Matching Items (12)
Filtering by
- All Subjects: Water
- Creators: Fox, Peter
- Creators: Westerhoff, Paul
Description
Nitrate is the most prevalent water pollutant limiting the use of groundwater as a potable water source. The overarching goal of this dissertation was to leverage advances in nanotechnology to improve nitrate photocatalysis and transition treatment to the full-scale. The research objectives were to (1) examine commercial and synthesized photocatalysts, (2) determine the effect of water quality parameters (e.g., pH), (3) conduct responsible engineering by ensuring detection methods were in place for novel materials, and (4) develop a conceptual framework for designing nitrate-specific photocatalysts. The key issues for implementing photocatalysis for nitrate drinking water treatment were efficient nitrate removal at neutral pH and by-product selectivity toward nitrogen gases, rather than by-products that pose a human health concern (e.g., nitrite). Photocatalytic nitrate reduction was found to follow a series of proton-coupled electron transfers. The nitrate reduction rate was limited by the electron-hole recombination rate, and the addition of an electron donor (e.g., formate) was necessary to reduce the recombination rate and achieve efficient nitrate removal. Nano-sized photocatalysts with high surface areas mitigated the negative effects of competing aqueous anions. The key water quality parameter impacting by-product selectivity was pH. For pH < 4, the by-product selectivity was mostly N-gas with some NH4+, but this shifted to NO2- above pH = 4, which suggests the need for proton localization to move beyond NO2-. Co-catalysts that form a Schottky barrier, allowing for localization of electrons, were best for nitrate reduction. Silver was optimal in heterogeneous systems because of its ability to improve nitrate reduction activity and N-gas by-product selectivity, and graphene was optimal in two-electrode systems because of its ability to shuttle electrons to the working electrode. "Environmentally responsible use of nanomaterials" is to ensure that detection methods are in place for the nanomaterials tested. While methods exist for the metals and metal oxides examined, there are currently none for carbon nanotubes (CNTs) and graphene. Acknowledging that risk assessment encompasses dose-response and exposure, new analytical methods were developed for extracting and detecting CNTs and graphene in complex organic environmental (e.g., urban air) and biological matrices (e.g. rat lungs).
ContributorsDoudrick, Kyle (Author) / Westerhoff, Paul (Thesis advisor) / Halden, Rolf (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2013
Description
Granular activated carbon (GAC) filters are final polishing step in the drinking water treatment systems for removal of dissolved organic carbon fractions. Generally filters are colonized by bacterial communities and their activity reduces biodegradable solutes allowing partial regeneration of GAC's adsorptive capacity. When the bacteria pass into the filtrate due to increased growth, microbiological quality of drinking water is compromised and regrowth in the distribution system occurs. Bacteria attached to carbon particles as biofilms or in conjugation with other bacteria were observed to be highly resistant to post filtration microbial mitigation techniques. Some of these bacteria were identified as pathogenic.
This study focuses on one such pathogen Legionella pneumophila which is resistant to environmental stressors and treatment conditions. It is also responsible for Legionnaires' disease outbreak through drinking water thus attracting attention of regulatory agencies. The work assessed the attachment and colonization of Legionella and heterotrophic bacteria in lab scale GAC media column filters. Quantification of Legionella and HPC in the influent, effluent, column's biofilms and on the GAC particles was performed over time using fluorescent microscopy and culture based techniques.
The results indicated gradual increase in the colonization of the GAC particles with HPC bacteria. Initially high number of Legionella cells were detected in the column effluent and were not detected on GAC suggesting low attachment of the cells to the particles potentially due to lack of any previous biofilms. With the initial colonization of the filter media by other bacteria the number of Legionella cells on the GAC particles and biofilms also increased. Presence of Legionella was confirmed in all the samples collected from the columns spiked with Legionella. Significant increase in the Legionella was observed in column's inner surface biofilm (0.25 logs up to 0.52 logs) and on GAC particles (0.42 logs up to 0.63 logs) after 2 months. Legionella and HPC attached to column's biofilm were higher than that on GAC particles indicating the strong association with biofilms. The bacterial concentration slowly increased in the effluent. This may be due to column's wall effect decreasing filter efficiency, possible exhaustion of GAC capacity over time and potential bacterial growth.
