Iodine and silver ions (Ag+), added as silver fluoride (AgF) or silver nitrate (AgNO3), are currently being used as a biocide to control the spread of bacteria in the water storage tanks of the International Space Station (ISS). Due to the complications of the iodine system, NASA is interested to completely replace iodine with silver and apply it as an antibacterial surface coating on stainless steel (SS) surfaces for biofouling control in extended space missions. However, Ag+ is highly soluble and rapidly dissolves in water, as a result, the coated surface loses its antibacterial properties. The dissolution of NPs into Ag+ and subsequent solubilization reduces its effectivity or extended period application. This study focuses on the in-situ nucleation of silver nanoparticles (AgNP) on stainless steel followed by their partial passivation by the formation of a low solubility silver sulfide (Ag2S), silver bromide (AgBr), and silver iodide (AgI) shell with various concentrations for an increased long-term biofouling performance and a slower silver release over time. Antibacterial activity was evaluated using Pseudomonas aeruginosa. The highest bacterial inactivation (up to 75%) occurred with sulfidized AgNPs as opposed to bromidized (up to 50%) and iodized NPs (up to 60%). Surface analysis by scanning electron microscopy (SEM) showed considerably fewer particles on AgBr and AgI compared to Ag2S-coated samples. Silver iodide was not tested in additional experiments due to its drawbacks and its poor antibacterial performance compared to sulfidized samples. Compared to pristine AgNPs, Ag release from both sulfidized and bromidized NPs was significantly low (16% vs 6% or less) depending on the extent of sulfidation or bromidation. Experiments were also carried out to investigate the effect of passivation on biofilm formation. Biofilm growth was smaller on surfaces treated with 10-3 M Na2S and 10-3 M NaBr compared to the surface of pristine AgNPs. Overall, sulfidation appears to be the most effective option to control biofilm formation on stainless steel. However, future research is needed to verify the effectiveness of sulfidized AgNPs on other metals including Inconel 718 and Titanium 6Al-4V used in the spacecraft potable water systems.

Nitrogen removal and energy reduction in wastewater treatment are shared goals. Approaches to achieve those goals include the techniques of shortcut nitrogen removal utilizing nitrite shunt, biocatalyst, nitritation, deammonification, and simultaneous nitrification-denitrification. The practice of those techniques is newer in the industry of wastewater treatment but continues to develop, along with the understanding of the biological and chemical activities that drive those processes. The kinetics and stoichiometry of traditional and shortcut nitrogen removal reactions are generally well understood to date. However, the thermodynamics of those processes are complex and deserve additional research to better understand the dominant factors that drive cell synthesis. Additionally, the implementation of nitrogen shortcut techniques can reduce the footprint of wastewater treatment processes that implement nitrogen removal by approximately 5 percent and can reduce operating costs by between 12 and 26 percent annually. Combined, nitrogen shortcut techniques can contribute to significant reduction in the long-term cost to operate, due to lower energy and consumable requirements, fast reaction times resulting in shorter solids retention times, and improvement efficiency in nitrogen removal from wastewater. This dissertation explores and defines the dominant factors that contribute to the success of efficiencies in traditional and shortcut nitrogen removal techniques, focusing on the natural microbiological processes. The culmination of these efforts was used to develop decision matrices to promote consideration of nitrogen shortcut techniques by practitioners during conceptual planning and design of wastewater treatment facilities.

This dissertation focuses on the structure-function relationships of nanomaterials (NMs) and some of their applications in environmental engineering. The aim is to investigate NMs of different surface chemistries and assess their interactions with biological models, evaluate the weathering impact and degradation parameters to improve polymer coatings, test their efficiency for contaminant removal and provide further understanding in the safe design of nanomaterials. Nanoecotoxicological risk assessment currently suffers from a lack of testing procedures adapted to nanomaterials. Graphene oxide (GO) is a carbon nanomaterial (CNM) that consists of a single layer of carbon atoms arranged in a hexagonal network. It is decorated with a high density of oxygen functional groups including epoxide and hydroxyl moieties on the basal planes and carboxylic and carbonyl groups at the edges. The changes in surface chemistry give GO unique properties that can be tailored for a function. Additionally, because of its simple synthesis and flexible chemistry, GO has been a popular building block of many composite CNMs. In environmental engineering, specifically, water treatment, GO has been studied by itself or as a composite for pollutant removal, biofouling reduction, and as an antimicrobial agent, just to name a few. Like GO, silver (Ag) is another NM widely used in water treatment for its biocidal properties. Despite the recent growth in this field, a fundamental understanding of the function-structure relationships in NMs is still progressing. Through a systematic set of experiments, the structure-properties-function and structure-properties-hazard relationships were investigated. These relationships can be used to establish guidelines to engineer “safe-by-design” functional nanomaterials, where materials are tailored to enhance their function while minimizing their inherent biological or environmental hazard.

