cost in the case of TiO2 while, in the case of
SnO2(110), it made it weaker. This decrease was due mainly to the magnitude of
the interaction between a hydroxyl group and the Sn4+ surface atom, that was large
compared with that for O.
Comparative Creation of Surface Schottky Defects on SnO2(110) and TiO2(110).
A.Markovits, C.Minot: Journal of Physics - Conference Series, 2008, 117[1],
012021