This study focuses on one such pathogen Legionella pneumophila which is resistant to environmental stressors and treatment conditions. It is also responsible for Legionnaires' disease outbreak through drinking water thus attracting attention of regulatory agencies. The work assessed the attachment and colonization of Legionella and heterotrophic bacteria in lab scale GAC media column filters. Quantification of Legionella and HPC in the influent, effluent, column's biofilms and on the GAC particles was performed over time using fluorescent microscopy and culture based techniques.
The results indicated gradual increase in the colonization of the GAC particles with HPC bacteria. Initially high number of Legionella cells were detected in the column effluent and were not detected on GAC suggesting low attachment of the cells to the particles potentially due to lack of any previous biofilms. With the initial colonization of the filter media by other bacteria the number of Legionella cells on the GAC particles and biofilms also increased. Presence of Legionella was confirmed in all the samples collected from the columns spiked with Legionella. Significant increase in the Legionella was observed in column's inner surface biofilm (0.25 logs up to 0.52 logs) and on GAC particles (0.42 logs up to 0.63 logs) after 2 months. Legionella and HPC attached to column's biofilm were higher than that on GAC particles indicating the strong association with biofilms. The bacterial concentration slowly increased in the effluent. This may be due to column's wall effect decreasing filter efficiency, possible exhaustion of GAC capacity over time and potential bacterial growth.
ContributorsSharma, Harsha (Author) / Abbaszadegan, Morteza (Thesis advisor) / Alum, Absar (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2014
Description
Chloroform (CHCl3) is an important atmospheric pollutant by its direct health effects as well as by its contribution to photochemical smog formation. Chloroform outgassing from swimming pools is not typically considered a source of atmospheric CHCl3 because swimming pools are scarce compared to other sources. However, large urban areas in hot climates such as Phoenix, AZ contain a substantial amount of swimming pools, potentially resulting in significant atmospheric fluxes. In this study, CHCl3 formation potential (FP) from disinfection of swimming pools in Phoenix was investigated through laboratory experiments and annual CHCl3 emission fluxes from swimming pools were estimated based on the experimental data.
Swimming pool water (collected in June 2014 in Phoenix) and model contaminants (Pharmaceuticals and Personal Care Products (PPCPs), Endocrine Disrupting Compounds (EDCs), artificial sweeteners, and artificial human waste products) were chlorinated in controlled laboratory experiments. The CHCl3 production during chlorination was determined using Gas Chromatography-Mass Spectrometry (GC-MS) following solid-phase microextraction (SPME). Upon chlorination, all swimming pool water samples and contaminants produced measureable amounts of chloroform. Chlorination of swimming pool water produced 0.005-0.134 mol CHCl3/mol C and 0.004-0.062 mol CHCl3/mol Cl2 consumed. Chlorination of model contaminants produced 0.004-0.323 mol CHCl3/mol C and 0.001-0.247 mol CHCl3/mol Cl2 consumed. These numbers are comparable and indicate that the model contaminants react similarly to swimming pool water during chlorination. The CHCl3 flux from swimming pools in Phoenix was estimated at approximately 3.9-4.3 Gg/yr and was found to be largely dependent on water temperature and wind speed while air temperature had little effect. This preliminary estimate is orders of magnitude larger than previous estimates of anthropogenic emissions in Phoenix suggesting that swimming pools might be a significant source of atmospheric CHCl3 locally.
Swimming pool water (collected in June 2014 in Phoenix) and model contaminants (Pharmaceuticals and Personal Care Products (PPCPs), Endocrine Disrupting Compounds (EDCs), artificial sweeteners, and artificial human waste products) were chlorinated in controlled laboratory experiments. The CHCl3 production during chlorination was determined using Gas Chromatography-Mass Spectrometry (GC-MS) following solid-phase microextraction (SPME). Upon chlorination, all swimming pool water samples and contaminants produced measureable amounts of chloroform. Chlorination of swimming pool water produced 0.005-0.134 mol CHCl3/mol C and 0.004-0.062 mol CHCl3/mol Cl2 consumed. Chlorination of model contaminants produced 0.004-0.323 mol CHCl3/mol C and 0.001-0.247 mol CHCl3/mol Cl2 consumed. These numbers are comparable and indicate that the model contaminants react similarly to swimming pool water during chlorination. The CHCl3 flux from swimming pools in Phoenix was estimated at approximately 3.9-4.3 Gg/yr and was found to be largely dependent on water temperature and wind speed while air temperature had little effect. This preliminary estimate is orders of magnitude larger than previous estimates of anthropogenic emissions in Phoenix suggesting that swimming pools might be a significant source of atmospheric CHCl3 locally.
