Coastal Pollution and Food Resources as Determinants of Population Health in American Samoa

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Description
Heavy metals and persistent organic pollutants contribute to human health risks worldwide. Among the most common routes of exposure to pollutants for humans are through the consumption of contaminated water and food, with fish being among the greatest vectors for

Heavy metals and persistent organic pollutants contribute to human health risks worldwide. Among the most common routes of exposure to pollutants for humans are through the consumption of contaminated water and food, with fish being among the greatest vectors for ingestion of heavy metals in humans, particularly mercury.This dissertation consists of three chapters with a central theme of investigating heavy metal and persistent organic pollutant concentrations in fish and corned beef, which are two commonly consumed food items in American Samoa. A literature review illustrated that historically the primary pollutants of concern in fish muscle tissue from American Samoa have been mercury, arsenic, and polycyclic aromatic hydrocarbon mixtures. To better understand the changes in heavy metals and persistent organic pollutants in fish, this study reports an updated data set, comparing concentrations in pollutants as they have changed over time. To further investigate pollutants in fish tissue, 77 locally caught and commonly consumed fish were analyzed for heavy metals and persistent organic pollutants, and baseline human health risk assessments were calculated for contaminants that had available oral reference doses. While in American Samoa collecting fish for contaminant analyses, it was realized that canned corned beef appeared to be more commonly consumed than fresh fish. An IRB approved consumption survey revealed that 89% of American Samoan adults regularly consume fish, which is the same percentage of people that reported eating canned corned beef, indicating a dramatic increase in this food item to their diet since its introduction in the 20th century. Results of this study indicate that fish muscle tissue generally has higher heavy metal concentrations than canned corned beef, and that mercury continues to be a main contaminant of concern when consuming fresh and canned fish in American Samoa. While none of the heavy metal concentrations in corned beef exceeded calculated action levels, these foods might contribute to negative health outcomes in other ways. One of the main findings of this study is that either the presence or the ability to detect persistent organic pollutant concentrations are increasing in fish tissue and should be periodically monitored to adequately reflect current conditions.
Date Created
2023
Agent

Influence of Sampling Frequency on Wastewater-based Public Health Assessments of Opioid Consumption and SARS-CoV-2 Infections

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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

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.
Date Created
2023
Agent

Detection and quantification of microplastics via LC-MS/MS analysis

Description
Current methods for quantifying microplastics via LC-MS/MS analysis have been adapted from environmental monitoring protocols and are often inadequate for sampling within complex matrices. This study explores the application of liquid chromatography-tandem mass spectrometry (LC-MS/MS) method for the detection of

Current methods for quantifying microplastics via LC-MS/MS analysis have been adapted from environmental monitoring protocols and are often inadequate for sampling within complex matrices. This study explores the application of liquid chromatography-tandem mass spectrometry (LC-MS/MS) method for the detection of microplastics. The initial phase of this research utilized pork kidney samples to establish a baseline for background and efficacy of sample processing. These findings underscore the complexity of developing a sensitive and specific analytical technique for microplastics in tissues. The observed discrepancies in contamination and replicability between samples emphasize the need for continual method optimization.
Date Created
2023-12
Agent

Understanding Drinking Water Quality and Evaluating the Risks of Opportunistic Pathogens in Building Water Systems

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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

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.
Date Created
2023
Agent

Studying phthalates in the built environment using wastewater-based epidemiology (WBE) and a materials health investigation using the Health Product Declaration (HPD) Collaborative repository

Description

Phthalates are ubiquitous in the built environment and are used across various fields, despite known endocrine disruptive properties, and other associated health hazards, including abnormalities in reproductive health and development. I investigated the presence of phthalates in the built environment

Phthalates are ubiquitous in the built environment and are used across various fields, despite known endocrine disruptive properties, and other associated health hazards, including abnormalities in reproductive health and development. I investigated the presence of phthalates in the built environment using the Health Product Declaration (HPD) repository to survey for products containing these chemicals, investigated the literature for possible health effects and alternatives to phthalates, and conducted a laboratoy-based feasibility study of urinary biomarkers associated with phthalates using wastewater-based epidemiology (WBE) on a US university campus at the building-scale. Of the 5,278 products in the HPD repository, 73 contained phthalates and were most commonly found in windows, doors, flooring, sealants, insulations, and furnishings. Alternative plasticizers (cardanol, epoxidized soybean oil, hydrogenated castor oil) usage were identified in 10 products from HPD repository. The two wastewater samples analyzed by liquid chromatography-tandem mass spectrometry (LC-MS-MS) showed that dimethyl phthalate (DMP) was detectable, as well as its human metabolite, monomethyl phthalate (MMP), observed at a concentration of 163-202 ng/L. These results indicate low human exposure from the building materials in the limited convenience sample investigated. Future studies of building scale wastewater-based epidemiology are recommended to investigate these and other phthalates commonly found in the built environment, including diisononyl phthalate (DINP) and diisononyl hexahydrophthalate (DINCH).

