Adsorption and oxidation of sulfur dioxide on the yttria-stabilized zirconia surface: ab initio atomistic thermodynamics study

摘要

The interaction of SO_2 with the yttria-stabilized zirconia (YSZ) (111) and oxygen-enriched YSZ (111)(YSZ+O) surface is investigated using the first-principles method based density functional theory (DFT). It is found that SO_2 is adsorbed either as a molecule or forms SO_3~(2-) species with new S-O bonds to a surface oxygen on the YSZ (111) surface. In addition, there exist other species, e.g., SO_3 and SO_4~(2-) on the very active YSZ+O (111) surface. Using the ab initio atomistic thermodynamics method, we present a detailed analysis on the stability of the SO_2-YSZ/YSZ+O system as a function of the ambient conditions.