Dissertation/Thesis Abstract

Monitoring and Removal of Water Contaminants of Emerging Concern: Development of A Multi-Walled Carbon Nanotube Based-Biosensor and Highly Tailor-Designed Titanium Dioxide Photocatalysts
by Han, Changseok, Ph.D., University of Cincinnati, 2014, 188; 3622058
Abstract (Summary)

In this dissertation, as a monitoring technology for cyanotoxins, a multiwalled carbon nanotube (MWCNT)-based electrochemical biosensor was developed to determine microcystin-LR (MC-LR), a potent cyanobacterial toxin, in sources of drinking water supplies. The performance of the MWCNT array biosensor is evaluated using micro-Raman spectroscopy, X-ray photoelectron spectroscopy, cyclic voltammetry, optical microscopy, and Faradaic electrochemical impedance spectroscopy. A linear dependence of the electron-transfer resistance on the MC-LR concentration is observed in the range of 0.05 to 20 µg L-1, which enables cyanotoxin monitoring well below the World Health Organization provisional concentration limit of 1 µg L-1 for MC-LR in drinking water.

In addition to the development of monitoring tools for cyanotoxins, visible light-activated (VLA) TiO2 and monodisperse TiO2 were developed and evaluated for treatment of water contaminants of emerging concern. These materials were synthesized using modified sol-gel methods (i.e., wet chemistry-based methods) such as self-assembly-based and ionic strength-assisted techniques. For this study, first, VLA-sulfur-doped TiO2 (S-TiO 2) nanocrystalline films were synthesized by a self-assembly-based sol-gel method using nonionic surfactant to control nanostructure and an inorganic sulfur source for decomposing MC-LR under visible light illumination. Second, the effects of solvent on the synthesis of VLA-S-TiO2 films were scrutinized. Four different polar, protic solvents, isopropanol, 1-butanol, ethanol, and methanol, were chosen as the solvent in four titania sol-gel preparations. Third, monodisperse anatase titania nanoparticles with controllable sizes (typically 10-300 nm) were synthesized using an efficient and straightforward protocol via fine tuning of the ionic strength in the devised sol-gel methodology. Finally, noble metal Ag-decorated, monodisperse TiO2 (TiO 2-Ag) aggregates were successfully synthesized by an ionic strength-assisted, simple sol-gel method and were used for the photocatalytic degradation of the pharmaceutical oxytetracycline (OTC) under both UV and visible light irradiation. With a self-assembly-based sol-gel method, nanostructured anatase S-TiO 2 with high surface area (> 100 m2 g-1) and porosity (> 30 %) was synthesized and the sample calcined at 350 oC demonstrated the highest visible light absorption and visible light-induced photocatalytic activity in the decomposition of MC-LR. The structural and morphological properties of S-TiO2 could be also tailor-designed using different solvents in the sol-gel synthesis, while inducing negligible effects on the sulfur doping and the visible light activation of TiO 2. Thus, it can be concluded that the enhancement of photocatalytic activity of S-TiO2 films can be achieved by judicious choice of the main solvent for the sol-gel method. With an ionic strength-assisted sol-gel method, monodisperse spherical anatase TiO2 (10-300 nm in diameter) as well as monodisperse TiO2-Ag aggregates with 350 nm of diameter were synthesized. For TiO2-Ag, its visible light absorption increased due to the presence of Ag on the surface of monodisperse TiO2, which resulted in the enhancement of the photocatalytic degradation of OTC under both UV-visible light and visible light irradiation compared to pure TiO2. There was an optimal Ag content to obtain the highest photocatalytic degradation of OTC. These newly developed materials demonstrated the efficient decomposition of water contaminants of emerging concern, especially MC-LR and OTC, under UV-visible light and visible light illumination.

Indexing (document details)
Advisor: Dionysiou, Dionysios
Commitee: Kupferle, Margaret, Nadagouda, Mallikarjuna, Sorial, George
School: University of Cincinnati
Department: Environmental Engineering
School Location: United States -- Ohio
Source: DAI-B 75/09(E), Dissertation Abstracts International
Subjects: Nanotechnology, Environmental engineering
Keywords: Advanced oxidation process, Biosensors, Carbon nanotubes, Cyanotoxins, Emerging contaminants, Titanium dioxide, Visible light activation
Publication Number: 3622058
ISBN: 978-1-303-93638-8
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