ContributorsRose, Christy J (Author) / Herckes, Pierre (Thesis advisor) / Fraser, Matthew (Committee member) / Hayes, Mark (Committee member) / Westerhoff, Paul (Committee member) / Arizona State University (Publisher)
Created2014
Description
Population growth and fresh water depletion challenge drinking water utilities. Surface water quality is impacted significantly by climate variability, human activities, and extreme events like natural disasters. Dissolved organic carbon (DOC) is an important water quality index and the precursor of disinfection by-products (DBPs) that varies with both hydrologic and anthropogenic factors. Granular activated carbon (GAC) is a best available technology for utilities to meet Stage 2 D/DBP rule compliance and to remove contaminants of emerging concern (CECs) (e.g., pharmaceutical, personal care products (PCPs), etc.). Utilities can operate GAC with more efficient and flexible strategies with the understanding of organic occurrence in source water and a model capable predicting DOC occurrence. In this dissertation, it was found that DOC loading significantly correlated with spring runoff and was intensified by dry-duration antecedent to first flush. Dynamic modeling based on reservoir management (e.g., pump-back operation) was established to simulate the DOC transport in the reservoir system. Additionally, summer water recreational activities were found to raise the level of PCPs, especially skin-applied products, in raw waters. GAC was examined in this dissertation for both carbonaceous and emerging nitrogenous DBP (N-DBP) precursors (i.e., dissolved organic nitrogen (DON)) removal. Based on the experimental findings, GAC preferentially removes UV254-absorbing material, and DOC is preferentially removed over DON which may be composed primarily of hydrophilic organic and results in the low affinity for adsorption by GAC. The presence of organic nitrogen can elevate the toxicity of DBPs by forming N-DBPs, and this could be a major drawback for facilities considering installation of a GAC adsorber owing to the poor removal efficiency of DON by GAC. A modeling approach was established for predicting DOC and DON breakthrough during GAC operation. However, installation of GAC adsorber is a burden for utilities with respect to operational and maintenance cost. It is common for utilities to regenerate saturated GAC in order to save the cost of purchasing fresh GAC. The traditional thermal regeneration technology for saturated GAC is an energy intensive process requiring high temperature of incineration. Additionally, small water treatment sites usually ship saturated GAC to specialized facilities for regeneration increasing the already significant carbon footprint of thermal regeneration. An innovative GAC regeneration technique was investigated in this dissertation for the feasibility as on-site water treatment process. Virgin GAC was first saturated by organic contaminant then regenerated in-situ by iron oxide nanocatalysts mixed with hydrogen peroxide. At least 70 % of adsorption capacity of GAC can be regenerated repeatedly for experiments using modeling compound (phenol) or natural organic matter (Suwannee River humic acid). The regeneration efficiency increases with increasing adsorbate concentration. Used-iron nanocatalysts can be recovered repeatedly without significant loss of catalytic ability. This in-situ regeneration technique provides cost and energy efficient solution for water utilities considering GAC installation. Overall, patterns were found for DOC and CEC variations in drinking water sources. Increasing concentrations of bulk (DOC and DON) and/or trace organics challenge GAC operation in utilities that have limited numbers of bed-volume treated before regeneration is required. In-situ regeneration using iron nanocatalysts and hydrogen peroxide provides utilities an alternative energy-efficient operation mode when considering installation of GAC adsorber.
