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Drinking water filtration using reverse osmosis (RO) membranes effectively removes salts and most other inorganic, organic, and microbial pollutants. RO technologies are utilized at both the municipal and residential scale. The formation of biofilms on RO membranes reduces water flux and increases energy consumption. The research conducted for this thesis

Drinking water filtration using reverse osmosis (RO) membranes effectively removes salts and most other inorganic, organic, and microbial pollutants. RO technologies are utilized at both the municipal and residential scale. The formation of biofilms on RO membranes reduces water flux and increases energy consumption. The research conducted for this thesis involves In-Situ coating of silver, a known biocide, on the surface of RO membranes. This research was adapted from a protocol developed for coating flat sheet membranes with silver nanoparticles, and scaled up into spiral-wound membranes that are commonly used at the residential scale in point-of-use (POU) filtration systems. Performance analyses of the silver-coated spiral-wound were conducted in a mobile drinking water treatment system fitted with two POU units for comparison. Five month-long analyses were performed, including a deployment of the mobile system. In addition to flux, salt rejection, and other water quality analyses, additional membrane characterization tests were conducted on pristine and silver-coated membranes.

For flat sheet membranes coated with silver, the surface charge remained negative and contact angle remained below 90. Scaling up to spiral-wound RO membrane configuration was successful, with an average silver-loading of 1.93 g-Ag/cm2. Results showed the flux of water through the membrane ranged from 8 to 13 liters/m2*hr. (LMH) operating at 25% recovery during long-term of operation. The flux was initially decreased due to the silver coating, but no statistically significant differences were observed after 14 days of operation (P < 0.05). The salt rejection was also not effected due to the silver coating (P < 0.05). While 98% of silver was released during long-term studies, the silver release from the spiral-wound membrane was consistently below the secondary MCL of 100 ppb established by the EPA, and was consistently below 5 ppb after two hours of operation. Microbial assays in the form of heterotrophic plate counts suggested there was no statistically significant difference in the prevention of biofouling formation due to the silver coating (P < 0.05). In addition to performance tests and membrane characterizations, a remote data acquisition system was configured to remotely monitor performance and water quality parameters in the mobile system.
ContributorsZimmerman, Sean (Author) / Westerhoff, Paul K (Thesis advisor) / Sinha, Shahnawaz (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2017
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Description
With the application of reverse osmosis (RO) membranes in the wastewater treatment and seawater desalination, the limitation of flux and fouling problems of RO have gained more attention from researchers. Because of the tunable structure and physicochemical properties of nanomaterials, it is a suitable material that can be used to

With the application of reverse osmosis (RO) membranes in the wastewater treatment and seawater desalination, the limitation of flux and fouling problems of RO have gained more attention from researchers. Because of the tunable structure and physicochemical properties of nanomaterials, it is a suitable material that can be used to incorporate with RO to change the membrane performances. Silver is biocidal, which has been used in a variety of consumer products. Recent studies showed that fabricating silver nanoparticles (AgNPs) on membrane surfaces can mitigate the biofouling problem on the membrane. Studies have shown that Ag released from the membrane in the form of either Ag ions or AgNP will accelerate the antimicrobial activity of the membrane. However, the silver release from the membrane will lower the silver loading on the membrane, which will eventually shorten the antimicrobial activity lifetime of the membrane. Therefore, the silver leaching amount is a crucial parameter that needs to be determined for every type of Ag composite membrane.

This study is attempting to compare four different silver leaching test methods, to study the silver leaching potential of the silver impregnated membranes, conducting the advantages and disadvantages of the leaching methods. An In-situ reduction Ag loaded RO membrane was examined in this study. A custom waterjet test was established to create a high-velocity water flow to test the silver leaching from the nanocomposite membrane in a relative extreme environment. The batch leaching test was examined as the most common leaching test method for the silver composite membrane. The cross-flow filtration and dead-end test were also examined to compare the silver leaching amounts.

The silver coated membrane used in this experiment has an initial silver loading of 2.0± 0.51 ug/cm2. The mass balance was conducted for all of the leaching tests. For the batch test, water jet test, and dead-end filtration, the mass balances are all within 100±25%, which is acceptable in this experiment because of the variance of the initial silver loading on the membranes. A bad silver mass balance was observed at cross-flow filtration. Both of AgNP and Ag ions leached in the solution was examined in this experiment. The concentration of total silver leaching into solutions from the four leaching tests are all below the Secondary Drinking Water Standard for silver which is 100 ppb. The cross-flow test is the most aggressive leaching method, which has more than 80% of silver leached from the membrane after 50 hours of the test. The water jet (54 ± 6.9% of silver remaining) can cause higher silver leaching than batch test (85 ± 1.2% of silver remaining) in one-hour, and it can also cause both AgNP and Ag ions leaching from the membrane, which is closer to the leaching condition in the cross-flow test.
ContributorsHan, Bingru (Author) / Westerhoff, Paul (Thesis advisor) / Perreault, Francois (Committee member) / Sinha, Shahnawaz (Committee member) / Arizona State University (Publisher)
Created2017
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Description
Electrospinning is a means of fabricating micron-scale diameter fiber networks with enmeshed nanomaterials. Polymeric nanocomposites for water treatment require the manipulation of fiber morphology to expose nanomaterial surface area while anchoring the nanomaterials and maintaining fiber integrity; that is the overarching goal of this dissertation. The first investigation studied the

