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- Genre: Doctoral Dissertation
Description
This dissertation presents a systematic study of the sorption mechanisms of hydrophobic silica aerogel (Cabot Nanogel®) granules for oil and volatile organic compounds (VOCs) in different phases. The performance of Nanogel for removing oil from laboratory synthetic oil-in-water emulsions and real oily wastewater, and VOCs from their aqueous solution, in both packed bed (PB) and inverse fluidized bed (IFB) modes was also investigated. The sorption mechanisms of VOCs in the vapor, pure liquid, and aqueous solution phases, free oil, emulsified oil, and oil from real wastewater on Nanogel were systematically studied via batch kinetics and equilibrium experiments. The VOC results show that the adsorption of vapor is very slow due to the extremely low thermal conductivity of Nanogel. The faster adsorption rates in the liquid and solution phases are controlled by the mass transport, either by capillary flow or by vapor diffusion/adsorption. The oil results show that Nanogel has a very high capacity for adsorption of pure oils. However, the rate for adsorption of oil from an oil-water emulsion on the Nanogel is 5-10 times slower than that for adsorption of pure oils or organics from their aqueous solutions. For an oil-water emulsion, the oil adsorption capacity decreases with an increasing proportion of the surfactant added. An even lower sorption capacity and a slower sorption rate were observed for a real oily wastewater sample due to the high stability and very small droplet size of the wastewater. The performance of Nanogel granules for removing emulsified oil, oil from real oily wastewater, and toluene at low concentrations in both PB and IFB modes was systematically investigated. The hydrodynamics characteristics of the Nanogel granules in an IFB were studied by measuring the pressure drop and bed expansion with superficial water velocity. The density of the Nanogel granules was calculated from the plateau pressure drop of the IFB. The oil/toluene removal efficiency and the capacity of the Nanogel granules in the PB or IFB were also measured experimentally and predicted by two models based on equilibrium and kinetic batch measurements of the Nanogel granules.
ContributorsWang, Ding (Author) / Lin, Jerry Y.S. (Thesis advisor) / Pfeffer, Robert (Thesis advisor) / Westerhoff, Paul (Committee member) / Nielsen, David (Committee member) / Lind, Mary Laura (Committee member) / Arizona State University (Publisher)
Created2011
Description
Of the potential technologies for pre-combustion capture, membranes offer the advantages of being temperature resistant, able to handle large flow rates, and having a relatively small footprint. A significant amount of research has centered on the use of polymeric and microporous inorganic membranes to separate CO2. These membranes, however, have limitations at high temperature resulting in poor permeation performance. To address these limitations, the use of a dense dual-phase membrane has been studied. These membranes are composed of conductive solid and conductive liquid phases that have the ability to selectively permeate CO2 by forming carbonate ions that diffuse through the membrane at high temperature. The driving force for transport through the membrane is a CO2 partial pressure gradient. The membrane provides a theoretically infinite selectivity. To address stability of the ceramic-carbonate dual-phase membrane for CO2 capture at high temperature, the ceramic phase of the membrane was studied and replaced with materials previously shown to be stable in harsh conditions. The permeation properties and stability of La0.6Sr0.4Co0.8Fe0.2O3-δ (LSCF)-carbonate, La0.85Ce0.1Ga0.3Fe0.65Al0.05O3-δ (LCGFA)-carbonate, and Ce0.8Sm0.2O1.9 (SDC)-carbonate membranes were examined under a wide range of experimental conditions at high temperature. LSCF-carbonate membranes were shown to be unstable without the presence of O2 due to reaction of CO2 with the ceramic phase. In the presence of O2, however, the membranes showed stable permeation behavior for more than one month at 900oC. LCGFA-carbonate membranes showed great chemical and permeation stability in the presence of various conditions including exposure to CH4 and H2, however, the permeation performance was quite low when compared to membranes in the literature. Finally, SDC-carbonate membranes showed great chemical and permeation stability both in a CO2:N2 environment for more than two weeks at 900oC as well as more than one month of exposure to simulated syngas conditions at 700oC. Ceramic phase chemical stability increased in the order of LSCF < LCGFA < SDC while permeation performance increased in the order of LCGFA < LSCF < SDC.
