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- All Subjects: Environmental engineering
- Creators: Halden, Rolf
- Creators: Halden, Rolf U.
Description
The objective of this research was to predict the persistence of potential future contaminants in indirect potable reuse systems. In order to accurately estimate the fates of future contaminants in indirect potable reuse systems, results describing persistence from EPI Suite were modified to include sorption and oxidation. The target future contaminants studied were the approximately 2000 pharmaceuticals currently undergoing testing by United States Food and Drug Administration (US FDA). Specific organic substances such as analgesics, antibiotics, and pesticides were used to verify the predicted half-lives by comparing with reported values in the literature. During sub-surface transport, an important component of indirect potable reuse systems, the effects of sorption and oxidation are important mechanisms. These mechanisms are not considered by the quantitative structure activity relationship (QSAR) model predictions for half-lives from EPI Suite. Modifying the predictions from EPI Suite to include the effects of sorption and oxidation greatly improved the accuracy of predictions in the sub-surface environment. During validation, the error was reduced by over 50% when the predictions were modified to include sorption and oxidation. Molecular weight (MW) is an important criteria for estimating the persistence of chemicals in the sub-surface environment. EPI Suite predicts that high MW compounds are persistent since the QSAR model assumes steric hindrances will prevent transformations. Therefore, results from EPI Suite can be very misleading for high MW compounds. Persistence was affected by the total number of halogen atoms in chemicals more than the sum of N-heterocyclic aromatics in chemicals. Most contaminants (over 90%) were non-persistent in the sub-surface environment suggesting that the target future drugs do not pose a significant risk to potable reuse systems. Another important finding is that the percentage of compounds produced from the biotechnology industry is increasing rapidly and should dominate the future production of pharmaceuticals. In turn, pharmaceuticals should become less persistent in the future. An evaluation of indirect potable reuse systems that use reverse osmosis (RO) for potential rejection of the target contaminants was performed by statistical analysis. Most target compounds (over 95%) can be removed by RO based on size rejection and other removal mechanisms.
ContributorsLim, Seung (Author) / Fox, Peter (Thesis advisor) / Abbaszadegan, Morteza (Committee member) / Halden, Rolf (Committee member) / Arizona State University (Publisher)
Created2011
Description
This thesis examines the composition, flow rate, and recyclability of two abundant materials generated in modern society: municipal sewage sludge (SS) generated during conventional wastewater treatment, and single-use plastic packaging (specifically, plastic bottles) manufactured and dispersed by fast-moving consumer goods companies (FMCG). The study found the presence of 5 precious metals in both American and Chinese sewage sludges. 13 rare elements were found in American sewage sludge while 14 were found in Chinese sewage sludge. Modeling results indicated 251 to 282 million metric tons (MMT) of SS from 2022 to 2050, estimated to contain some 6.8 ± 0.5 MMT of valuable elements in the USA, the reclamation of which is valued at $24B ± $1.6B USD. China is predicted to produce between 819 - 910 MMT of SS between 2022 and 2050 containing an estimated 14.9 ± 1.7 MMT of valuable elements worth a cumulative amount of $94B ± 20B (Chapter 2 and 3). The 4th chapter modeled how much plastic waste Coca-Cola, PespiCo and Nestlé produced and globally dispersed in 21 years: namely an estimated 126 MMT ± 8.7 MMT of plastic. Some 15.6 MMT ± 1.3 MMT (12%) is projected to have become aquatic pollution costing estimated at $286B USD. Some 58 ± 5 MMT or 46% of the total mass were estimated to result in terrestrial plastic pollution, with only minor amounts of 9.9 ± 0.7 MMT, deemed actually recycled. Absent of change, the three companies are predicted to generate an additional 330 ± 15 MMT of plastic by 2050, thereby creating estimated externalities of $8 ± 0.4 trillion USD. The analysis suggests that a small subset of FMCG companies are well positioned to change the current trajectory of global plastic pollution and ocean plastic littering. Chapter 5 examined the barriers to Circular Economy. In an increasingly uncertain post pandemic world, it is becoming progressively important to conserve local resources and extract value from materials that are currently interpreted a “waste” rather than a current or potential future resource.