Electrospinning is a means of fabricating micron-scale diameter fiber networks with enmeshed nanomaterials. Polymeric nanocomposites for water treatment require the manipulation of fiber morphology to expose nanomaterial surface area while anchoring the nanomaterials and maintaining fiber integrity; that is the overarching goal of this dissertation. The first investigation studied the effect of metal oxide nanomaterial loadings on electrospinning process parameters such as critical voltage, viscosity, fiber diameter, and nanomaterial distribution. Increases in nanomaterial loading below 5% (w/v) were not found to affect critical voltage or fiber diameter. Nanomaterial dispersion was conserved throughout the process. Arsenic adsorption tests determined that the fibers were non-porous. Next, the morphologies of fibers made with carbonaceous materials and the effect of final fiber assembly on adsorption kinetics of a model organic contaminant (phenanthrene, PNT) was investigated. Superfine powdered activated carbon (SPAC), C60 fullerenes, multi-walled carbon nanotubes, and graphene platelets were added to PS and electrospun. SPAC maintained its internal pore structure and created porous fibers which had 30% greater PNT sorption than PS alone and a sevenfold increase in surface area. Carbon-based nanomaterial-PS fibers were thicker but less capacious than neat polystyrene electrospun fibers. The surface areas of the carbonaceous nanomaterial-polystyrene composites decreased compared to neat PS, and PNT adsorption experiments yielded decreased capacity for two out of three carbonaceous nanomaterials. Finally, the morphology and arsenic adsorption capacity of a porous TiO2-PS porous fiber was investigated. Porous fiber was made using polyvinylpyrrolidone (PVP) as a porogen. PVP, PS, and TiO2 were co-spun and the PVP was subsequently eliminated, leaving behind a porous fiber morphology which increased the surface area of the fiber sevenfold and exposed the nanoscale TiO2 enmeshed inside the PS. TiO2-PS fibers had comparable arsenic adsorption performance to non-embedded TiO2 despite containing less TiO2 mass. The use of a sacrificial polymer as a porogen facilitates the creation of a fiber morphology which provides access points between the target pollutant in an aqueous matrix and the sorptive nanomaterials enmeshed inside the fiber while anchoring the nanomaterials, thus preventing release.
ContributorsHoogesteijn von Reitzenstein, Natalia Virginia (Author) / Westerhoff, Paul (Thesis advisor) / Hristovski, Kiril (Committee member) / Perreault, Francois (Committee member) / Herckes, Pierre (Committee member) / Arizona State University (Publisher)
Created2018
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Description
C.C. Cragin Reservoir’s location in the Coconino National Forest, Arizona makes it prone to wild fire. This study focused on the potential impacts of such a wild fire on the reservoir’s annual thermal stratification cycle impacts and water quality. The annual thermal stratification cycle impacted the reservoir’s water

C.C. Cragin Reservoir’s location in the Coconino National Forest, Arizona makes it prone to wild fire. This study focused on the potential impacts of such a wild fire on the reservoir’s annual thermal stratification cycle impacts and water quality. The annual thermal stratification cycle impacted the reservoir’s water quality by increasing hypolimnion concentrations of magnesium, iron, turbidity, and specific ultraviolet absorbance (SUVA) values, as well as resulting in the hypolimnion having decreased dissolved oxygen concentrations during stratified months. The scarification process did not affect the dissolved organic carbon (DOC) concentrations in the reservoir or the total/dissolved nitrogen and phosphorous concentrations. Some general water quality trends that emerged were that phosphorous was the limiting nutrient, secchi disk depth and chlorophyll a concentration are inversely related, and no metals were found to be in concentrations that would violate an EPA drinking water maximum contaminant level (MCL). A carbon mass model was developed and parameterized using DOC measurements, and then using historic reservoir storage and weather data, the model simulated DOC concentrations in the reservoir following four hypothetical wild fire events. The model simulated varying initial reservoir storage volumes, initial flush volumes, and flush DOC concentrations, resulting in reservoir DOC concentrations varying from 17.41 mg/L to 8.82 mg/L.
ContributorsFlatebo, Theodore (Author) / Westerhoff, Paul K (Thesis advisor) / Fox, Peter (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2018
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Description
This report analyzes the potential for accumulation of boron in direct potable reuse. Direct potable reuse treats water through desalination processes such as reverse osmosis or nanofiltration which can achieve rejection rates of salts sometimes above 90%. However, boron achieves much lower rejection rates near 40%. Because of this low

