Date of Award

1-1-2013

Language

English

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

College/School/Department

Department of Nanoscale Science and Engineering

Program

Nanoscale Engineering

Content Description

1 online resource (x, 166 pages) : illustrations (some color)

Dissertation/Thesis Chair

Michael Carpenter

Keywords

Harsh Environment, Nanoparticles, Plasmonic, Sensing, Plasmons (Physics), High temperatures, Detectors, Surface plasmon resonance, Thin films

Subject Categories

Nanoscience and Nanotechnology

Abstract

Thin metal oxide films embedded with Au nanoparticles (AuNPs) have been investigated as high temperature localized surface plasmon resonance (LSPR) based sensing materials to monitor H2, CO, and NO2 at a temperature of 500°C. Applications for this technology include turbine engines as well as other combustion environments where it is important to monitor emission gases for both regulatory purposes as well as combustion control. These high temperature applications, which may be oxidizing or reducing in nature, present challenges to sensor reliability and selectivity, and have therefore necessitated the development of novel sensing devices. While there has been work on developing semiconductor-based electrical sensing methods, this work examines the optical response of AuNPs in yttria-stabilized zirconia (YSZ), TiO2, and CeO2. The main challenge with this technique is to achieve a selective response to the target gases. As a means of addressing this issue, both materials and data analysis techniques have been investigated. From the materials aspect, a sensor array was developed for a direct comparison of Au-YSZ, Au-TiO2, and Au-CeO2. In order to analyze the data, the multivariate method of principle component analysis was applied. The result of this analysis showed that a unique response was seen for each of the three target gases during separate exposures, which is an initial step towards selective detection in a gas mixture. Additional material control has also been achieved with the use of electron beam lithography to pattern Au nanoparticles for size and shape control. A particular emphasis has been placed on the nanorod geometry due to its tunable longitudinal LSPR peak; however, thermal stability of this geometry has been a challenge. Encapsulating the Au nanorods with YSZ was shown to help stabilize the nanorods for sensing tests performed at 500°C. Apart from material control, a kinetics analysis has also been performed for H2 reactions with Au-YSZ in an oxygen deprived environment. While this type of environment may not be directly applicable to current sensing needs, it demonstrates the ability of these films to monitor reaction rates in order to develop an understanding of the reaction mechanism.

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