Date of Award

6-21-2012

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Applied Science

First Advisor

Alexandru. Biris

Abstract

As the worldwide demand for fossil-based fuel increases every day and the fossil reserve continues to be depleted, the need for alternative/renewable energy sources has gained momentum. Electric, hybrid, and hydrogen cars have been at the center of discussion lately among consumers, automobile manufacturers, and politicians, alike. The development of a fuel-cell based engine using hydrogen has been an ambitious research area over the last few decades-ever since Fujishima showed that hydrogen can be generated via the solar-energy driven photo-electrolytic splitting of water. Such solar cells are known as Photo-Electro-Chemical (PEC) solar cells. In order to commercialize this technology, various challenges associated with photo-conversion efficiency, chemical corrosion resistance, and longevity need to be overcome. In general, metal oxide semiconductors such as titanium dioxide (TiO2, titania) are excellent candidates for PEC solar cells. Titania nanotubes have several advantages, including biocompatibility and higher chemical stability. Nevertheless, they can absorb only 5-7% of the solar spectrum which makes it difficult to achieve the higher photo-conversion efficiency required for successful commercial applications. A two-prong approach was employed to enhance photo-conversion efficiency: 1) surface modification of titania nanotubes using plasma treatment and 2) nano-capping of the titania nanotubes using titanium disilicide. The plasma surface treatment with N2 was found to improve the photo-current efficiency of titania nanotubes by 55%. Similarly, a facile, novel approach of nano-capping titania nanotubes to enhance their photocurrent response was also investigated. Electrochemically anodized titania nanotubes were capped by coating a 25 nm layer of titanium disilicide using RF magnetron sputtering technique. The optical properties of titania nanotubes were not found to change due to the capping, however, a considerable increase (40%) in the photocurrent density was observed for the nano-capped titania nanotubes due to the enhanced charge transfer process. Similarly, another metal oxide semiconductor was investigated tungsten trioxide (WO3), which has a much higher absorption capability (12%) in the solar spectrum. The WO3 porous nanostructures suffered from surface corrosion resulting in a large reduction in the photocurrent density as a function of time in the alkaline electrolytes. However, with a protective coating of Indium Tin Oxide (100 nm), the surface corrosion of WO3 porous nanostructures was reduced. A large increase in the photocurrent density of as much as 340% was observed after the ITO was applied to the WO3 porous nanostructures

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