Date on Master's Thesis/Doctoral Dissertation

5-2017

Document Type

Doctoral Dissertation

Degree Name

Ph. D.

Department

Chemical Engineering

Degree Program

Chemical Engineering, PhD

Committee Chair

Fu, Xiao-an

Committee Co-Chair (if applicable)

Nantz, Michael

Committee Member

Nantz, Michael

Committee Member

Watters, James

Committee Member

Willing, Gerold

Committee Member

Sumanasekera, Gamini

Abstract

Exhaled breath is a complex mixture containing numerous volatile organic compounds (VOCs) at trace levels (ppb to ppt) including hydrocarbons, alcohols, ketones, aldehydes, esters and other non-volatile compounds. Different patterns of VOCs have been correlated with various diseases. The concentration levels of VOCs in exhaled breath depend on an individual subject’s health status. Therefore, breath analysis has great potential for clinical diagnostics, monitoring therapeutic progress and drug metabolic products. Even though up to 3000 compounds may be detected in breath, the matrix of exhaled breath is less complex than that of blood or other body fluids. Breath analysis can be performed on people irrespective of age, gender, lifestyle, or other confounding factors. Breath gas concentration can be related to VOC concentrations in blood via mathematical modeling; for example, as in blood alcohol testing. Since exhaled breath samples are easy to collect and online instruments are commercially available, VOC analysis in exhaled breath appears to be a promising tool for noninvasive detection and monitoring of diseases. Breath analysis has been very successful in identifying cancer, diabetes and other diseases by using a chemiresistor sensor array to detect biomarkers. The objective of this research project is to develop sensor arrays ― or so-called electronic nose ― for analysis of VOCs in air and exhaled breath. In this dissertation, we have investigated both commercial and synthesized thiol functionalized gold nanoparticles (AuNPs) as sensing materials for analysis of VOCs in air and exhaled breath. The advantages of these sensors include very high sensitivity, selectivity for detection of target analytes and operation at ambient temperature. The synthesis and material characterization of new thiols and AuNPs for increasing sensitivity and selectivity have been studied. Selected commercial thiols and in-house synthesized new functional thiols have been used to modify AuNP-based sensors for detection of VOCs in air and exhaled breath. The interdigitated electrodes (IDE) used for the sensors were fabricated by microelectromechanical systems (MEMS) microfabrication technologies. The sensor arrays were characterized by measuring the resistance difference from vacuum and different spiked analyte concentrations in air and breath samples. Air samples and breath samples were collected using Tedlar bags, and analyzed using the thiol functionalized AuNP sensors. The analysis of air samples provides a reference for analysis of exhaled breath samples. The sensors have demonstrated a low detection limit of 0.1 ppbv of acetone and ethanol in dry air and exhaled breath. The concentrations of acetone in air and exhaled breath were determined by a silicon microreactor approach. The measurements of acetone by the microreactor approach were correlated with the sensor signals. The intellectual thrust of this research is the rational design of an electronic nose for analysis of VOCs in exhaled breath, which offers a new frontier in medical diagnostics because of its non-invasive and inexpensive characteristics.

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