ContributorsBiyani, Nivedita (Author) / Halden, Rolf U. (Thesis advisor) / Allenby, Braden (Committee member) / Jalbert, Kirk (Committee member) / Arizona State University (Publisher)
Created2022
Description
Wastewater-based epidemiology (WBE) has emerged as a powerful tool for community health assessment, using wastewater-borne biological and chemical markers as analytical targets. This study investigates the critical influence of sampling frequency on the resultant estimates of opioid consumption and the prevalence of SARS-CoV-2 infections at the neighborhood level using common WBE biomarkers including fentanyl, norfentanyl, and the SARS-CoV-2 N1 gene as targets. The goal was to assess sampling methodologies that include the impact of the day of the week and of the sampling frequency. Wastewater samples were collected two or three times per week over the course of five months (n=525) and analyzed by liquid chromatography-tandem mass spectrometry (LC-MS/MS) or reverse transcriptase quantitative polymerase chain reaction (RT-qPCR) for target chemical or molecular indicators of interest. Results showed no statistically significant differences for days of the week (i.e., Tuesday vs. Thursday vs. Saturday) for 24-hour composite samples analyzed for fentanyl or SARS-CoV-2; however, concentrations of the human metabolite of fentanyl, norfentanyl, were statistically different between Tuesday and Saturday (p < 0.05). When data were aggregated either by Tuesday/Thursday or Tuesday/Thursday/Saturday to examine sensitivity to sampling frequency, data were not statistically different except for the Tuesday/Thursday weekly average and Saturday for norfentanyl (p < 0.05). These results highlight how sample collection and data handling methodologies can impact wastewater-derived public health assessments. Care should be taken when selecting an approach to the sampling frequency based on the public health concerns under investigation.
ContributorsAJDINI, ARIANNA (Author) / Halden, Rolf (Thesis advisor) / Driver, Erin (Committee member) / Conroy-Ben, Otakuye (Committee member) / Arizona State University (Publisher)
Created2023
Description
This dissertation focused on studying risks associated with emerging drinking water contaminants and tradeoffs related to water management interventions. The built environment impacts health, as humans on average spend ~90% of their time indoors. Federal regulations generally focus on drinking water at the water treatment plant and within the distribution system as opposed to when it enters buildings after crossing the property line. If drinking water is not properly managed in buildings, it can be a source or amplifier of microbial and chemical contaminants. Unlike regulations for chemical contaminants that are risk-based, for pathogens, regulations are either based on recommended treatment technologies or designated as zero, which is not achievable in practice. Practice-based judgments are typically made at the building level to maintain water quality. This research focuses on two drinking water opportunistic pathogens of public health concern, Legionella pneumophila and Mycobacterium avium complex (MAC). Multiple aspects of drinking water quality in two green buildings were monitored in tandem with water management interventions. Additionally, a quantitative microbial risk assessment framework was used to predict risk-based critical concentrations of MAC for drinking water-related exposures in the indoor environment corresponding to a 1 in 10,000 annual infection target risk benchmark. The overall goal of this work was to inform the development of water management plans and guidelines for buildings that will improve water quality in the built environment and promote better public health. It was determined that a whole building water softening system with ion exchange softening resin and expansion tanks were unexplored reservoirs for the colonization of L. pneumophila. Furthermore, it was observed that typical water management interventions such as flushing and thermal disinfection did not always mitigate water quality issues. Thus, there was a need to implement several atypical interventions such as equipment replacement to improve the building water quality. This work has contributed comprehensive field studies and models that have highlighted the need for additional niches, facility management challenges, and risk tradeoffs for focus in water safety plans. The work also informs additional risk-based water quality policy approaches for reducing drinking water risks.
