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This research investigated the influence of bromide-ion concentrations upon trihalomethane (THM) formation and speciation. There is some speculation that bromide will increase the amount of THMs on a mass and/or molar basis. Previous research had indicated that bromide will affect the speciation to form the more brominated forms of THMs, but the extent of this speciation has not been clearly defined. Speciation is important when evaluating THM removal processes. The brominated species may require activated carbon for removal as opposed to air stripping for removal of the volatile species (chloroform). To investigate the role of bromide ion, a half-fractional, factorial matrix was used in which the DOC, pH, and temperature were varied at two levels; chlorine dosage and bromide-ion concentration were varied at three levels; and time was varied at five levels (up to six days). Over 750 experimental observations were used to generate five empirical models employing the six factors. An empirical model was generated to determine the mass for the THM species and to estimate the Total THMs. The results indicate the following: 1) all variables were positively correlated to trihalomethane formation; 2) bromide-ion concentration is a significant factor for each species; 3) bromide increased the THM yield both on a mass and a molar basis; and 4) bromide shifted the species distribution almost completely suppressing chloroform production in favor of the brominated THM species.

This research investigated the relationships between molecular size and the TOC, TTHM, acid strength and color concentrations present in raw and coagulated water from Lake Washington. Three separate coagulants were utilized for investigation. There were: Al, Fe and Mg. Results indicated that the majority of the TOC, color and TTHM precursors were in the colloidal size range and removed by coagulation. The remaining TTHM precursors are mostly molecular and require a process other than coagulation for removal from the potable water before environmental standards are met.

This work represents an interdisciplinary effort to investigate microbiological and chemical manganese (Mn) cycling in drinking water systems using concepts and tools from civil and environmental engineering, microbiology, chemistry, surface science, geology, and applied physics. Microorganisms were isolated from four geographically diverse drinking water systems using selective Mn-oxidizing and -reducing culture media. 16S rRNA gene sequencing revealed that most are bacteria of the Bacillus spp. (i.e., Bacillus pumilus and Bacillus cereus). These bacteria are capable of performing Mn-oxidation and -reduction under controlled laboratory conditions. Pseudo-first order rate constants obtained for microbiological Mn-oxidation and -reduction (aerobic and anaerobic) of these isolates ranged from 0.02 - 0.66 days⁻¹. It is likely that spores formed by Bacillus spp. protect them from chlorine and other disinfectants applied in drinking water systems, explaining their ubiquitous presence. A new method was developed using X-ray photoelectron spectroscopy (XPS) to identify Mn(II), Mn(III), and Mn(IV) on the surfaces of pure oxide standards and filtration media samples from drinking water treatment plants. A necessary step for the comprehensive analysis of Mn-cycling in drinking water systems is to characterize the chemical properties of filtration media surfaces. Analyses of filtration media samples show that, while Mn(IV) was predominant in most samples, a mixture of Mn(III) and Mn(IV) was also identified in some of the filtration media samples studied. The use of both the XPS Mn 3s multiplet splitting and the position and shape of the Mn 3p photo-line provide added confidence for the determination of the oxidation state of Mn in complex heterogeneous environmental samples. XPS was applied to investigate Mn(II) removal by MnOx(s)-coated media under experimental conditions that closely resemble situations encountered in drinking water treatment plants in the absence and presence of chlorine. Macroscopic and spectroscopic results suggest that Mn(II) removal in the absence of chlorine was mainly due to adsorption, while in the presence of chlorine was due to oxidation. Mn(IV) was predominant in all the XPS analyses while Mn(II) was detected only in samples operated without chlorine. Future research should apply XPS under different experimental conditions to understand the specific mechanisms affecting Mn(II) removal by MnOx(s)-coated media. / Ph. D.

