Date of Award

1-1-2012

Document Type

Campus Access Dissertation

Department

Chemistry and Biochemistry

Sub-Department

Chemistry

First Advisor

Donna A Chen

Abstract

It is essential to understand the growth, composition, and activity of catalysts on a fundamental atomic level in order to guide the development of future catalysts with higher product yield and selectivity. TiO2 supported bimetallic Pt-Au and Ni-Au clusters were studied as model catalysts for low temperature oxidation reactions. The properties of these model catalysts were investigated with scanning tunneling microscopy (STM), low energy ion scattering (LEIS), X-ray photoelectron spectroscopy (XPS), and temperature programmed desorption (TPD). The importance of the Au-titania interface for low temperature oxidation was illustrated by a series of experiments that show a correlation between the number of Au-titania interfacial sites and the activity on the surface. Bimetallic clusters were grown by first depositing Ni or Pt onto the surface in order to seed the more mobile Au at existing Ni or Pt clusters. The surfaces of the bimetallic clusters are significantly enriched in Au and are almost entirely pure Au for clusters with > 50% bulk Au composition. The presence of adsorbates, such as methanol and CO, are able to induce the diffusion of Ni and Pt to the surface of the clusters. Currently the supported model catalysts are being characterized under more industrially relevant conditions of an atmosphere of gas in a novel recirculating catalytic reactor that is coupled to an ultrahigh vacuum (UHV) chamber. The study of these model systems has provided valuable insight into their growth, composition, and chemical activity.

Rights

© 2012, Samuel Adam Tenney

Download

Share

COinS