Authors

Shen Zhao

Type

Text

Type

Dissertation

Advisor

Kim, Taejin | Orlov, Alexander | Su, Dong. | Clayton, Clive

Date

2013-12-01

Keywords

Energy, Environmental, Heterogeneous catalysis, Photocatalysis, precious metals, titanium dioxide | Materials Science

Department

Department of Materials Science and Engineering.

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/11401/76372

Publisher

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

Format

application/pdf

Abstract

Semiconductor photocatalysis is a dynamic field at the forefront of environmental and energy research. This dissertation has focused on the development of novel nanomaterials to exceed performance for environmental and energy related applications in both liquid and gas phases as compared to traditional materials. This project investigated the impact of size of noble metal clusters on photocatalytic activity induced by UV and visible light. Compared to larger particles, sub-nanometer particles have shown much better activity for catalytic reactions in both liquid and gas phases. These nanoclusters supported on various semiconductors, such as TiO2 and CdS showed outstanding catalytic properties for oxidation of phenol in gas phase, removal of NO2 from gas phase via both oxidation and reduction routes and hydrogen production from water. The catalytic activities of sub-nanometer particles were much higher than those of known commercially available catalysts. Overall, this project has provided the first ever demonstration of the unique properties of ultra-small nanoparticles in sub-nanometer range for photocatalytic applications. Additionally, this project has focused on utilization of novel nanostructures to provide a high surface area support for photocatalysts and to achieve better dispersion of nanoparticles. More specifically, this research has focused on a new generation of highly ordered mesoporous SBA-15 sieves, which have large pore diameter (22 nm) and short pore length (500 nm), which were subsequently templated to facilitate photo-oxidation reactions. In addition, this project has focused on inverse opal structures to facilitate a better light capture inside these 3D structures, which can potentially lead to enhancement of photocatalytic reactions. All catalysts and catalysts' precursors were characterized using high resolution electron microscopy (HR-EM), which included Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM) and Scanning Transmission Electron Microscopy (STEM); Matrix assisted laser desorption ionization/time of flight (MALDI-TOF), X-ray diffraction (XRD), Scanning Tunneling microscopy (STM); while catalytic activity was determined by diffuse reflectance infrared Fourier Transform Spectroscopy (DRIFTS), High Performance Liquid Chromatography (HPLC) and Gas Chromatography (GC). | 183 pages

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