Legionella pneumophila is a pathogen that can proliferate in premise (i.e., building) plumbing and, when aerosolized during water use, infect the lungs of exposed individuals and cause a deadly form of pneumonia known as Legionnaires' disease. Given that it is one of the primary sources of tap-water associated disease throughout much of the world, this organism has been the subject of intense research, ranging from aiming to understand key aspects of its physiology that allow it to proliferate in premise plumbing, to the specific virulence factors that make it so infectious to humans. The work presented here starts with a comprehensive review of published studies related to the L. pneumophila proteome, i.e., the set of expressed proteins associated with a given strain under a given set of environmental conditions, showing how the field has progressed in parallel to improvements in mass spectrometry technologies and how proteomics can be used as a tool to understand this unique and important organism. Copper is a natural antimicrobial that can be present in drinking water due to passive release from copper pipes or intentionally dosed (e.g., copper-silver ionization systems) for microbial control. However, some L. pneumophila strains have recently been found to exhibit copper resistance, an adaptive process that is not fully understood at the physiological level. Chapter Two describes the copper survivability of three outbreak-associated strains of L. pneumophila and examines the copper-induced proteome of QC1, a strain found to display high resistance to copper. Pairwise comparisons of the proteomes of copper-resistant and copper sensitive strains indicated that L. pneumophila QC1 adapts to copper exposure via the induction of redox and metal homeostasis proteins, while concomitantly inducing motility and pathogenesis related proteins, suggestive that copper induces a search for a host protozoan strain for protection. In 2014 and 2015, Flint, Michigan experienced the largest per capita community-wide Legionnaires' Disease outbreak in US history. The outbreak was associated with a change in the source of the municipal drinking water supply from Detroit water, which was sourced from the Great Lakes and subject to appropriate corrosion control, to the Flint River, which was not appropriately controlled for corrosivity. The underlying drivers of this outbreak have been debated and include: elevated iron in the water serving as a nutrient for L. pneumophila, diminished chlorine in the water due to reactions with iron, reduced copper in the water due to shifts in pH influencing release from copper pipes, and shifts in potentially key components of the microbial community. In Chapter Three of this dissertation, we employ controlled microcosm studies to establish a fundamental understanding of interactive effects of pipe material and water of varying iron bioavailability (ferric chloride, ferrous chloride and ferric pyrophosphate) on the microbial community and its relationship with L. pneumophila numbers. The combination of copper pipes and Flint River water decreased the diversity of the microbial community to a larger degree than copper pipes with Detroit water, implying greater copper bioavailability in the former condition. Several Order were found to be significantly associated with high or low numbers of culturable L. pneumophila recovered from the microcosms. Most notably, the Order Pseudomonadales was significantly associated to the reactors with low culturable L. pneumophila. This order contains Pseudomonas species known to inhibit the growth of L. pneumophila. The findings reported in this dissertation can be used to develop more informed management practices for drinking water systems to reduce the risk of Legionnaires' Disease outbreaks associated with premise plumbing. Specifically, 1) copper might be inducing a more pathogenic form of copper resistant L. pneumophila, 2) the use of corrosive control in municipal water systems goes beyond the influence on lead and copper pipes, but also on the microbial community, which in part influences L. pneumophila, and 3) there are organisms, such as Pseudomonadales species, associated with environments with low culturable L. pneumophila which might be introduced to the drinking water systems as probiotics. / Doctor of Philosophy / Legionella pneumophila is a microbe found in drinking water plumbing systems. This organism causes Legionnaires' Disease, a severe form of pneumonia that particularly affects immunocompromised individuals. Due to its health and economic impact, there are worldwide efforts to understand the biology of this organism, from the conditions that allows it to grow in the drinking water plumbing, to the specific components that allows it to infect humans. In this dissertation, we first review the published studies related to the L. pneumophila proteome, a powerful tool used to functionally describe biological organisms. This first chapter showed how proteomics can be used to understand this unique and important organism. In the next chapter we studied how copper metals may influence the proteome of L. pneumophila. Copper pipes have been extensively used to control the growth of microorganisms in drinking water systems, however some studies have reported that copper may promote the growth of L. pneumophila. In this chapter, we showed that a copper resistant strain of L. pneumophila adapts to copper exposure by inducing motility and pathogenesis related proteins, suggesting that it might be more infectious. In the last chapter of this dissertation, we investigated the combined effect of pipe material and water chemistry, on the microbial community and its relationship with L. pneumophila. The combination of copper pipes and a more corrosive water decreased the diversity to a larger degree, in comparison to the other evaluated conditions. Several organisms were also identified to be significantly associated with the high or low culturable L. pneumophila. This is of particular interest because they might be used as potential probiotics to control the growth of L. pneumophila. The findings reported in this dissertation can help to better understand the significance of water chemistry and pipe material, particularly copper pipes, for the purpose of reducing risk of Legionnaires' Disease outbreaks associated with drinking water systems.