This report analyzes the potential for accumulation of boron in direct potable reuse. Direct potable reuse treats water through desalination processes such as reverse osmosis or nanofiltration which can achieve rejection rates of salts sometimes above 90%. However, boron achieves much lower rejection rates near 40%. Because of this low rejection rate, there is potential for boron to accumulate in the system to levels that are not recommended for potable human consumption of water. To analyze this issue a code was created that runs a steady state system that tracks the internal concentration, permeate concentration, wastewater concentration and reject concentration at various rejection rates, as well as all the flows. A series of flow and mass balances were performed through five different control volumes that denoted different stages in the water use. First was mixing of clean water with permeate; second, consumptive uses; third, addition of contaminant; fourth, wastewater treatment; fifth, advanced water treatments. The system cycled through each of these a number of times until steady state was reached. Utilities or cities considering employing direct potable reuse could utilize this model by estimating their consumption levels and input of contamination, and then seeing what percent rejection or inflow of makeup water they would need to obtain to keep boron levels at a low enough concentration to be fit for consumption. This code also provides options for analyzing spikes and recovery in the system due to spills, and evaporative uses such as cooling towers and their impact on the system.
ContributorsDoidge, Sydney (Author) / Fox, Peter (Thesis director) / Perreault, Francois (Committee member) / Civil, Environmental and Sustainable Engineering Program (Contributor) / School of International Letters and Cultures (Contributor) / Barrett, The Honors College (Contributor)
Created2017-12
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Description
The purpose of this research was to produce reduced graphene oxides for the fabrication of desalination membranes. Graphene has typically been considered a way to create more energy efficient desalination membranes. However, graphene is expensive and unstable, while graphene oxide has similar properties, but is less expensive and

The purpose of this research was to produce reduced graphene oxides for the fabrication of desalination membranes. Graphene has typically been considered a way to create more energy efficient desalination membranes. However, graphene is expensive and unstable, while graphene oxide has similar properties, but is less expensive and more stable. Graphene oxide membranes have the potential to perform above the permeability-selectivity tradeoff that is typical in membranes through size-based exclusion. Reduction through heat or Vitamin C reduces the size of graphene oxide nanochannels so salt and organic materials can be rejected in higher numbers. Both reduced and unreduced graphene oxide membranes were created and evaluated by their ability to filter dye and salt in a pressurized membrane cell. The permeability and rejection of the graphene oxide membrane is found to be dependent on the oxidation level of the graphene oxide material and the concentration on the graphene oxide on the membrane. Unreduced graphene oxide membranes were created in three concentrations: 7.37, 14.74, and 29.47 μg/cm2. As graphene oxide concentration increased, dye rejection and salt rejection increased, while water flux decreased. Graphene oxide was reduced in solution using Vitamin C and was used to create a 14.74 μg/cm2 membrane. The reduction resulted in an increase in salt rejection from 12.59% to 100%, an increase in dye rejection from 30.44% to 100%, and a decrease in water flux from 9.502 to 0.198 L/(hr*m2*bar). Future research should focus on creating membranes using different methods of synthesizing graphene oxide from graphene and creating a reduced graphene oxide membrane with a higher water flux.
Created2017-12
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Description
As selenium is toxic at low levels, treatment methods to remove selenium from industrial waste waters are needed. In this work, three groups of sorbent materials were investigated in detail for their effectiveness for selenium and arsenic removal from water: 1) nanostructured carbon-based materials, 2) layered double hydroxide (LDH)-based materials,