Date Created
2023-05
Agent

Quantifying phthalate esters, bisphenols, and terephthalic acid concentrations in common bottled water brands after various levels of temperature exposure

Description

Synthetic plastics are ubiquitously used in a broad range of applications, including food and drink packaging. Plastics often contain chemical additives, including bisphenols, phthalates, and terephthalic acid, which can degrade under thermal stress. The environmental presence of these chemicals is

Synthetic plastics are ubiquitously used in a broad range of applications, including food and drink packaging. Plastics often contain chemical additives, including bisphenols, phthalates, and terephthalic acid, which can degrade under thermal stress. The environmental presence of these chemicals is cause for public concern, especially in consumer products that utilize plastic packaging, as many have been identified as endocrine disruptors. This study sought to determine exposure to phthalates, bisphenols, and terephthalic acid by quantifying a broad spectrum of these analytes within three bottled water brands at varying temperature exposure levels using the combination of solid phase extraction followed by isotope dilution liquid chromatography-tandem mass spectrometry. Monobenzyl phthalate was detected in two of the three brands after bottles were heated to ~100 °C, ranging from 98 – 107 ng/L, and bisphenol A was detected in one brand at ~100 °C at an average concentration of 748 ± 36 ng/L. Subsequent mass loading calculations demonstrated that bioaccumulation of BPA from Brand C after high levels of temperature exposure well exceeded the tolerable daily intake (TDI). Findings in this study indicate that consumers should not be expected to incur harmful exposures to the target compounds under normal conditions as analytes were not measured in water bottle samples at 25 °C or 60 °C. Further studies should explore a more nuisance approach to heating over long durations, including that of ultraviolet exposure.

Date Created
2022-12
Agent

Near-infrared Contrast Agents for Cell Type Identification and Detection Utilizing Photoacoustics

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Description
The imaging and detection of specific cell types deep in biological tissue is critical for the diagnosis of cancer and the study of biological phenomena. Current high-resolution optical imaging techniques are depth limited due to the high degree of optical

The imaging and detection of specific cell types deep in biological tissue is critical for the diagnosis of cancer and the study of biological phenomena. Current high-resolution optical imaging techniques are depth limited due to the high degree of optical scattering that occurs in tissues. To address these limitations, photoacoustic (PA) techniques have emerged as noninvasive methods for the imaging and detection of specific biological structures at extended depths in vivo. In addition, near-infrared (NIR) contrast agents have further increased the depth at which PA imaging can be achieved in biological tissues. The goal of this research is to combine novel PA imaging and NIR labeling strategies for the diagnosis of disease and for the detection of neuronal subtypes. Central Hypothesis: Utilizing custom-designed PA systems and NIR labeling techniques will enable the detection of specific cell types in vitro and in mammalian brain slices. Work presented in this dissertation addresses the following: (Chapter 2): The custom photoacoustic flow cytometry system combined with NIR absorbing copper sulfide nanoparticles for the detection of ovarian circulating tumor cells (CTCs) at physiologically relevant concentrations. Results obtained from this Chapter provide a unique tool for the future detection of ovarian CTCs in patient samples at the point of care. (Chapter 3): The custom photoacoustic microscopy (PAM) system can detect genetically encoded near-infrared fluorescent proteins (iRFPs) in cells in vitro. Results obtained from this Chapter can significantly increase the depth at which neurons and cellular processes can be targeted and imaged in vitro. (Chapter 4): Utilizing the Cre/lox recombination system with AAV vectors will enable selective tagging of dopaminergic neurons with iRFP for detection in brain slices using PAM. Thus, providing a new means of increasing the depth at which neuronal subtypes can be imaged and detected in the mammalian brain. Significance: Knowledge gained from this research could have significant impacts on the PA detection of ovarian cancer and extend the depth at which neuronal subtypes are imaged in the mammalian brain.
Date Created
2022
Agent

Assessing the Potential to Determine Diabetes Prevalence at the Community-Level Using Wastewater-Based Epidemiology

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Description

Diabetes affects millions of people globally and can lead to other severe health complications when undiagnosed or not properly managed. The incidence of diabetes has rapidly increased over the past several years, however, not all individuals have access to affordable