ContributorsNorton, Tyler (Author) / Lin, Jerry Y.S. (Thesis advisor) / Alford, Terry (Committee member) / Lind, Mary Laura (Committee member) / Smith, David (Committee member) / Torres, Cesar (Committee member) / Arizona State University (Publisher)
Created2013
Description
Membrane based technology is one of the principal methods currently in widespread use to address the global water shortage. Pervaporation desalination is a membrane technology for water purification currently under investigation as a method for processing reverse osmosis concentrates or for stand-alone applications. Concentration polarization is a potential problem in any membrane separation. In desalination concentration polarization can lead to reduced water flux, increased propensity for membrane scaling, and decreased quality of the product water. Quantifying concentration polarization is important because reducing concentration polarization requires increased capital and operating costs in the form of feed spacers and high feed flow velocities. The prevalent methods for quantifying concentration polarization are based on the steady state thin film boundary layer theory. Baker’s method, previously used for pervaporation volatile organic compound separations but not desalination, was successfully applied to data from five previously published pervaporation desalination studies. Further investigation suggests that Baker’s method may not have wide applicability in desalination. Instead, the limitations of the steady state assumption were exposed. Additionally, preliminary results of nanophotonic enhancement of pervaporation membranes were found to produce significant flux enhancement. A novel theory on the mitigation of concentration polarization by the photothermal effect was discussed.
ContributorsMann, Stewart, Ph.D (Author) / Lind, Mary Laura (Thesis advisor) / Walker, Shane (Committee member) / Green, Matthew (Committee member) / Forzani, Erica (Committee member) / Emady, Heather (Committee member) / Arizona State University (Publisher)
Created2019
Description
Existing water quality sensors in surface, environmental, and drinking water systems are not well suited for long-term, scalable use as they require calibration, replacement of reagents, and are subject to biofouling which degrades measurement accuracy. Microbial Potentiometric Sensors (MPSs) offer an alternative approach to water quality monitoring by monitoring a biofilm-mediated potentiometric response to diverse water quality parameters. MPS biofilms grow naturally on graphite electrodes in diverse aqueous systems, are regenerative, and their potentiometric response correlates with numerous water quality parameters. As such, the overarching hypothesis of this dissertation is that MPS signal can be used to assess water quality trends and that its signal is driven by biofilm vitality. To test this hypothesis, machine learning, statistical regression, and the use of more complex, impedimetric measurement techniques were explored to characterize water quality trends in diverse water systems. This was accomplished by completing three dissertation objectives: 1.) Assess whether Machine Learning/Artificial Intelligence (ML/AI) tools can be used to disaggregate various surface water quality parameter values from Open Circuit Potential (OCP) signals produced by MPSs; 2.) Determine whether residual free chlorine concentration in drinking water could be determined by monitoring MPSs; and 3.) Determine whether OCP and/or Electrochemical Impedance Spectroscopy (EIS)-derived impedance data from an MPS can be used to determine water quality trends while confirming its biological origins. The findings confirm the hypothesis by demonstrating that ML/AI can be used to disaggregate MPS signal and determine numerous water quality parameters, offering unique opportunities for real-time monitoring of aqueous environments. Additionally, MPSs are particularly useful in measuring free chlorine concentrations in drinking water distribution systems which offers opportunities for scalable, in-situ, continuous monitoring of chlorine throughout a distribution network. Finally, the findings demonstrate that coupling MPSs’ OCP signal with more advanced measurement techniques such as EIS can improve understanding of drinking water quality trends, however current open source, affordable technologies capable of conducting EIS are prone to high measurement noise and are not currently accurate enough to be used in drinking water systems.
