Document Type

Dissertation

Date of Degree

Summer 2013

Degree Name

PhD (Doctor of Philosophy)

Degree In

Civil and Environmental Engineering

First Advisor

David M. Cwiertny

Abstract

Increasing demand for limited fresh water resources necessitates that alternative water sources be developed. Nonpotable reuse of treated wastewater represents one such alternative. However, the ubiquitous presence of organic micropollutants such as pharmaceuticals and personal care products (PPCPs) in wastewater effluents limits use of this resource. Numerous investigations have examined PPCP fate during wastewater treatment, focusing on their removal during conventional and advanced treatment processes. Analysis of influent and effluent data from published studies reveals that at best 1-log10 concentration unit of PPCP removal can generally be achieved with conventional treatment. In contrast, plants employing advanced treatment methods, particularly ozonation and/or membranes, remove most PPCPs often to levels below analytical detection limits. However, membrane treatment is cost prohibitive for many facilities, and ozone treatment can be very selective. Ozone-recalcitrant compounds require the use of Advanced Oxidation Processes (AOPs), which utilize highly reactive hydroxyl radicals (*OH) to target resistant pollutants. Due to cost and energy use concerns associated with current AOPs, alternatives such as catalytic ozonation are under investigation. Catalytic ozonation uses substrates such as activated carbon to promote *OH formation during ozonation. Here, we show that multi-walled carbon nanotubes (MWCNTs) represent another viable substrate, promoting *OH formation during ozonation to levels exceeding activated carbon and equivalent to conventional ozone-based AOPs. Via a series of batch reactions, we observ a strong correlation between *OH formation and MWCNT surface oxygen concentrations. Results suggest that deprotonated carboxyl groups on the CNT surface are integral to their reactivity toward ozone and corresponding *OH formation. From a practical standpoint, we show that industrial grade MWCNTs exhibit similar *OH production as their research-grade counterparts. Accelerated aging studies indicate that MWCNTs maintain surface reactivity for an extended period during ozonation treatment. Further, *OH generation is essentially unaffected in complex water matrices containing known radical scavengers, and is effective for degradation of the ozone-recalcitrant herbicide atrazine. A proof-of-concept study verified that results from batch systems can be replicated in a flow-through reactor utilizing MWCNTs immobilized on a ceramic membrane support. Collective, results suggest that CNT-enhanced ozonation may provide a viable treatment alternative for emerging organic micropollutants.

Pages

xi, 219 pages

Bibliography

Includes bibliographical references (pages 191-219).

Comments

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Copyright

Copyright 2013 Rebekah Lynn Oulton

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