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- All Subjects: Environmental engineering
- Creators: Halden, Rolf
- Creators: Halden, Rolf U.
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
Environmental releases of neonicotinoid and fipronil insecticides via U.S. wastewater infrastructure
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 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
Description
Microplastics are emerging to be major problem when it comes to water pollution and they pose a great threat to marine life. These materials have the potential to affect a wide range of human population since humans are the major consumers of marine organisms. Microplastics are less than 5 mm in diameter, and can escape from traditional wastewater treatment plant (WWTP) processes and end up in our water sources. Due to their small size, they have a large surface area and can react with chlorine, which it encounters in the final stages of WWTP. After the microplastics accumulate in various bodies of water, they are exposed to sunlight, which contains oxidative ultraviolet (UV) light. Since the microplastics are exposed to oxidants during and after the treatment, there is a strong chance that they will undergo chemical and/or physical changes. The WWTP conditions were replicated in the lab by varying the concentrations of chlorine from 70 to 100 mg/L in increments of 10 mg/L and incubating the samples in chlorine baths for 1–9 days. The chlorinated samples were tested for any structural changes using Raman spectroscopy. High density polyethylene (HDPE), polystyrene (PS), and polypropylene (PP) were treated in chlorine baths and observed for Raman intensity variations, Raman peak shifts, and the formation of new peaks over different exposure times. HDPE responded with a lot of oxidation peaks and shifts of peaks after just one day. For the degradation of semi-crystalline polymers, there was a reduction in crystallinity, as verified by thermal analysis. There was a decrease in the enthalpy of melting as well as the melting temperature with an increase in the exposure time or chlorine concentration, which pointed at the degradation of plastics and bond cleavages. To test the plastic response to
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UV, the samples were exposed to sunlight for up to 210 days and analyzed under Raman spectroscopy. Overall the physical and chemical changes with the polymers are evident and makes a way for the wastewater treatment plant to take necessary steps to capture the microplastics to avoid the release of any kind of degraded microplastics that could affect marine life and the environment.
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UV, the samples were exposed to sunlight for up to 210 days and analyzed under Raman spectroscopy. Overall the physical and chemical changes with the polymers are evident and makes a way for the wastewater treatment plant to take necessary steps to capture the microplastics to avoid the release of any kind of degraded microplastics that could affect marine life and the environment.
ContributorsKelkar, Varun (Author) / Green, Matthew D (Thesis advisor) / Tongay, Sefaattin (Committee member) / Halden, Rolf U. (Committee member) / Arizona State University (Publisher)
Created2017
Description
This dissertation focuses on the application of urban metabolism metrology (UMM) to process streams of the natural and built water environment to gauge public health concerning exposure to carcinogenic N-nitrosamines and abuse of narcotics. A survey of sources of exposure to N-nitrosamines in the U.S. population identified contaminated food products (1,900 ± 380 ng/day) as important drivers of attributable cancer risk (Chapter 2). Freshwater sediments in the proximity of U.S. municipal wastewater treatment plants were shown for the first time to harbor carcinogenic N-nitrosamine congeners, including N-nitrosodibutylamine (0.2-3.3 ng/g dw), N-nitrosodiphenylamine (0.2-4.7 ng/g dw), and N-nitrosopyrrolidine (3.4-19.6 ng/g dw) were, with treated wastewater discharge representing one potential factor contributing to the observed contamination (p=0.42) (Chapter 3). Opioid abuse rates in two small midwestern communities were estimated through the application of wastewater-based epidemiology (WBE). Average concentrations of opioids (City 1; City 2) were highest for morphine (713 ± 38, 306 ± 29 ng/L) and varied by for the remainder of the screened analytes. Furthermore, concentrations of the powerful opioid fentanyl (1.7 ± 0.2, 1.0 ± 0.5 ng/L) in wastewater were reported for the first time in the literature for the U.S. (Chapter 4). To gauge narcotic consumption within college-aged adults the WBE process used in Chapter 4 was applied to wastewater collected from a large university in the Southwestern U.S. Estimated narcotics consumption, in units of mg/day/1,000 persons showed the following rank order: cocaine (470 ± 42), heroin (474 ± 32), amphetamine (302 ± 14) and methylphenidate (236 ± 28). Most parental drugs and their respective metabolites showed detection frequencies in campus wastewater of 80% or more, with the notable exception of fentanyl, norfentanyl, buprenorphine, and norbuprenorphine. Estimated consumption of all narcotics, aside from attention-deficit/hyperactivity disorder medication, were higher than values reported in previous U.S. WBE studies for U.S. campuses (Chapter 5). The analyses presented here have identified variation in narcotic consumption habits across different U.S. communities, which can be gauged through UMM. Application of these techniques should be implemented throughout U.S. communities to provide insight into ongoing substance abuse and health issues within a community.