ContributorsSaboe, Daniel (Author) / Hristovski, Kiril (Thesis advisor) / Olson, Larry (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2022
Description
Water quality assessment is essential for maintaining healthy ecosystems and protecting human health. Data interrogation and exploratory data analysis techniques are used to analyze the spatial and temporal variability of water quality parameters, identifying correlations, and to better understand the factors that impacts microbial and chemical quality of water. The seasonal dynamics of microbiome in surface waters were investigated to identify the factors driving these dynamics. Initial investigation analyzed two decades of regional water quality data from 20 various locations in Central Arizona, USA. Leveraging advanced data science techniques, the study uncovered correlations between crucial parameters, including dissolved organic carbon (DOC), ultraviolet absorbance (UVA), and specific ultraviolet absorbance (SUVA). These findings provide foundational insights into the dynamic of overall water quality. A comprehensive 12-month surface water sample collection and study was conducted to investigate potential bias in bacterial detection using EPA approved Membrane Filtration (MF) technique. The results underscore that while MF excels in recovering bacteria of public health significance, it exhibits biases, particularly against small and spore-forming bacteria and Archaea, such as Bacilli, Mollicutes, Methylacidiphilae, and Parvarchaea. This emphasizes the importance of complementing standard microbiology approaches to mitigate technological biases and enhance the accuracy of microbial water quality testing, especially for emerging pathogens. Furthermore, a complementary study of microbial dynamics within a model drinking water distribution systems (DWDSs) using treated water from the same source water as the above study. The influence of pipe material and water temperature on the microbiome and trace element composition was investigated. The research unveiled a preferential link between pipe material and trace elements, with water temperature significantly impacting the microbiome to a higher degree than the chemical composition of water. Notably, Legionellaceae and Mycobacteriaceae were found to be prevalent in warmer waters, highlighting the substantial influence of water temperature on the microbiome, surpassing that of pipe material. These studies provide comprehensive insights into the spatial and temporal variability of water quality parameters. Analyzing microbial data in depth is crucial in detecting bacterial species within a monitoring program for adjusting operational conditions to reduce the presence of microbial pathogens and enhance the quality of drinking water.
ContributorsAloraini, Saleh (Author) / Abbaszadegan, Morteza (Thesis advisor) / Fox, Peter (Committee member) / Perreault, Francois (Committee member) / Alum, Absar (Committee member) / Arizona State University (Publisher)
Created2023
Description
Glasses have many applications such as containers, substrates of displays, high strength fibers and portable electronic display panels. Their excellent mechanical properties such as high hardness, good forming ability and scratch resistance make glasses ideal for these applications. Many factors affect the selection of one glass over another for a given purpose such as cost, ingredients, scalability of manufacturing, etc. Typically, silicate based glasses are often selected because they satisfy most of the selection criteria. However, with the recent abundant use of these glasses in touch-based applications, understanding their abilities to dissipate energy due to surface contact loads has become increasingly desirable. The most common silicate glasses worldwide are glassy silica and soda lime. Calcium aluminosilicates are also gaining popularity due to their importance as substrates for display screens in electronic devices. The surface energy dissipation and strength of these glasses are based on several factors, but predominantly rely on ingredient composition and the so-called Indentation Size Effect (ISE), where the strength depends on the maximum surface force. Both the composition and ISE alter the strength and favored energy dissipation mechanisms of the glass. Unlocking the contribution of these mechanisms and elucidating their dependence on composition and force is the underlining goal of this thesis.Prior to cracking, silicate glasses can inelastically deform by shear and densification. However, the link between the mechanical properties, strength, glass structure and maximum force and the propensity by which either of these mechanisms are favored still remains unclear. In this study, the first aim is to elucidate the causes of the ISE and
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explore the relationships between the ISE and the dissipation mechanisms, and identify what feature(s) of the glass can be used to infer their behavior. All glasses have shown a strong link between the ISE and shear flow and densification. Second, the link between composition and the dissipation mechanisms will be elucidated. This is accomplished by performing indentation tests coupled with an annealing method to independently quantify the amount of volume associated with each dissipation mechanism and elucidate relationships with ingredients and structure of the glasses. Some conclusions will then be presented that link all these behaviors together.
