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A meta-analysis was conducted to compare the total amount of ionic liquid (IL) literature (n = 39,036) to the body of publications dealing with IL toxicity (n = 213), with the goal of establishing the state of knowledge and existing information gaps. Publications on IL toxicity were collected from the

A meta-analysis was conducted to compare the total amount of ionic liquid (IL) literature (n = 39,036) to the body of publications dealing with IL toxicity (n = 213), with the goal of establishing the state of knowledge and existing information gaps. Publications on IL toxicity were collected from the SciFinder database and sorted by cation and model organism studied. Studies focusing on pharmacokinetics and drug development were excluded, as were structure-activity relationship methods of data collection. Total publishing activity was used as a measure to gauge research and industrial usage of ILs as well as the knowledge base of toxicology. Five of the most commonly studied IL cations were identified and used to establish a relationship between toxicity data and potential of commercial use: imidazolium, ammonium, phosphonium, pyridinium, and pyrrolidinium. Toxicology publications for all IL cations represented 1.2% ± 0.62% of the total publishing activity; compared with other industrial chemicals, these numbers indicate that there is still a paucity of studies on the adverse effects of this class of chemicals. In vitro models and marine bacteria were the most frequently studied biological systems, contributing 18% and 15%, respectively, to the total body of IL toxicity studies. Whole animal studies (n = 87) comprised 41% of IL toxicity studies, with a subset of in vivo mammalian models consisting of 8%. Human toxicology data were found to be limited to in vitro analyses, indicating substantial knowledge gaps. Risks from long-term and chronic low-level exposure to ILs have not been established yet for any model organisms, reemphasizing the need for filling crucial knowledge gaps concerning human health effects and the environmental safety of ILs. Adding to the existing knowledge of the molecular toxicity characteristics of ILs can help inform the design of greener, less toxic and more benign IL technologies.
ContributorsHeckenbach, Mary (Co-author) / Halden, Rolf (Co-author, Thesis director) / Jehn, Megan (Committee member) / Barrett, The Honors College (Contributor) / School of Life Sciences (Contributor)
Created2015-05
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Description
Current methods measuring the consumption of prescription and illicit drugs are often hampered by innate limitations, the data is slow and often restricted, which can impact the relevance and robustness of the associated data. Here, wastewater-based epidemiology (WBE) was applied as an alternative metric to measure trends in the consumption

Current methods measuring the consumption of prescription and illicit drugs are often hampered by innate limitations, the data is slow and often restricted, which can impact the relevance and robustness of the associated data. Here, wastewater-based epidemiology (WBE) was applied as an alternative metric to measure trends in the consumption of twelve narcotics within a collegiate setting from January 2018 to May 2018 at a Southwestern U.S. university. The present follow-up study was designed to identify potential changes in the consumption patterns of prescription and illicit drugs as the academic year progressed. Samples were collected from two sites that capture nearly 100% of campus-generated wastewater. Seven consecutive 24-hour composite raw wastewater samples were collected each month (n = 68) from both locations. The study identified the average consumption of select narcotics, in units of mg/day/1000 persons in the following order: cocaine (528 ± 266), heroin (404 ± 315), methylphenidate (343 ± 396), amphetamine (308 ±105), ecstasy (MDMA; 114 ± 198), oxycodone (57 ± 28), methadone (58 ± 73), and codeine (84 ± 40). The consumption of oxycodone, methadone, heroin, and cocaine were identified as statistically lower in the Spring 2018 semester compared to the Fall 2017. Universities may need to increase drug education for the fall semester to lower the consumption of drugs in that semester. Data from this research encompasses both human health and the built environment by evaluating public health through collection of municipal wastewater, allowing public health officials rapid and robust narcotic consumption data while maintaining the anonymity of the students, faculty, and staff.
ContributorsCarlson, Alyssa Rose (Author) / Halden, Rolf (Thesis director) / Gushgari, Adam (Committee member) / School of Human Evolution & Social Change (Contributor) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2020-05
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Description

The combined use of methamphetamine and opioids has been reported to be on the rise throughout the United States (U.S.). However, our knowledge of this phenomenon is largely based upon reported overdoses and overdose-related deaths, law enforcement seizures, and drug treatment records; data that are often slow, restricted, and only