As selenium is toxic at low levels, treatment methods to remove selenium from industrial waste waters are needed. In this work, three groups of sorbent materials were investigated in detail for their effectiveness for selenium and arsenic removal from water: 1) nanostructured carbon-based materials, 2) layered double hydroxide (LDH)-based materials, and 3) biopolymer-based sorbents. The materials were investigated in spiked de-ionized water and waters collected from different locations at Salt River Project’s (SRP) Santan Generating Station in Gilbert, AZ. The results show that nanostructured carbon-based materials removed ~80% and up to 100% selenium and arsenic, respectively in spiked DI water. Heat treated layered double hydroxides removed close to 100% removal in selenium and arsenic spiked DI water. Isotherms conducted in spiked DI water fit the Langmuir model and showed a maximum selenate adsorption capacity of 67 mg/g for the calcined LDH powder. Results from SRP waters showed that certain LDH sorbents were effective for removing the selenium, but that higher pH and existence of competing ions affected the removal efficiencies. The functionalized biopolymer sorbent from Crystal Clear Technologies: CCT-149/OCI-B showed good removal efficiencies for both selenate and selenite in DI water. Isotherms conducted in spiked DI water for CCT-149 fit the Langmuir model and showed a maximum selenate adsorption capacity of 90.9 mg/g. Column tests using spiked DI water and waters obtained from SRP wells were investigated using both LDH and CCT-149/OCI-B. Removal of sulfate using chemical pre-treatment of the water with barium chloride resulted in about three times higher selenate loading onto the granular LDH and doubled the water volume that can be treated using CCT-149/OCI-B. The results from the column tests are being used to guide the pilot testing investigating the implementation of LDH sorbents at pilot scale at the Santan plant. The good results in the cooling tower #5 blowdown water and combined discharge waste water of SRP provide valuable information about the efficacy and efficiency of adsorptive media for the removal of selenium. Composites comprising LDH nanosheets with different substrates were successfully synthesized that were able to retain the performance in removing selenate of nanosheet LDH.
ContributorsLi, Man (Author) / Chan, Candace (Thesis advisor) / Lind, Mary Laura (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2017
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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
Reverse osmosis (RO) membranes are considered the most effective treatment to remove salt from water. Specifically, thin film composite (TFC) membranes are considered the gold standard for RO. Despite TFC membranes good performance, there are drawbacks to consider including: permeability-selectivity tradeoff, chlorine damage, and biofouling potential. In order to counter

Reverse osmosis (RO) membranes are considered the most effective treatment to remove salt from water. Specifically, thin film composite (TFC) membranes are considered the gold standard for RO. Despite TFC membranes good performance, there are drawbacks to consider including: permeability-selectivity tradeoff, chlorine damage, and biofouling potential. In order to counter these drawbacks, polyamide matrixes were embedded with various nanomaterials called mixed matrix membranes (MMMs) or thin film nanocomposites (TFNs). This research investigates the use of graphene oxide (GO) and reduced graphene oxide (RGO) into the polyamide matrix of a TFC membrane. GO and RGO have the potential to alter the permeability-selectivity trade off by offering nanochannels for water molecules to sieve through, protect polyamide from trace amounts of chlorine, as well as increase the hydrophilicity of the membrane thereby reducing biofouling potential. This project focuses on the impacts of GO on the permeability selectivity tradeoff. The hypothesis of this work is that the permeability and selectivity of GO can be tuned by controlling the oxidation level of the material. To test this hypothesis, a range of GO materials were produced in the lab using different graphite oxidation methods. The synthesized GOs were characterized by X-ray diffraction and X-ray photoelectron microscopy to show that the spacing is a function of the GO oxygen content. From these materials, two were selected due to their optimal sheet spacing between 3.4 and 7 angstroms and embedded into desalination MMM. This work reveals that the water permeability coefficient of MMM embedded with GO and RGO increased significantly; however, that the salt permeability coefficient of the membrane also increased. Future research directions are proposed to overcome this limitation.
ContributorsInurria, Adam A (Author) / Perreault, Francois (Thesis advisor) / Fox, Peter (Thesis advisor) / Lind, Mary Laura (Committee member) / Arizona State University (Publisher)
Created2017
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Description
Bacteriophage provide high specificity to bacteria; receiving interest in various applications and have been used as target recognition tools in designing bioactive surfaces. Several current immobilization strategies to detect and capture bacteriophage require non-deliverable bioactive substrates or modifying the chemistry of the phage, procedures that are labor intensive and can

Bacteriophage provide high specificity to bacteria; receiving interest in various applications and have been used as target recognition tools in designing bioactive surfaces. Several current immobilization strategies to detect and capture bacteriophage require non-deliverable bioactive substrates or modifying the chemistry of the phage, procedures that are labor intensive and can damage the integrity of the virus. The aim of this research was to develop the framework to physisorb and chemisorb T4 coliphage on varied sized functionalized silica particles while retaining its infectivity. First, silica surface modification, silanization, altered pristine silica colloids to positively, amine coated silica. The phages remain infective to their host bacteria while adsorbed on the surface of the silica particles. It is reported that the number of infective phage bound to the silica is enhanced by the immobilization method. It was determined that covalent attachment yielded 106 PFU/ml while electrostatic attachment resulted in 105 PFU/ml.
ContributorsBone, Stephanie (Author) / Perreault, Francois (Thesis advisor) / Alum, Absar (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2017