ContributorsGushgari, Adam Jon (Author) / Halden, Rolf U. (Thesis advisor) / Kavazanjian, Edward (Committee member) / Fraser, Matthew (Committee member) / Venkatesan, Arjun (Committee member) / Mascaro, Giuseppe (Committee member) / Arizona State University (Publisher)
Created2018
Description
Uncertainty is inherent in predictive decision-making, both with respect to forecasting plausible future conditions based on a historic record, and with respect to backcasting likely upstream states from downstream observations. In the first chapter, I evaluated the status of current water resources management policy in the United States (U.S.) with respect to its integration of projective uncertainty into state-level flooding, drought, supply and demand, and climate guidance. I found uncertainty largely absent and discussed only qualitatively rather than quantitatively. In the second chapter, I turned to uncertainty in the interpretation of downstream observations as indicators of upstream behaviors in the field of Wastewater-Based Epidemiology (WBE), which has made possible the near real-time, yet anonymous, monitoring of public health via measurements of biomarkers excreted to wastewater. I found globally, seasonality of air and soil temperature causes biomarker degradation to vary up to 13-fold over the course of a year, constituting part of the background processes WBE must address, or detrend, prior to decision-making. To determine whether the seasonal change in degradation rates was introducing previously unaccounted for uncertainty with respect to differences in observed summertime and winter-time populations, I evaluated demographic indicators recorded by the Census Bureau for correlation with their distance from all major wastewater treatment plants across the U.S. The analysis identified statistically significant correlation for household income, education attainment, unemployment, military service, and the absence of health insurance. Finally, the model was applied to a city-wide case study to test whether temperature could explain some of the trends observed in monthly observations of two opiate compounds. Modeling suggests some of the monthly changes were attributed to natural temperature fluctuation rather than to trends in the substances’ consumption, and that uncertainty regarding discharge location can dominate even relative observed differences in opiate detections. In summary, my work has found temperature an important modulator of WBE results, influencing both the type of populations observed and the likelihood of upstream behaviors disproportionally magnified or obscured, particularly for the more labile biomarkers. There exists significant potential for improving the understanding of empirical observations via numerical modeling and the application of spatial analysis tools.
ContributorsHart, Olga (Author) / Halden, Rolf (Thesis advisor) / Mascaro, Giuseppe (Committee member) / Renaut, Rosemary (Committee member) / Nelson, Keith (Committee member) / Arizona State University (Publisher)
Created2019
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), 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.
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
Description
Novel means are needed to diagnose neurodegenerative diseases (NDDs) and cancer, given delays in medical diagnosis and rising rates of disease incidence, prevalence, and mortality worldwide. Development of NDDs and cancer has been linked to environmental toxins. Ensuing epigenetic changes may serve as helpful biomarkers to diagnose amyotrophic lateral sclerosis (ALS), Parkinson’s Disease (PD), and Alzheimer’s Disease (AD) as well as various cancers sooner and more accurately. This dissertation tabulates and evaluates a spectrum of diagnostic matrixes (i.e., soil, sewage sludge, blood) and markers of disease to inform disease surveillance. A literature search using Preferred Reporting Items for Systematic Reviews and Meta-Analyses (PRISMA) and Bradford Hill criteria implicated BMAA, formaldehyde, Mn, Hg, and Zn as environmental factors with strong association to ALS risk. Another PRISMA search identified epigenetic changes (e.g., DNA methylation) in NDD patients associated with environmental toxic exposures to air pollutants, heavy metals, and organic chemicals. Of the 180 environmental toxins hypothesized to be associated with AD, PD, or ALS, four heavy metals (As, Cd, Mn, and Hg) were common to these NDDs. Sources, as well as evidence and proxies of human exposure to these heavy metals and Pb were investigated here, namely the metal industries, and metal concentrations in topsoil, sewage sludge, and blood. Concentrations of Cd and Pb in sewage sludge were found to be significantly correlated with NDD prevalence rates in co-located populations (state-level) with odds ratios of 2.91 and 4.08, respectively. Markers of exposure and disease in urine and feces were also evaluated using PRISMA, finding 73 of 94 epigenetic biomarker panels to be valid for tracking primarily gastric and urinary cancers. In all studies, geospatial analyses indicated a preference in study cohorts located in the U.S., Europe, and the northern hemisphere, leaving underserved many populous regions particularly in the southern hemisphere. This dissertation draws attention to sewage sludge as a currently underutilized proxy matrix for assessing toxic human exposures and further identified a spectrum of particularly attractive, non-invasive biomarkers for future diagnostic use to promote early detection, survivability, and quality of life of individuals at risk of NDDs and cancer.
ContributorsNewell, Melanie Engstrom (Author) / Halden, Rolf U. (Thesis advisor) / Mastroeni, Diego (Committee member) / Lee, Heewook (Committee member) / Arizona State University (Publisher)
Created2023