ContributorsChiu, Chao-An (Author) / Westerhoff, Paul (Thesis advisor) / Rittmann, Bruce (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2012
Description
Local municipalities in the Phoenix Metropolitan Area have voiced an interest in purchasing alternate source water with lower DBP precursors. Along the primary source is a hydroelectric dam in which water will be diverted from. This project is an assessment of optimizing the potential blends of source water to a water treatment plant in an effort to enable them to more readily meet DBP regulations. To perform this analysis existing water treatment models were used in conjunction with historic water quality sampling data to predict chemical usage necessary to meet DBP regulations. A retrospective analysis was performed for the summer months of 2007 regarding potential for the WTP to reduce cost through optimizing the source water by an average of 30% over the four-month period, accumulating to overall treatment savings of $154 per MG ($82 per AF).
ContributorsRice, Jacelyn (Author) / Westerhoff, Paul (Thesis advisor) / Fox, Peter (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2011
Description
The purpose of this study was to determine the applicability of fluorescent microspheres as a surrogate to measure the removal of Cryptosporidium oocysts through the coagulation, flocculation, sedimentation, and filtration steps of conventional water treatment. In order to maintain accuracy and applicability, a local water treatment facility was chosen as the system to model. The city of Chandler Arizona utilizes conventional treatment methodologies to remove pathogens from municipal drinking water and thus the water, coagulant, polymer, and doses concentrations were sourced directly from the plant. Jar testing was performed on four combinations of coagulant, polymer, and fluorescent microsphere to determine if the log removal was similar to that of Cryptosporidium oocysts.
Complications with the material properties of the microspheres arose during testing that ultimately yielded unfavorable but conclusive results. Log removal of microspheres did not increase with added coagulant in the predicted manner, though the beads were seen aggregating, the low density of the particles made the sedimentation step inefficient. This result can be explained by the low density of the microspheres as well as the potential presence of residual coagulant present in the system. Given the unfavorable properties of the beads, they do not appear to be a suitable candidate for the surrogacy of Cryptosporidium oocysts in conventional drinking water treatment. The beads in their current state are not an adequate surrogate; however, future testing has been outlined to modify the experiment in such a way that the microspheres should behave like oocysts in terms of physical transportation.
Complications with the material properties of the microspheres arose during testing that ultimately yielded unfavorable but conclusive results. Log removal of microspheres did not increase with added coagulant in the predicted manner, though the beads were seen aggregating, the low density of the particles made the sedimentation step inefficient. This result can be explained by the low density of the microspheres as well as the potential presence of residual coagulant present in the system. Given the unfavorable properties of the beads, they do not appear to be a suitable candidate for the surrogacy of Cryptosporidium oocysts in conventional drinking water treatment. The beads in their current state are not an adequate surrogate; however, future testing has been outlined to modify the experiment in such a way that the microspheres should behave like oocysts in terms of physical transportation.
ContributorsLinks, Alexander Glenn (Author) / Abbaszadegan, Morteza (Thesis advisor) / Alum, Absar (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2015
Description
Quagga mussels are an aquatic invasive species capable of causing economic and ecological damage. Despite the quagga mussels’ ability to rapidly spread, two watersheds, the Salt River system and the Verde River system of Arizona, both had no quagga mussel detections for 8 years. The main factor thought to deter quagga mussels was the stratification of the two watersheds during the summer, resulting in high temperatures in the epilimnion and low dissolved oxygen in the hypolimnion. In 2015, Canyon Lake, a reservoir of the Salt River watershed, tested positive for quagga mussel veligers. In this study, I used Landsat 7 and Landsat 8 satellite data to determine if changes in the surface temperature have caused a change to the reservoir allowing quagga mussel contamination. I used a location in the center of the lake with a root mean squared error (RMSE) of 0.80 and a correlation coefficient (R^2) of 0.82, but I did not detect any significant variations in surface temperatures from recent years. I also measured 21 locations on Canyon Lake to determine if the locations in Canyon Lake were able to harbor quagga mussels. I found that summer stratification caused hypolimnion dissolved oxygen levels to drop well below the quagga mussel threshold of 2mg/L. Surface temperatures, however were not high enough throughout the lake to prevent quagga mussels from inhabiting the epilimnion. It is likely that a lack of substrate in the epilimnion have forced any quagga mussel inhabitants in Canyon Lake to specific locations that were not necessarily near the point of quagga veliger detection sampling. The research suggests that while Canyon Lake may have been difficult for quagga mussels to infest, once they become established in the proper locations, where they can survive through the summer, quagga mussels are likely to become more prevalent.
