Document Type

Dissertation

Date of Degree

Fall 2016

Degree Name

PhD (Doctor of Philosophy)

Degree In

Civil and Environmental Engineering

First Advisor

David M. Cwiertny

Abstract

A range of chemical pollutants now contaminate drinking water sources and present a public health concern, including organic compounds, such as pharmaceuticals and pesticides, and both metalloids and heavy metals, such as arsenic and lead. Metalloids and heavy metals have been detected in private drinking water wells, which do not fall under federal drinking water regulations, as well as in urban tap water, due to the introduction of contamination to the drinking water distribution system. Further, many so-called “emerging organic contaminants,” which are present in drinking water sources at detectable levels but have unknown long-term health implications, do not fall under federal drinking water regulations. To protect the health of consumers, drinking water treatment at the point-of-use (POU) (i.e., the tap) is essential. Next-generation POU treatment technologies must require minimal energy inputs, be simple enough to permit broad application among different users, and be easily adaptable for removal of a wide range of pollutants.

Nanomaterials, such as carbon nanotubes and iron oxide nanoparticles, are ideal candidates for next-generation drinking water treatment, as they exhibit unique, high reactivity and necessitate small treatment units. However, concerns regarding water pressure requirements and nanomaterial release into the treated supply limit their application in traditional reactor designs. To bridge the gap between potential and practical application of nanomaterials, this study utilizes electrospinning to fabricate composite nanofiber filters that effectively deploy nanomaterials in drinking water treatment. In electrospinning, a high voltage draws a polymer precursor solution (which can contain nanomaterial additives, in the case of nanocomposites) from a needle to deposit a non-woven nanofiber filter on a collector surface.

Using electrospinning, we develop an optimized, macroporous carbon nanotube-carbon nanofiber composite that utilizes the sorption capacity of embedded carbon nanotubes, and achieves a key balance between material strength and reactivity towards organic pollutants. Additionally, via single-pot syntheses, we develop two optimized polymer-iron oxide composites for removal of heavy metal contamination by inclusion of iron oxide nanoparticles and either cationic or anionic surfactants in the electrospinning precursor solution. In hybrid materials that contain a well-retained quaternary ammonium surfactant (tetrabutylammonium bromide) and iron oxide nanoparticles, ion exchange sites and iron oxide sites are selective for chromate and arsenate removal, respectively. We demonstrated that a sulfonate surfactant, sodium dodecyl sulfate, acted as a removable porogen and an agent for surface segregation of iron oxide nanoparticles, thus enhancing composite performance for removal of lead, copper, and cadmium. Notably, nanoparticles embedded in composites exhibited comparable activity to freely dispersed nanoparticles. Collectively, the composites developed in this work represent a substantial advance towards the overlap of effective nanomaterial immobilization and utilization of nanomaterial reactivity. Outcomes of this work advance current knowledge of nanocomposite fabrication, and contribute to the responsible and effective deployment of nanomaterials in POU drinking water treatment.

Keywords

electrospinning, heavy metals, nanocomposite, organic micropollutants, point-of-use, water treatment

Pages

xxv, 287 pages

Bibliography

Includes bibliographical references (pages 261-287).

Copyright

Copyright © 2016 Katherine T. Peter

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