The combined use of methamphetamine and opioids has been reported to be on the rise throughout the United States (U.S.). However, our knowledge of this phenomenon is largely based upon reported overdoses and overdose-related deaths, law enforcement seizures, and drug treatment records; data that are often slow, restricted, and only track a portion of the population participating in drug consumption activities. As an alternative, wastewater-based epidemiology (WBE) has the capability to track licit and illicit drug trends within an entire community, at a low cost and in near real-time, while providing anonymity to those contributing to the sewer shed. In this study, wastewater was collected from two Midwestern U.S. cities (2017-2019) and analyzed for the prevalence of methamphetamine and the opioids oxycodone, codeine, fentanyl, tramadol, hydrocodone, and hydromorphone. Monthly 24-hour time-weighted composite samples (n = 48) from each city were analyzed using isotope dilution liquid chromatography tandem mass spectrometry. Results showed that methamphetamine and total opioid consumption (milligram morphine equivalents) in City 1 were strongly correlated only in 2017 (Spearman rank order correlation coefficient, ρ = 0.78), the relationship driven by fentanyl, hydrocodone, and hydromorphone. For City 2, methamphetamine and total opioid consumption were strongly positively correlated during the entire study (ρ = 0.54), with the correlations driven by hydrocodone and hydromorphone. In both cities, hydrocodone and hydromorphone mass loads were highly correlated, suggesting a parent and metabolite relationship. WBE provides important insights into licit and illicit drug consumption patterns in near real-time as they evolve; important information for community stakeholders in municipalities across the U.S.

ContributorsClick, Kathleen Grace (Author) / Halden, Rolf (Thesis director) / Gushgari, Adam (Committee member) / Driver, Erin (Committee member) / School of Life Sciences (Contributor) / School of Human Evolution & Social Change (Contributor) / Barrett, The Honors College (Contributor)
Created2020-05
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Description
Alzheimer’s disease (AD) is a neurodegenerative disease resulting in loss of cognitive function and is not considered part of the typical aging process. Recently, research is being conducted to study environmental effects on AD because the exact molecular mechanisms behind AD are not known. The associations between various toxins and

Alzheimer’s disease (AD) is a neurodegenerative disease resulting in loss of cognitive function and is not considered part of the typical aging process. Recently, research is being conducted to study environmental effects on AD because the exact molecular mechanisms behind AD are not known. The associations between various toxins and AD have been mixed and unclear. In order to better understand the role of the environment and toxic substances on AD, we conducted a literature review and geospatial analysis of environmental, specifically wastewater, contaminants that have biological plausibility for increasing risk of development or exacerbation of AD. This literature review assisted us in selecting 10 wastewater toxic substances that displayed a mixed or one-sided relationship with the symptoms or prevalence of Alzheimer’s for our data analysis. We utilized data of toxic substances in wastewater treatment plants and compared them to the crude rate of AD in the different Census regions of the United States to test for possible linear relationships. Using data from the Targeted National Sewage Sludge Survey (TNSSS) and the Centers for Disease Control and Prevention (CDC), we developed an application using R Shiny to allow users to interactively visualize both datasets as choropleths of the United States and understand the importance of this area of research. Pearson’s correlation coefficient was calculated resulting in arsenic and cadmium displaying positive linear correlations with AD. Other analytes from this statistical analysis demonstrated mixed correlations with AD. This application and data analysis serve as a model in the methodology for further geospatial analysis on AD. Further data analysis and visualization at a lower level in terms of scope is necessary for more accurate and reliable evidence of a causal relationship between the wastewater substance analytes and AD.
GitHub Repository: https://github.com/komal-agrawal/AD_GIS.git
ContributorsAgrawal, Komal (Author) / Scotch, Matthew (Thesis director) / Halden, Rolf (Committee member) / College of Health Solutions (Contributor, Contributor) / Barrett, The Honors College (Contributor)
Created2019-05
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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

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
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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

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
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Description
This dissertation is focused on environmental releases from U.S. wastewater infrastructure of recently introduced, mass-produced insecticides, namely neonicotinoids as well as fipronil and its major degradates (sulfone, sulfide, amide, and desulfinyl derivatives), jointly known as fiproles. Both groups of compounds recently have caught the attention of regulatory agencies worldwide due