ContributorsLau, Theresa (Author) / Fox, Peter (Thesis advisor) / Neuer, Susanne (Committee member) / Abbaszadegan, Morteza (Committee member) / Arizona State University (Publisher)
Created2018
Description
Safe, readily available, and reliable sources of water are an essential component of any municipality’s infrastructure. Phoenix, Arizona, a southwestern city, has among the highest per capita water use in the United States, making it essential to carefully manage its reservoirs. Generally, municipal water bodies are monitored through field sampling. However, this approach is limited spatially and temporally in addition to being costly. In this study, the application of remotely sensed reflectance data from Landsat 7’s Enhanced Thematic Mapper Plus (ETM+) and Landsat 8’s Operational Land Imager (OLI) along with data generated through field-sampling is used to gain a better understanding of the seasonal development of algal communities and levels of suspended particulates in the three main terminal reservoirs supplying water to the Phoenix metro area: Bartlett Lake, Lake Pleasant, and Saguaro Lake. Algal abundances, particularly the abundance of filamentous cyanobacteria, increased with warmer temperatures in all three reservoirs and reached the highest comparative abundance in Bartlett Lake. Prymnesiophytes (the class of algae to which the toxin-producing golden algae belong) tended to peak between June and August, with one notable peak occurring in Saguaro Lake in August 2017 during which time a fish-kill was observed. In the cooler months algal abundance was comparatively lower in all three lakes, with a more even distribution of abundance across algae classes. In-situ data from March 2017 to March 2018 were compared with algal communities sampled approximately ten years ago in each reservoir to understand any possible long-term changes. The findings show that the algal communities in the reservoirs are relatively stable, particularly those of the filamentous cyanobacteria, chlorophytes, and prymnesiophytes with some notable exceptions, such as the abundance of diatoms, which increased in Bartlett Lake and Lake Pleasant. When in-situ data were compared with Landsat-derived reflectance data, two-band combinations were found to be the best-estimators of chlorophyll-a concentration (as a proxy for algal biomass) and total suspended sediment concentration. The ratio of the reflectance value of the red band and the blue band produced reasonable estimates for the in-situ parameters in Bartlett Lake. The ratio of the reflectance value of the green band and the blue band produced reasonable estimates for the in-situ parameters in Saguaro Lake. However, even the best performing two-band algorithm did not produce any significant correlation between reflectance and in-situ data in Lake Pleasant. Overall, remotely-sensed observations can significantly improve our understanding of the water quality as measured by algae abundance and particulate loading in Arizona Reservoirs, especially when applied over long timescales.
ContributorsRussell, Jazmine Barkley (Author) / Neuer, Susanne (Thesis advisor) / Fox, Peter (Committee member) / Myint, Soe (Committee member) / Arizona State University (Publisher)
Created2018
Description
Radioactive cesium (137Cs), released from nuclear power plants and nuclear accidental releases, is a problem due to difficulties regarding its removal. Efforts have been focused on removing cesium and the remediation of the contaminated environment. Traditional treatment techniques include Prussian blue and nano zero-valent ion (nZVI) and nano-Fe/Cu particles to remove Cs from water; however, they are not efficient at removing Cs when present at low concentrations of about 10 parts-per-billion (ppb), typical of concentrations found in the radioactive contaminated sites.
The objective of this study was to develop an innovative and simple method to remove Cs+ present at low concentrations by engineering a proteoliposome transporter composed of an uptake protein reconstituted into a liposome vesicle. To achieve this, the uptake protein, Kup, from E. coli, was isolated through protein extraction and purification procedures. The new and simple extraction methodology developed in this study was highly efficient and resulted in purified Kup at ~1 mg/mL. A new method was also developed to insert purified Kup protein into the bilayers of liposome vesicles. Finally, removal of CsCl (10 and 100 ppb) was demonstrated by spiking the constructed proteoliposome in lab-fortified water, followed by incubation and ultracentrifugation, and measuring Cs+ with inductively coupled plasma mass spectrometry (ICP-MS).
