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.
Dissertation
Development of nanomaterial-enabled advanced oxidation techniques for treatment of organic micropollutants
University of Iowa
Doctor of Philosophy (PhD), University of Iowa
Summer 2013
DOI: 10.17077/etd.0ojjh04t
Free to read and download, Open Access
Abstract
Details
- Title: Subtitle
- Development of nanomaterial-enabled advanced oxidation techniques for treatment of organic micropollutants
- Creators
- Rebekah Lynn Oulton - University of Iowa
- Contributors
- David M. Cwiertny (Advisor)Vicki Grassian (Committee Member)Sarah Larsen (Committee Member)Tim Mattes (Committee Member)Richard Valentine (Committee Member)
- Resource Type
- Dissertation
- Degree Awarded
- Doctor of Philosophy (PhD), University of Iowa
- Degree in
- Civil and Environmental Engineering
- Date degree season
- Summer 2013
- Publisher
- University of Iowa
- DOI
- 10.17077/etd.0ojjh04t
- Number of pages
- xi, 219 pages
- Copyright
- Copyright © 2013 Rebekah Lynn Oulton
- Comment
This thesis has been optimized for improved web viewing. If you require the original version, contact the University Archives at the University of Iowa: https://www.lib.uiowa.edu/sc/contact/.
- Language
- English
- Description illustrations
- color illustrations, color map
- Description bibliographic
- Includes bibliographical references (pages 191-219).
- Academic Unit
- Civil and Environmental Engineering
- Record Identifier
- 9983777233202771
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