This dissertation is focused on environmental releases from U.S. wastewater infrastructure of recently introduced, mass-produced insecticides, namely neonicotinoids as well as fipronil and its major degradates (sulfone, sulfide, amide, and desulfinyl derivatives), jointly known as fiproles. Both groups of compounds recently have caught the attention of regulatory agencies worldwide due to their toxic effects on pollinators and on aquatic invertebrates at very low, part-per-trillion levels (Chapter 1). Mass balance studies conducted for 13 U.S. wastewater treatment plants (WWTPs) showed ubiquitous occurrence (3-666 ng/L) and persistence of neonicotinoids (Chapter 2). For the years 2001 through 2016, a longitudinal nationwide study was conducted on the occurrence of fiproles, via analysis of sludge as well as raw and treated wastewater samples. Sludge analysis revealed ubiquitous fiprole occurrence since 2001 (0.2-385 µg/kg dry weight) and a significant increase (2.4±0.3-fold; p<0.005) to elevated levels found both in 2006/7 and 2015/6. This study established a marked persistence of fiproles during both wastewater and sludge treatment, while also identifying non-agricultural uses as a major source of fiprole loading to wastewater (Chapter 3). Eight WWTPs were monitored in Northern California to assess pesticide inputs into San Francisco Bay from wastewater discharge. Per-capita-contaminant-loading calculations identified flea and tick control agents for use on pets as a previously underappreciated source term dominating the mass loading of insecticides to WWTPs in sewage and to the Bay in treated wastewater (Chapter 4). A nationwide assessment of fipronil emissions revealed that pet products, while representing only 22±7% of total fipronil usage (2011-2015), accounted for 86±5% of the mass loading to U.S. surface waters (Chapter 5). In summary, the root cause for considerable annual discharges into U.S. surface waters of the neonicotinoid imidacloprid (3,700-5,500 kg/y) and of fipronil related compounds (1,600-2,400 kg/y) is domestic rather than agricultural insecticide use. Reclaimed effluent from U.S. WWTPs contained insecticide levels that exceed toxicity benchmarks for sensitive aquatic invertebrates in 83% of cases for imidacloprid and in 67% of cases for fipronil. Recommendations are provided on how to limit toxic inputs in the future.
ContributorsSadaria, Akash Mahendra (Author) / Halden, Rolf (Thesis advisor) / Fraser, Matthew (Committee member) / Perreault, Francois (Committee member) / Mascaro, Giuseppe (Committee member) / Arizona State University (Publisher)
Created2017
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Description
Plastic pollution has become a global threat to ecosystems worldwide, with microplastics now representing contaminants reported to occur in ambient air, fresh water, seawater, soils, fauna and people. Over time, larger macro-plastics are subject to weathering and fragmentation, resulting in smaller particles, termed ‘microplastics’ (measuring < 5 mm in diameter),

Plastic pollution has become a global threat to ecosystems worldwide, with microplastics now representing contaminants reported to occur in ambient air, fresh water, seawater, soils, fauna and people. Over time, larger macro-plastics are subject to weathering and fragmentation, resulting in smaller particles, termed ‘microplastics’ (measuring < 5 mm in diameter), which have been found to pollute virtually every marine and terrestrial ecosystem on the planet. This thesis explored the transfer of plastic pollutants from consumer products into the built water environment and ultimately into global aquatic and terrestrial ecosystems.

A literature review demonstrated that municipal sewage sludge produced by wastewater treatment plants around the world contains detectable quantities of microplastics. Application of sewage sludge on land was shown to represent a mechanism for transfer of microplastics from wastewater into terrestrial environments, with some countries reporting as high as 113 ± 57 microplastic particles per gram of dry sludge.

To address the notable shortcoming of inconsistent reporting practices for microplastic pollution, this thesis introduced a novel, online calculator that converts the number of plastic particles into the unambiguous metric of mass, thereby making global studies on microplastic pollution directly comparable.

This thesis concludes with an investigation of a previously unexplored and more personal source of plastic pollution, namely the disposal of single-use contact lenses and an assessment of the magnitude of this emerging source of environmental pollution. Using an online survey aimed at quantifying trends with the disposal of lenses in the US, it was discovered that 20 ± 0.8% of contact lens wearers flushed their used lenses down the drain, amounting to 44,000 ± 1,700 kg y-1 of lens dry mass discharged into US wastewater.

From the results it is concluded that conventional and medical microplastics represent a significant global source of pollution and a long-term threat to ecosystems around the world. Recommendations are provided on how to limit the entry of medical microplastics into the built water environment to limit damage to ecosystems worldwide.
ContributorsRolsky, Charles (Author) / Halden, Rolf (Thesis advisor) / Green, Matthew (Committee member) / Neuer, Susanne (Committee member) / Polidoro, Beth (Committee member) / Smith, Andrew (Committee member) / Arizona State University (Publisher)
Created2020
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Description

The Future of Wastewater Sensing workshop is part of a collaboration between Arizona State University Center for Nanotechnology in Society in the School for the Future of Innovation in Society, the Biodesign Institute’s Center for Environmental Security, LC Nano, and the Nano-enabled Water Treatment (NEWT) Systems NSF Engineering Research Center.

The Future of Wastewater Sensing workshop is part of a collaboration between Arizona State University Center for Nanotechnology in Society in the School for the Future of Innovation in Society, the Biodesign Institute’s Center for Environmental Security, LC Nano, and the Nano-enabled Water Treatment (NEWT) Systems NSF Engineering Research Center. The Future of Wastewater Sensing workshop explores how technologies for studying, monitoring, and mining wastewater and sewage sludge might develop in the future, and what consequences may ensue for public health, law enforcement, private industry, regulations and society at large. The workshop pays particular attention to how wastewater sensing (and accompanying research, technologies, and applications) can be innovated, regulated, and used to maximize societal benefit and minimize the risk of adverse outcomes, when addressing critical social and environmental challenges.

ContributorsWithycombe Keeler, Lauren (Researcher) / Halden, Rolf (Researcher) / Selin, Cynthia (Researcher) / Center for Nanotechnology in Society (Contributor)
Created2015-11-01