Diabetes affects millions of people globally and can lead to other severe health complications when undiagnosed or not properly managed. The incidence of diabetes has rapidly increased over the past several years, however, not all individuals have access to affordable or convenient healthcare. We hypothesize that wastewater-based epidemiology (WBE) has the potential to assess community health status by analyzing biomarkers indicative of human health and disease, including diabetes. Used in tandem with current methods, monitoring indicators of diabetes in community wastewater could provide a comprehensive assessment tool for disease prevalence in large and small populations. Specifically, the proposed targeted biomarker evaluated in this study to indicate population-wide diabetes prevalence was 8-hydroxy-2’-deoxyguanosine (8-OHdG). This work combines a rigorous literature review and initial laboratory studies to explore the possibility of diabetes monitoring at the community level using WBE. Here, 24-hour composite wastewater samples were collected from within two wastewater sub-catchments of Greater Tempe, AZ. Overall goals of this study were to: i) Determine the feasibility to detect endogenous markers of diabetes in community wastewater; ii) Assess the potential impact of confounding factors, such as smoking, cancer, and atherosclerosis, through a literature analysis; and iii) Evaluate the socioeconomic status and demographics of the study population. Preliminary results of the experiments suggest this methodology to be feasible, as indicated by the observation of detectable signals of 8-OHdG in community wastewater collected from the sewer infrastructure; however, future work and continued experimentation will be required to address low signal intensity and assay precision and accuracy. Thus, the work presented here provides valuable proof-of-concept data, with detailed information on the method employed and identified opportunities to further determine the relationship between 8-OHdG concentrations in municipal wastewater and diabetes prevalence at the community level.

Date Created
2022-05
Agent

Assessing the Potential to Determine Diabetes Prevalence at the Community-Level Using Wastewater-Based Epidemiology

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Description

Diabetes affects millions of people globally and can lead to other severe health complications when undiagnosed or not properly managed. The incidence of diabetes has rapidly increased over the past several years, however, not all individuals have access to affordable

Diabetes affects millions of people globally and can lead to other severe health complications when undiagnosed or not properly managed. The incidence of diabetes has rapidly increased over the past several years, however, not all individuals have access to affordable or convenient healthcare. We hypothesize that wastewater-based epidemiology (WBE) has the potential to assess community health status by analyzing biomarkers indicative of human health and disease, including diabetes. Used in tandem with current methods, monitoring indicators of diabetes in community wastewater could provide a comprehensive assessment tool for disease prevalence in large and small populations. Specifically, the proposed targeted biomarker evaluated in this study to indicate population-wide diabetes prevalence was 8-hydroxy-2’- deoxyguanosine (8-OHdG). This work combines a rigorous literature review and initial laboratory studies to explore the possibility of diabetes monitoring at the community level using WBE. Here, 24-hour composite wastewater samples were collected from within two wastewater sub-catchments of Greater Tempe, AZ. Overall goals of this study were to: i) Determine the feasibility to detect endogenous markers of diabetes in community wastewater; ii) Assess the potential impact of confounding factors, such as smoking, cancer, and atherosclerosis, through a literature analysis; and iii) Evaluate the socioeconomic status and demographics of the study population. Preliminary results of the experiments suggest this methodology to be feasible, as indicated by the observation of detectable signals of 8-OHdG in community wastewater collected from the sewer infrastructure; however, future work and continued experimentation will be required to address low signal intensity and assay precision and accuracy. Thus, the work presented here provides valuable proof-of-concept data, with detailed information on the method employed and identified opportunities to further determine the relationship between 8-OHdG concentrations in municipal wastewater and diabetes prevalence at the community level.

Date Created
2022-05
Agent

Tracking Population Trends in Acetaminophen and Ibuprofen Through Wastewater-Based Epidemiology During the COVID-19 Pandemic

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Description

The COVID-19 pandemic caused uncertainty and changing public health recommendations across the world as our understanding of the SARS-CoV-2 virus changed. Following a preliminary assessment by the World Health Organization, non-steroidal anti-inflammatory drugs were said to worsen symptoms and should

The COVID-19 pandemic caused uncertainty and changing public health recommendations across the world as our understanding of the SARS-CoV-2 virus changed. Following a preliminary assessment by the World Health Organization, non-steroidal anti-inflammatory drugs were said to worsen symptoms and should be avoided before the recommendation was subsequently revoked. There also was pain associated with infection, leading to the hypothesis that use of over-the-counter pain medication increases may correlate with increases of SARS-CoV-2 infections. Wastewater samples were collected from two communities in Tempe, AZ from December 2019 to July 2020 (n = 35) and were analyzed by liquid chromatography tandem mass spectrometry (LC-MS/MS) to identify levels of acetaminophen, ibuprofen and their metabolites, acetaminophen sulfate and carboxy-ibuprofen. Results showed 100% detection frequency of all analytes in all samples across the duration of the study. Mass loadings of acetaminophen (918.4 g day-1 +/- 354.8 g day-1) were higher than ibuprofen (182.9 g day-1 +/- 49.8 g day-1), potentially driven by flushing behaviors rather than consumption activities. However, ibuprofen was more heavily consumed than acetaminophen across all days of the study period. Comparisons to COVID-19 clinical cases data showed increased use in ibuprofen with increases in clinical cases loads, while acetaminophen showed no change, suggesting ibuprofen was the over the counter (OTC) medication of choice during the first wave of the pandemic.

Date Created
2022-05
Agent