ContributorsJoshi, Sayalee (Author) / Hamilton, Kerry A (Thesis advisor) / Abbaszadegan, Morteza (Committee member) / Conroy-Ben, Otakuye (Committee member) / Halden, Rolf (Committee member) / Arizona State University (Publisher)
Created2023
Description
Zero-Valent Metals (ZVM) are highly reactive materials and have been proved to be effective in contaminant reduction in soils and groundwater remediation. In fact, zero-Valent Iron (ZVI) has proven to be very effective in removing, particularly chlorinated organics, heavy metals, and odorous sulfides. Addition of ZVI has also been proved in enhancing the methane gas generation in anaerobic digestion of activated sludge. However, no studies have been conducted regarding the effect of ZVM stimulation to Municipal Solid Waste (MSW) degradation. Therefore, a collaborative study was developed to manipulate microbial activity in the landfill bioreactors to favor methane production by adding ZVMs. This study focuses on evaluating the effects of added ZVM on the leachate generated from replicated lab scale landfill bioreactors. The specific objective was to investigate the effects of ZVMs addition on the organic and inorganic pollutants in leachate. The hypothesis here evaluated was that adding ZVM including ZVI and Zero Valent Manganese (ZVMn) will enhance the removal rates of the organic pollutants present in the leachate, likely by a putative higher rate of microbial metabolism. Test with six (4.23 gallons) bioreactors assembled with MSW collected from the Salt River Landfill and Southwest Regional Landfill showed that under 5 grams /liter of ZVI and 0.625 grams/liter of ZVMn additions, no significant difference was observed in the pH and temperature data of the leachate generated from these reactors. The conductivity data suggested the steady rise across all reactors over the period of time. The removal efficiency of sCOD was highest (27.112 mg/lit/day) for the reactors added with ZVMn at the end of 150 days for bottom layer, however the removal rate was highest (16.955 mg/lit/day) for ZVI after the end of 150 days of the middle layer. Similar trends in the results was observed in TC analysis. HPLC study indicated the dominance of the concentration of heptanoate and isovalerate were leachate generated from the bottom layer across all reactors. Heptanoate continued to dominate in the ZVMn added leachate even after middle layer injection. IC analysis concluded the chloride was dominant in the leachate generated from all the reactors and there was a steady increase in the chloride content over the period of time. Along with chloride, fluoride, bromide, nitrate, nitrite, phosphate and sulfate were also detected in considerable concentrations. In the summary, the addition of the zero valent metals has proved to be efficient in removal of the organics present in the leachate.
ContributorsPandit, Gandhar Abhay (Author) / Cadillo – Quiroz, Hinsby (Thesis advisor) / Olson, Larry (Thesis advisor) / Boyer, Treavor (Committee member) / Arizona State University (Publisher)
Created2019
Description
This dissertation critically evaluated methodologies and devices for assessing and protecting the health of human populations, with particular emphasis on groundwater remediation and the use of wastewater-based epidemiology (WBE) to inform population health. A meta-analysis and assessment of laboratory-scale treatability studies for removing chlorinated solvents from groundwater found that sediment microcosms operated as continuous-flow columns are preferable to batch bottles when seeking to emulate with high fidelity the complex conditions prevailing in the subsurface in contaminated aquifers (Chapter 2). Compared to monitoring at the field-scale, use of column microcosms also showed (i) improved chemical speciation, and (ii) qualitative predictability of field parameters (Chapter 3). Monitoring of glucocorticoid hormones in wastewater of a university campus showed (i) elevated stress levels particularly at the start of the semester, (ii) on weekdays relative to weekend days (p = 0.05) (161 ± 42 μg d-1 per person, 122 ± 54 μg d-1 per person; p ≤ 0.05), and (iii) a positive association between levels of stress hormones and nicotine (rs: 0.49) and caffeine (0.63) consumption in this student population (Chapter 4). Also, (i) alcohol consumption determined by WBE was in line with literature estimates for this young sub-population (11.3 ± 7.5 g d-1 per person vs. 10.1 ± 0.8 g d-1 per person), whereas caffeine and nicotine uses were below (114 ± 49 g d-1 per person, 178 ± 19 g d-1 per person; 627 ± 219 g d-1 per person, 927 ± 243 g d-1 per person). The introduction of a novel continuous in situ sampler to WBE brought noted benefits relative to traditional time-integrated sampling, including (i) a higher sample coverage (93% vs. 3%), (ii) an ability to captured short-term analyte pulses (e.g., heroin, fentanyl, norbuprenorphine, and methadone), and (iii) an overall higher mass capture for drugs of abuse like morphine, fentanyl, methamphetamine, amphetamine, and the opioid antagonist metabolite norbuprenorphine (p ≤ 0.01). Methods and devices developed in this work are poised to find applications in the remediation sector and in human health assessments.