“Airborne dispersal of microorganisms influences their biogeography, gene flow, atmospheric processes, human health and transmission of pathogens that affect humans, plants and animals” (Alsved et al., 2018). Many airborne pathogens cause diseases, such as Legionnaires disease, which is a type of pneumonia caused due to Legionella. Since the first report of a Legionella outbreak in 1976, or reports of Non – tuberculous Mycobacterium (NTM) outbreaks in hospital and healthcare settings by the CDC, it is significant to understand the behavior, occurrence and persistence of opportunistic pathogenic aerosols in the atmosphere. This study comprises a literature review and experimental work on airborne dispersion of 4 microorganisms – E. coli, Legionella pneumophila, Mycobacterium phlei and bacteriophage P22. The literature review summarizes their characteristics, their potential sources, disease outbreaks, collection and detection methodologies, environmental conditions for their growth and survival and few recommendations for reducing potential outbreaks. Aerosolization of each of these microorganisms was carried out separately in a closed environment using a spray gun and a nebulizer. The spraying time consisted of 1 sec, 5secs or 10secs, from one end of a chamber, and collecting air sample from the other end of the chamber, using a microbial air sampler. The air sample collection was performed to understand their transport, dispersion and reduction in air. Legionella showed a log reduction of ~4 using spray gun and ≤0.6 using nebulizer, whereas Mycobacterium showed a log reduction of ~4.5 using spray gun and ≤0.7 using nebulizer, respectively. Bacteriophage P22 on the other hand showed a 4 log reduction using spray gun and ≤1.4 using the nebulizer. This shows that aerosolization of microorganisms depends on its cell structure, size and survivability. Legionella follows the air – to – water transmission route, and Mycobacterium is hydrophobic, due to which their aerosols are more stable and active, than E. coli. Other environmental properties such as relative humidity and temperature impact the transport and dispersion of microorganisms in air.

The experiments in this study validated the aerosolization and transport of Legionella, Mycobacterium and bacteriophage P22 in a closed environment over time. In general, microbial concentration collected in air increased with aerosolization time of the test water. On the other hand, their concentration significantly decreased as elapsed time progressed after aerosolization, due to settling effect of larger particles and potential reduction due to inactivation of bacterial and viruses in the air.

The impact of physical/chemical properties of gray water on microbial inactivation in gray water using chlorine was investigated through creating artificial gray water in lab, varying specific components, and then measuring microbial inactivation. Gray water was made through taking autoclaved nanopure water, and increasing the concentration of surfacants, the turbidity, the concentration of organic content, and spiking E. coli grown in tryptic soy broth (TSB); chlorine was introduced using Clorox Disinfecting Bleach2. Bacteria was detected using tryptic soy agar (TSA), and E. coli was specifically detected using the selective media, brilliance. The log inactivation of bacteria detected using TSA was shown to be inversely related to the turbidity of the solution. Complete inactivation of E. coli concentrations between 104-105 CFU/100 ml in gray water with turbidities between 10-100 NTU, 0.1-0.5 mg/L of humic acid, and 0.1 ml of Dawn Ultra, was shown to occur, as detected by brilliance, at chlorine concentrations of 1-2 mg/L within 30 seconds. These result in concentration time (CT) values between 0.5-1 mg/L·min. Under the same gray water conditions, and an E. coli concentration of 104 CFU/100 ml and a chlorine concentration of 0.01 mg/L, complete inactivation was shown to occur in all trials within two minutes. These result in CT values ranging from 0.005 to 0.02. The turbidity and humic acid concentration were shown to be inversely related to the log inactivation and directly related to the CT value. This study shows that chlorination is a valid method of treatment of gray water for certain irrigation reuses.