Thirteen volunteer panelists were trained according to <i>Standard Method</i> 2170, flavor profile analysis (FPA). Following training these panelists underwent triangle test screening to determine whether or not they could detect the odorants used in this study. Following triangle testing, panelists underwent directional difference testing to determine if temperature affected odor perception when presented with two water samples. Following directional difference testing, panelists used FPA and evaluated water samples that contained odorants at either 25°C or 45°C. Samples containing geosmin cooled to 5°C were also evaluated. Sensory analyses experiments indicate that odor intensity is a function of both aqueous concentration and water temperature for geosmin, MIB, nonadienal, n-hexanal, free chlorine, and 1-butanol. The higher water temperature resulted in an increase in odor intensity for some, but not all, concentrations of geosmin, 2-methylisoborneol, <i>trans-2,</i> <i>cis-6-</i>nonadienal, n-hexanal, free chlorine, and 1-butanol. Additionally, above 400 ng/L of geosmin, 400 ng/L of MIB, and 100 ng/L the odor intensity was equal to or less than the odor intensity at 600, 600, and 200 ng/L, respectively. Henry's Law should predict that an increase in concentration would increase the amount of odorant the panelist comes into contact with; however, results demonstrated that at specific aqueous odorant concentrations odor perception did not follow Henry's Law. Odor response to drinking water containing isobutanal was affected by concentration but not water temperature. / Master of Science

A simulation-optimization methodology was used to assess monitoring strategies for a drinking water distribution network. Multiple simulation trials of contamination events were used to create input data for an integer optimization problem. A network model, based on the Blacksburg, VA water distribution system, was used as the basis for a case study of contaminant transport under conditions of uncertainty. The model was not calibrated due to the lack of reliable field data. Optimization of monitoring plans was performed within the context event based simulation trials. This precluded the design of monitoring plans that were directly compatible with requirements of water quality regulations. However, the results of the optimization did provide information that may be of use to the broader problem of compliance monitoring. Optimal plans were assessed in comparison with several alternative plans using a separate set of simulation trials. Optimization of monitoring plans derived from simulated source node contamination events was generally effective at choosing points that provided better detection of source node contamination than alternative plans based on random sampling or judgement sampling. Optimal monitoring plans derived from simulated random node contamination events were ineffective at detecting random node contamination. The results of optimization and the separate analysis of monitoring plan performance indicated that the number of simulation trials may have been inadequate to completely describe the stochastic behavior of the system. Additionally, comparison of these results with those obtained from a previous simulation study indicate that the results of any simulation of distribution system contamination may be very sensitive to the level of contaminant loading and the size and layout of the system. / Master of Science