ContributorsDriver, Erin Michelle (Author) / Halden, Rolf (Thesis advisor) / Conroy-Ben, Otakuye (Committee member) / Kavazanjian, Edward (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2018
Description
This dissertation studies the larger issue of antibiotic resistance with respect to how antibiotics are being introduced into the environment, focusing on two major anthropogenic pathways: animal husbandry for human consumption, and the recycling of wastewater and municipal sludge generated during conventional biological sewage treatment.
For animal production on land (agriculture) antibiotics are often used for growth enhancement and increased feed efficiency. For animal production in water (aquaculture) antibiotics are often used as a prophylactic. I found that the same antibiotics are being used in both industries and that the same strains of human pathogens have also been isolated from both sources, expressing identical resistance mechanisms. In U.S. seafood, five out of 47 antibiotics screened for were detected at levels of 0.3 to 7.7 ng/g fresh weight. Although compliant with FDA regulations, the risk for resistance still exists, as even low antibiotic concentrations have been shown to exert selective pressure on bacteria.
Similarly low concentrations of antibiotics were found in U.S. biosolids at levels of 0.6 to 19.1 ng/g dry weight. Of the five antibiotics detected, two have never been reported before in biosolids. Three have never been reported before in U.S. biosolids. Using the raw numbers obtained from antibiotic screenings in biosolids, I assessed the impact of employing four different LC-MS/MS methods, concluding that analysts should experimentally determine the most appropriate quantitation method based on the analyte targeted, matrix investigated, and research goals pursued. Preferred quantitation approaches included the isotope dilution method with use of an analogous standard and, although time and resource demanding, the method of standard addition.
In conclusion, antibiotics introduced into the environment via agriculture, aquaculture, and wastewater recycling pose a combination of chemical and biological threats. Aside from exerting outright chemical toxicity to non-target organisms, antibiotic residues can promote the development of multi-drug resistance in human pathogens. Public health protection approaches to stem the risks posed by animal husbandry may include reserving drugs for exclusive, human use, decreasing their usage altogether, improving reporting efforts, reevaluating existing regulations on agricultural and aquacultural antibiotic usage, and improved risk assessment for biosolids application on land.
For animal production on land (agriculture) antibiotics are often used for growth enhancement and increased feed efficiency. For animal production in water (aquaculture) antibiotics are often used as a prophylactic. I found that the same antibiotics are being used in both industries and that the same strains of human pathogens have also been isolated from both sources, expressing identical resistance mechanisms. In U.S. seafood, five out of 47 antibiotics screened for were detected at levels of 0.3 to 7.7 ng/g fresh weight. Although compliant with FDA regulations, the risk for resistance still exists, as even low antibiotic concentrations have been shown to exert selective pressure on bacteria.
Similarly low concentrations of antibiotics were found in U.S. biosolids at levels of 0.6 to 19.1 ng/g dry weight. Of the five antibiotics detected, two have never been reported before in biosolids. Three have never been reported before in U.S. biosolids. Using the raw numbers obtained from antibiotic screenings in biosolids, I assessed the impact of employing four different LC-MS/MS methods, concluding that analysts should experimentally determine the most appropriate quantitation method based on the analyte targeted, matrix investigated, and research goals pursued. Preferred quantitation approaches included the isotope dilution method with use of an analogous standard and, although time and resource demanding, the method of standard addition.