Turbidity is a known problem for UV water treatment systems as suspended particles can shield contaminants from the UV radiation. UV systems that utilize a reflective radiation chamber may be able to decrease the impact of turbidity on the efficacy of the system. The purpose of this study was to determine how kaolin clay and gram flour turbidity affects inactivation of Escherichia coli (E. coli) when using a UV system with a reflective chamber. Both sources of turbidity were shown to reduce the inactivation of E. coli with increasing concentrations. Overall, it was shown that increasing kaolin clay turbidity had a consistent effect on reducing UV inactivation across UV doses. Log inactivation was reduced by 1.48 log for the low UV dose and it was reduced by at least 1.31 log for the low UV dose. Gram flour had a similar effect to the clay at the lower UV dose, reducing log inactivation by 1.58 log. At the high UV dose, there was no change in UV inactivation with an increase in turbidity. In conclusion, turbidity has a significant impact on the efficacy of UV disinfection. Therefore, removing turbidity from water is an essential process to enhance UV efficiency for the disinfection of microbial pathogens.

This dissertation investigates the mechanisms that lead to fouling, as well as how an understanding of how these mechanisms can be leveraged to mitigate fouling.

To limit fouling on feed spacers, various coatings were applied. The results showed silver-coated biocidal spacers outperformed other spacers by all measures. The control polypropylene spacers performed in-line with, or better than, the other coatings. Polypropylene’s relative anti-adhesiveness is due to its surface free energy (SFE; 30.0 +/- 2.8 mN/m), which, according to previously generated models, is near the ideal SFE for resisting adhesion of bacteria and organics (~25 mN/m).

Previous research has indicated that electrochemical surfaces can be used to remove biofilms. To better elucidate the conditions and kinetics of biofilm removal, optical coherence tomography microscopy was used to visualize the biofouling and subsequent cleaning of the surface. The 50.0 mA cm-2 and 87.5 mA cm-2 current densities proved most effective in removing the biofilm. The 50.0 mA cm-2 condition offers the best balance between performance and energy use for anodic operation.

To test the potential to incorporate electrochemical coatings into infrastructure, membranes were coated with carbon nanotubes (CNTs), rendering the membranes electrochemically active. These membranes were biofouled and subsequently cleaned via electrochemical reactions. P. aeruginosa was given 72h to develop a biofilm on the CNT-coated membranes in a synthetic medium simulating desalination brines. Cathodic reactions, which generate H2 gas, produce vigorous bubbling at a current density of 12.5 mA cm-2 and higher, leading to a rapid and complete displacement of the biofilm from the CNT-functionalized membrane surface. In comparison, anodic reactions were unable to disperse the biofilms from the surface at similar current densities.

The scaling behavior of a nanophotonics-enabled solar membrane distillation (NESMD) system was investigated. The results showed the NESMD system to be resistant to scaling. The system operated without any decline in flux up to concentrations 6x higher than the initial salt concentration (8,439 mg/L), whereas in traditional membrane distillation (MD), flux essentially stopped at a salt concentration factor of 2x. Microscope and analytical analyses showed more fouling on the membranes from the MD system.