The ICP-MS results from testing water contaminated with 100 ppb CsCl, revealed that adding 0.1 – 8 mL of Kup proteoliposome resulted in 0.29 – 12.7% Cs removal. Addition of 0.1 – 2 mL of proteoliposome to water contaminated with 10 ppb CsCl resulted in 0.65 – 3.43% Cs removal. These removal efficiencies were greater than the control, liposome with no protein.
A linear relationship was observed between the amount of proteoliposome added to the contaminated water and removal percentage. Consequently, by adding more volumes of proteoliposome, removal can be simply improved. This suggests that with ~ 60-70 mL of proteoliposome, removal of about 90% can be achieved. The novel technique developed herein is a contribution to emerging technologies in the water and wastewater treatment industry.
The objective of this study was to develop an innovative and simple method to remove Cs+ present at low concentrations by engineering a proteoliposome transporter composed of an uptake protein reconstituted into a liposome vesicle. To achieve this, the uptake protein, Kup, from E. coli, was isolated through protein extraction and purification procedures. The new and simple extraction methodology developed in this study was highly efficient and resulted in purified Kup at ~1 mg/mL. A new method was also developed to insert purified Kup protein into the bilayers of liposome vesicles. Finally, removal of CsCl (10 and 100 ppb) was demonstrated by spiking the constructed proteoliposome in lab-fortified water, followed by incubation and ultracentrifugation, and measuring Cs+ with inductively coupled plasma mass spectrometry (ICP-MS).
The ICP-MS results from testing water contaminated with 100 ppb CsCl, revealed that adding 0.1 – 8 mL of Kup proteoliposome resulted in 0.29 – 12.7% Cs removal. Addition of 0.1 – 2 mL of proteoliposome to water contaminated with 10 ppb CsCl resulted in 0.65 – 3.43% Cs removal. These removal efficiencies were greater than the control, liposome with no protein.
A linear relationship was observed between the amount of proteoliposome added to the contaminated water and removal percentage. Consequently, by adding more volumes of proteoliposome, removal can be simply improved. This suggests that with ~ 60-70 mL of proteoliposome, removal of about 90% can be achieved. The novel technique developed herein is a contribution to emerging technologies in the water and wastewater treatment industry.
ContributorsHakim Elahi, Sepideh (Author) / Conroy-Ben, Otakuye (Thesis advisor) / Abbaszadegan, Morteza (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2018
Description
Six high-production-volume neonicotinoids were traced through a municipal wastewater treatment plant (WWTP) and engineered wetland located downstream, in a study motivated by reports on these insecticides posing threats to non-target invertebrate species and potentially playing a role in the global honeybee colony collapse disorder. An array of automated samplers was deployed in a five-day monitoring campaign and resultant flow-weighted samples were analyzed by liquid chromatography tandem mass spectrometry (LC-MS/MS) using the isotope dilution method. Concentrations in WWTP influent and effluent were 54.7 ± 2.9 and 48.6 ± 2.7 ng/L for imidacloprid, respectively, and 3.7 ± 0.3 and 1.8 ± 0.1 ng/L for acetamiprid, respectively. A mass balance over the WWTP showed no (p=0.09, CI = 95%) removal of imidacloprid, and 56 ± 6% aqueous removal of acetamiprid. In the constructed wetland downstream, a lack of removal was noted for both imidacloprid (from 54.4 ± 3.4 ng/L to 49.9 ± 14.6 ng/L) and acetamiprid (from 2.00 ± 0.03 ng/L to 2.30 ± 0.21 ng/L). Clothianidin was detected only inconsistently in the WWTP and wetland (>2 to 288 ng/L; 60% detection frequency), whereas thiamethoxam (<10 ng/L), thiacloprid (<2 ng/L), and dinotefuran (<180 ng/L) were not detected at all. Thus, imidacloprid and acetamiprid were identified as recalcitrant sewage constituents (estimated U.S. WWTP discharge of 1920- 4780 kg/y) that persist during conventional wastewater treatment to enter U.S. surface waters at potentially harmful concentrations.
ContributorsSadaria, Akash Mahendra (Author) / Halden, Rolf (Thesis advisor) / Fox, Peter (Committee member) / Popat, Sudeep (Committee member) / Arizona State University (Publisher)
Created2015