In conclusion, antibiotics introduced into the environment via agriculture, aquaculture, and wastewater recycling pose a combination of chemical and biological threats. Aside from exerting outright chemical toxicity to non-target organisms, antibiotic residues can promote the development of multi-drug resistance in human pathogens. Public health protection approaches to stem the risks posed by animal husbandry may include reserving drugs for exclusive, human use, decreasing their usage altogether, improving reporting efforts, reevaluating existing regulations on agricultural and aquacultural antibiotic usage, and improved risk assessment for biosolids application on land.
ContributorsDone, Hansa Yi-Yun (Author) / Halden, Rolf U. (Thesis advisor) / Haydel, Shelley E (Committee member) / Abbaszadegan, Morteza (Committee member) / Arizona State University (Publisher)
Created2015
Description
Up to 25 percent of the operating budget for contaminated site restoration projects is spent on site characterization, including long-term monitoring of contaminant concentrations. The sensitivity, selectivity, and reproducibility of analytical methods have improved to the point where sampling techniques bear the primary responsibility for the accuracy and precision of the data. Most samples represent discrete concentrations in time and space; with sampling points frequently limited in both dimensions, sparse data sets are heavily extrapolated and the quality of data further limited.
Methods are presented for characterizing contaminants in water (groundwater and surface waters) and indoor air. These techniques are integrative, providing information averaged over time and/or space, as opposed to instantaneous point measurements. Contaminants are concentrated from the environment, making these methods applicable to trace contaminants. These methods have the potential to complement existing techniques, providing the practitioner with opportunities to reduce costs and improve the quality of the data used in decision making.
A conceptual model for integrative sampling of environmental waters is developed and a literature review establishes an advantage in precision for active samplers. A programmable sampler was employed to measure the concentration of chromate in a shallow aquifer exhibiting time-dependent contaminant concentrations, providing a unique data set and sustainability benefits. The analysis of heat exchanger condensate, a waste stream generated by air conditioning, is demonstrated in a non-intrusive method for indoor air quality assessment. In sum, these studies present new opportunities for effective, sustainable environmental characterization.
Methods are presented for characterizing contaminants in water (groundwater and surface waters) and indoor air. These techniques are integrative, providing information averaged over time and/or space, as opposed to instantaneous point measurements. Contaminants are concentrated from the environment, making these methods applicable to trace contaminants. These methods have the potential to complement existing techniques, providing the practitioner with opportunities to reduce costs and improve the quality of the data used in decision making.
A conceptual model for integrative sampling of environmental waters is developed and a literature review establishes an advantage in precision for active samplers. A programmable sampler was employed to measure the concentration of chromate in a shallow aquifer exhibiting time-dependent contaminant concentrations, providing a unique data set and sustainability benefits. The analysis of heat exchanger condensate, a waste stream generated by air conditioning, is demonstrated in a non-intrusive method for indoor air quality assessment. In sum, these studies present new opportunities for effective, sustainable environmental characterization.