Approximately 80% of Virginians with private drinking water (PDW) sources are unaware of the quality of their drinking water. Strontium is a water quality contaminant gaining recognition at the federal level. At concentrations >1.5 mg/L, strontium substitutes calcium in the bones leading to bone density disorders (e.g. rickets). This is particularly problematic for children and individuals with low calcium and low protein diets. Because most Virginians do not know the quality of their PDW and since strontium poses a public health risk, this study investigates the sources of strontium in PDW in Virginia and identifies the areas and populations most vulnerable. Physical factors such as rock type, rock age, and fertilizer use have been linked to elevated strontium concentrations in drinking water. Meanwhile, social factors such as poverty, poor diet, and adolescence also increase social vulnerability to health impacts of strontium. Thus, this study identifies both physically and socially vulnerable regions in Virginia using water quality data from the Virginia Household Water Quality Program and statistical and spatial analyses conducted in RStudio 1.0.153 and ArcMap 10.5.1. Physical vulnerabilities were highest in the Ridge and Valley province where geologic formations with high strontium concentrations (e.g., limestone, dolomite, sandstone, and shale) are the dominant the aquifer rocks. The complex relationship between agricultural land use and strontium concentrations made it difficult to determine the impact of fertilizer use on strontium concentrations in PDW in Virginia. In general, the spatial distribution of social vulnerability factors was distinct from physical factors with the exception of food deserts. This study provides information and analysis to help residents of Virginia understand their risk of strontium exposure in PDW. / Master of Science / There are 1.7 million residents in Virginia that rely on private drinking water supplies in their homes. Those individuals are responsible for knowing how often to test their water, what to test their water for, and how to treat their water, if needed, to achieve safe drinking standards. Unfortunately, approximately 80% of Virginians with private drinking water sources (e.g., wells, cisterns, and springs) do not know if their water is safe to drink. Strontium, an element closely related to calcium, is a contaminant that the federal government recognizes as dangerous because in high quantities (>1.5 mg/L of water) it can replace calcium in bones making them brittle (e.g. rickets). These health impacts are more extreme in children and individuals with low calcium and low protein diets. Since strontium poses a public health risk, this study identified areas and populations in Virginia that have higher chances of being exposed to strontium and higher chances of their health being impacted by high levels of strontium. Physical factors such as rock type, rock age, and fertilizer use have been linked to elevated strontium concentrations in drinking water, indicating various physical vulnerabilities. Meanwhile, social factors such as poverty, poor diet, and adolescence also increase social vulnerability to the health impacts of strontium. This paper investigates regions in Virginia that are likely to contain high strontium levels and thus potential health impacts from strontium. Statistical and spatial analyses of water quality data from Virginia Cooperative Extension’s Virginia Household Water Quality Program combined with risk factor data identified vulnerable areas in Virginia. The highest chance of exposure was in counties near the western border of the state (e.g., Augusta, Fredrick, Highland, Montgomery, Shenandoah, and Wythe) due to the presence of limestone, dolomite, sandstone, and shale, all of which naturally contain high amounts of strontium. The land use data indicated that there were no strong patterns of strontium occurrence relative to fertilizer use. In general, the spatial distribution of social vulnerability factors was distinct from physical factors with the exception of food deserts occurring at high rates in the same areas as the samples with high strontium levels (e.g., Augusta, Fredrick, Highland, Montgomery, Shenandoah, and Wythe). The presence of food deserts prevents individuals from obtaining a high calcium and high protein diet, which makes them more vulnerable to the impacts of strontium. Overall, this study can help people in Virginia who are not on public water systems understand their risk of from being exposed to strontium.

The influence of solution pH, DOC concentration, the relative molecular weight distribution of DOC, and the source of DOC were investigated for their effects on the removal of complexed Fe(II) by alum coagulation and/or KMn04 and H20 2 oxidation. The differentiation between particulate, colloidal, and soluble iron species was achieved through the use of 0.2 urn filters and 100K ultrafilters. Results from oxidation and ultrafiltration studies indicated incomplete complexation of the Fe(II) by DOC in solution. Following the addition of either oxidant, uncomplexed Fe(II) was oxidized to Fe (III) which was either complexed by high molecular weight DOC or formed colloidal iron oxides, both of which were efficiently removed by alum coagulation. Alum coagulation alone, however, was ineffective for removing Fe(II) in the presence of DOC. Results revealed the formation of particulate iron species to be a function of DOC source. The formation of colloidal iron was dependent upon DOC concentration and DOC source. The adsorption of DOC by iron oxides was observed to accompany the formation of colloidal iron species. / Master of Science

During the early 1980s, concern over the poor quality of the nation's drinking water began to arise. Though the Safe Drinking Water Act (SDWA) had been passed almost a decade earlier, many problems still existed. These problems included the inability of the Environmental Protection Agency to promulgate new drinking water standards and to enforce new and existing standards. To address the shortcomings of the original act, Congress passed the 1986 SDWA Amendments. This document attempts to accomplish two main goals. The first is to summarize selectively the requirements of the 1986 Safe Drinking Water Act (SDWA) Amendments as reflected in proposed and finalized drinking water regulations. The areas of coverage include proposed regulations for eight inorganic and thirty synthetic organic chemical contaminants, the Surface Water Treatment Rule (SWTR), and the Total Coliform Rule (TCR). In order to facilitate an understanding of the SDWA and the 1986 Amendments, a sectional analysis was provided in an appendix. The second goal of this document is to assess the economic impact of this legislation upon Virginia water facilities. In this regard, the cost of water treatment technologies whose use will likely increase as a result of the legislation have been estimated, compiled, and documented. These technologies include granular activated carbon (GAC); reverse osmosis; ion exchange; and various aeration, filtration, and disinfection technologies. Several case studies that assess and highlight the direct impacts of the 1986 SDWA Amendments upon Virginia water facilities are presented. / Master of Science