The study was to analyze the extent of bacterial transport in a two-dimensional tank under saturated conditions. The experiments were done in a 2-D tank packed with 3,700 in3 of fine grained, homogenous, chemically inert sand under saturated conditions. The tank used for transport was decontaminated by backwashing with 0.6% chlorine solution with subsequent backwashing with chlorine-neutral water (tap water and Na2S2O3) thus ensuring no residual chlorine in the tank. The transport of bacteria was measured using samples collected from ports at vertical distances of 5, 15 and 25 inches (12.7, 38.1 and 63.5 cm) from the surface of the sand on both sides for the 2-D tank. An influent concentration of 105 CFU/mL was set as a baseline for both microbes and the percolation rate was set at 11.37 inches/day using a peristaltic pump at the bottom outlet. At depths of 5, 15 and 25 inches, E. coli breakthroughs were recorded at 5, 17 and 28 hours for the ports on the right side and 7, 17 and 29 hours for the ports on the left sides, respectively. At respective distances Legionella breakthroughs were recorded at 8, 22 and 35 hours for the ports on the right side and 9, 24, 36 hours for the ports on the left side, respectively which is homologous to its pleomorphic nature. A tracer test was done and the visual breakthroughs were recorded at the same depths as the microbes. The breakthroughs for the dye at depths of 5, 15 and 25 inches, were recorded at 13.5, 41 and 67 hours for the ports on the right side and 15, 42.5 and 69 hours for the ports on the left side, respectively. However, these are based on visual estimates and the physical breakthrough could have happened at the respective heights before the reported times. This study provided a good basis for the premise that transport of bacterial cells and chemicals exists under recharge practices.

This dissertation aims at developing novel materials and processing routes using alkali activated aluminosilicate binders for porous (lightweight) geopolymer matrices and 3D-printing concrete applications. The major research objectives are executed in different stages. Stage 1 includes developing synthesis routes, microstructural characterization, and performance characterization of a family of economical, multifunctional porous ceramics developed through geopolymerization of an abundant volcanic tuff (aluminosilicate mineral) as the primary source material. Metakaolin, silica fume, alumina powder, and pure silicon powder are also used as additional ingredients when necessary and activated by potassium-based alkaline agents. In Stage 2, a processing route was developed to synthesize lightweight geopolymer matrices from fly ash through carbonate-based activation. Sodium carbonate (Na2CO3) was used in this study to produce controlled pores through the release of CO2 during the low-temperature decomposition of Na2CO3. Stage 3 focuses on 3D printing of binders using geopolymeric binders along with several OPC-based 3D printable binders. In Stage 4, synthesis and characterization of 3D-printable foamed fly ash-based geopolymer matrices for thermal insulation is the focus. A surfactant-based foaming process, multi-step mixing that ensures foam jamming transition and thus a dry foam, and microstructural packing to ensure adequate skeletal density are implemented to develop foamed suspensions amenable to 3D-printing. The last stage of this research develops 3D-printable alkali-activated ground granulated blast furnace slag mixture. Slag is used as the source of aluminosilicate and shows excellent mechanical properties when activated by highly alkaline activator (NaOH + sodium silicate solution). However, alkali activated slag sets and hardens rapidly which is undesirable for 3D printing. Thus, a novel mixing procedure is developed to significantly extend the setting time of slag activated with an alkaline activator to suit 3D printing applications without the use of any retarding admixtures. This dissertation, thus advances the field of sustainable and 3D-printable matrices and opens up a new avenue for faster and economical construction using specialized materials.

Humans are exposed up to thousands of per- and polyfluoroalkyl substances (PFAS) in the environment, but most of the research and action has been directed towards only two PFAS compounds. These two compounds are part of a subcategory of PFAS called perfluoroalkyl acids (PFAAs). It has been a challenge for the environmental community to mitigate risks caused by PFAAs due to their high persistence and lack of effective measures to remove them from the environment, especially in heavily impacted areas like fire-training sites. The goal of this work was to further answer some questions regarding the removal of PFAAs in the environment by looking at anion exchange resin characteristics and presence of a competing compound, natural organic matter (NOM), in the adsorption of environmentally relevant PFAS compounds including the two often monitored 8-carbon chain PFAAs. Two different resins were tested with two forms of counterions, in both groundwater and NOM impacted groundwater. Resin polymer matrix was the most important property in the adsorption of PFAAs, the two resins used A520E and A860 had similar properties except for their matrices polystyrene (PS) and polyacrylic (PA), respectively. The PS base is most effective at PFAAs adsorption, while the PA is most effective at NOM adsorption. The change in the counterion did not negatively affect the adsorption of PFAAs and is, therefore, a viable alternative for future studies that include regeneration and destruction of PFAAs. The presence of NOM also did not significantly affect the adsorption of PFAAs in the PS resin A520E, although for some PFAAs compounds it did affect adsorption for the PA resin. Ultimately, PS macroporous resins with a strong Type I or Type II base work best in PFAAs removal.