Berlin 2018 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 104: Oxides and Insulators: Adsorption I
O 104.4: Vortrag
Donnerstag, 15. März 2018, 17:30–17:45, MA 041
Ab initio Cluster Calculations on the Adsorption and Electronic Excitation of SO2 on TiO2-Rutile(110) — •Luca Gerhards and Thorsten Klüner — Carl von Ossietzky Universität, Oldenburg, Germany
The production of sulfonic acids as precursors for several products such as detergents or pharmaceutical drugs is a vital process for today’s society. An efficient way to synthesize these compounds can be conducted by the sulfoxidation of alkenes. The photocatalytic heterogeneous sulfoxidation on titanium dioxides seems to be a promising new and more energy efficient alternative to the industrially applied homogeneous reaction. Experimental investigations on the mechanism revealed that the adsorption of SO2 and the excitation with visible light lead to a formation of a charge-transfer complex on the surface which seems to catalyze the subsequent chain reaction.[1] These results stand in contrast to the homogenous mechanism and need a deeper investigation. In this contribution, we examine the adsorption and electronic excitation of SO2 on the ideal TiO2-rutile(110) surface from a quantum chemical perspective. For this purpose, an embedded cluster model was constructed in order to faithfully describe the substrate-adsorbate interaction. Along these lines, post-HF and multireference methods like MP2 or CASSCF/NEVPT2 as implemented in the program package ORCA were used to calculate electronic excitations of the adsorbate.
[1] F. Parrino, A. Ramakrishnan, H. Kisch, Angew. Chem. Int. Ed., 47(37), p. 7107-7109, 2008.