Authors

Lizhou Nie

Type

Text

Type

Thesis

Advisor

White, Michael G | Rodriguez, José | Jia, Jiangyong.

Date

2013-12-01

Keywords

Physical chemistry

Department

Department of Chemistry.

Language

en_US

Source

This work is sponsored by the Stony Brook University Graduate School in compliance with the requirements for completion of degree.

Identifier

http://hdl.handle.net/11401/77139

Publisher

The Graduate School, Stony Brook University: Stony Brook, NY.

Format

application/pdf

Abstract

In order to improve performance of heterogeneous catalysts used in industrially important processes, it is of critical importance to understand the interfacial electronic properties of adsorbates on solid surfaces. Among various important electronic properties, interfacial charge transfer between the active catalyst and its supporting material can be correlated with the chemical activity of the catalyst for certain reactions. The work presented in this thesis, focuses on the charge transfer and surface dipole study at the interface of metal oxide/sulfide clusters deposited on Cu(111) and metal oxide clusters deposited on a Cu2O/Cu(111) film, studied using two-photon photoemission (2PPE) spectroscopy and other surface analysis techniques. These materials represent models for nanocatalysts for alternative fuel production (hydrogen, methanol) through the water-gas-shift reaction and CO2 hydrogenation. Size-selected metal oxide clusters (Mo3O9, W3O9, Ti3O6, Mo3O6, W3O6 and Ti5O10) and metal sulfide cluster (Mo4S6) have been selectively deposited on Cu(111) surface or a Cu2O/Cu(111) film, using a size-selection cluster deposition apparatus. Cluster distribution on the substrate was monitored with Auger electron spectroscopy (AES), and follows a Gaussian distribution within the different cluster-substrate systems. The work function shift due to cluster deposition was measured with 2PPE spectroscopy, which showed a consistent trend of work function increase for all the cluster-substrate systems here. In addition, surface dipoles are derived from work function shift measurement using the Topping model, which provides a method to study the interfacial charge transfer orientation and magnitude. These results suggest strong cluster-substrate interactions that result in interfacial charge transfer that is highly cluster and substrate dependent. | 60 pages

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