ContributorsRoll, Isaac B (Author) / Halden, Rolf U. (Thesis advisor) / Johnson, Paul C (Committee member) / Kavazanjian, Edward (Committee member) / Arizona State University (Publisher)
Created2015
Description
The influence of climate variability and reclaimed wastewater on the water supply necessitates improved understanding of the treatability of trace and bulk organic matter. Dissolved organic matter (DOM) mobilized during extreme weather events and in treated wastewater includes natural organic matter (NOM), contaminants of emerging concern (CECs), and microbial extracellular polymeric substances (EPS). The goal of my dissertation was to quantify the impacts of extreme weather events on DOM in surface water and downstream treatment processes, and to improve membrane filtration efficiency and CECs oxidation efficiency during water reclamation with ozone. Surface water quality, air quality and hydrologic flow rate data were used to quantify changes in DOM and turbidity following dust storms, flooding, or runoff from wildfire burn areas in central Arizona. The subsequent impacts to treatment processes and public perception of water quality were also discussed. Findings showed a correlation between dust storm events and change in surface water turbidity (R2=0.6), attenuation of increased DOM through reservoir systems, a 30-40% increase in organic carbon and a 120-600% increase in turbidity following severe flooding, and differing impacts of upland and lowland wildfires. The use of ozone to reduce membrane fouling caused by vesicles (a subcomponent of EPS) and oxidize CECs through increased hydroxyl radical (HO●) production was investigated. An "ozone dose threshold" was observed above which addition of hydrogen peroxide increased HO● production; indicating the presence of ambient promoters in wastewater. Ozonation of CECs in secondary effluent over titanium dioxide or activated carbon did not increase radial production. Vesicles fouled ultrafiltration membranes faster (20 times greater flux decline) than polysaccharides, fatty acids, or NOM. Based upon the estimated carbon distribution of secondary effluent, vesicles could be responsible for 20-60% of fouling during ultrafiltration and may play a vital role in other environmental processes as well. Ozone reduced vesicle-caused membrane fouling that, in conjunction with the presence of ambient promoters, helps to explain why low ozone dosages improve membrane flux during full-scale water reclamation.
ContributorsBarry, Michelle (Author) / Barry, Michelle C (Thesis advisor) / Westerhoff, Paul (Committee member) / Fox, Peter (Committee member) / Halden, Rolf (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2014
Description
Arsenic (As) and chromium (Cr) occur naturally in AZ surface and groundwaters, pose different health impacts, and exhibit different treatment efficacies. Hexavalent chromium (Cr(VI)) has newly recognized human health concerns, and State and Federal agencies are evaluating a low Cr(VI)-specific maximum contaminant level (MCL) for drinking water. Occurrence of Cr and As in municipal drinking waters and industrial cooling tower waters was quantified by grab samples and compared with sampling results obtained from a new passive sampler developed specifically for Cr(VI). Cr(VI) and As concentrations in groundwater used for cooling tower make-up water concentrations were ~3 ppb and ~4 ppb, respectively, and were concentrated significantly in blowdown water (~20 ppb and ~40 ppb). Based upon pending Cr(VI), As, and other metal regulations, these blowdown waters will need routine monitoring and treatment. Cr(VI) concentrations in a water treatment plant (WTP) raw and finished water samples varied from 0.5 and 2 ppb for grab samples collected every 4 hours for 7 consecutive days using an ISCO sampler. The development of an ion exchange (IX) based passive sampler was validated in the field at the WTP and yielded an average exposure within 1 standard deviation of ISCO sampler grab data. Sampling at both the WTP and cooling towers suggested sources of Cr(III) from treatment chemicals or wood preservatives may exist. Since both facilities use chlorine oxidants, I quantified the apparent (pH=5) second-order rate constant for aqueous chlorine (HOCl/OCl-) with Cr(III) to form Cr(VI) as 0.7 M-1s-1. Under typical conditions (2 ppb Cr(III) ; 2 mg/L Cl2) the half-life for the conversion of Cr(III) to the more toxic form Cr(VI) is 4.7 hours. The occurrence studies in AZ and CA show the Cr(VI) and As treatment of groundwaters will be required to meet stringent Cr(VI) regulations. IX technologies, both strong base anion (SBA) and weak base anion (WBA) resin types were screened (and compared) for Cr removal. The SBA IX process for As removal was optimized by utilizing a reactive iron coagulation and filtration (RCF) process to treat spent IX brine, which was then reused to for SBA resin regeneration.
ContributorsBowen, Alexandra (Author) / Paul, Westerhoff K. (Thesis advisor) / Hristovski, Kiril (Committee member) / Halden, Rolf (Committee member) / Arizona State University (Publisher)
Created2014