ContributorsKazembeyki, Maryam (Author) / Hoover, Christian G (Thesis advisor) / Rajan, Subramaniam (Committee member) / Neithalath, Narayanan (Committee member) / Chawla, Nikhilesh (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2021
Description
Pervaporation is a membrane process suited to complex and highly contaminated wastewaters. Pervaporation desalination is an emerging area of study where the development of high-performance membranes is necessary to propel the field forward. This research demonstrated that sulfonated block polymer membranes (Nexar™)show excellent permeance (water passage normalized by driving force) of as much as 135.5 ± 29 kg m-2 hr-1 bar-1, with salt removal values consistently equal to or greater than 99.5%. Another challenging water management scenario is in spaceflight situations, such as on the International Space Station (ISS). Spaceflight wastewaters are highly complex, with low pH values, and high levels of contaminants. Current processes produce 70% wastewater recovery, necessitating the handling and processing of concentrated brines. Since recoveries of 85% are desired moving forward, further efforts in water recovery are desirable. An area of concern in these ISS water treatment systems is scalant deposition, especially of divalent ions such as calcium species. Zwitterions are molecules with localized positive and negative charges, but an overall neutral charge. Zwitterions have been used to modify the surface of membranes have shown to decrease fouling. Building a copolymer between zwitterions and other polymers, creates zwitterion layer on top of previously studied Nexar™ membranes. This coating demonstrates great promise to combat scaling, as it increases the hydrophilicity of the membrane surface measured via contact angle. The zwitterion membranes experienced reduced scaling, with the greatest difference being between 1617 ± 241 wt% on control membranes, to 317 ± 87 wt% on zwitterion coated membranes in the presence of CaCl2. In treating spaceflight wastewater, these zwitterion membranes are effective at retaining the acid in the feed, going from a pH value of 2 to 7 and reducing the contamination level of the feed, with a removal value of 99.3 ± 0.4%, measured through conductivity. These membranes also perform well in separation processes that do not require extreme vacuum and can be operated passively. By optimizing both membrane material properties and process conditions, achieving increased high levels of water recovery from spaceflight wastewaters is attainable.
ContributorsThomas, Elisabeth (Author) / Lind, Mary Laura (Thesis advisor) / Forzani, Erica (Committee member) / Perreault, Francois (Committee member) / Walker, W. Shane (Committee member) / Williamson, Jill P (Committee member) / Arizona State University (Publisher)
Created2023
Description
Freshwater as the resource for the survival of humans and all lives on earth is very precious but scarce. The shortage of the original freshwater resources and the interfering activities by human and other natural factors form this issue together. To reduce the water supply pressure and deterioration of freshwater systems (for example, river, wetland, and groundwater), the quantity-increase and the quality-increase strategies should be implemented at the same time. Therefore, corresponding membrane technologies have been developed to achieve water purification with high efficiency and low cost. For desalinating seawater and other types of saline water, pervaporation has been proved that has the potential to complete desalination with salt rejection rate over 99 % when dealing with high salinity water that reverse osmosis (RO) cannot handle. In this dissertation, except the discussion of commonly used materials to synthesize pervaporation membranes, two types of novel pervaporation desalination membranes (nanophotonic-enhanced membrane and free-standing sulfonated membrane) have been presented and discussed. The novel membranes were tested to see the potential of pervaporation to desalinate seawater and saline water with more complex ionic composition, and the possibility of achieving zero liquid discharge in the desalination field when having pervaporation as the assistance. For mitigating polluted water that is caused by human activities, especially agricultural activities, electrodialysis is an effective method to remove specific ions from water, and it does not require extra chemical cost or regeneration. A type of anion exchange membranes inspired by ion exchange resins was synthesized and tested, and the performance on nitrate removal has been evaluated in this dissertation.
ContributorsLi, Yusi (Author) / Lind, Mary Laura (Thesis advisor) / Perreault, Francois (Thesis advisor) / Forzani, Erica (Committee member) / Seo, S. Eileen (Committee member) / Walker, W. Shane (Committee member) / Arizona State University (Publisher)
Created2023
Description
Electrochemical technologies emerge as a feasible solution to monitor and treat pollutants. Although electrochemical technologies have garnered widespread attention, their commercial applications are still constrained by the use of expensive electrocatalysts, and the bulky and rigid plate design of electrodes that restricts electrochemical reactor design to systems with poor electrode surface/ volume treated ratios. By making electrodes flexible, more compact designs that maximize electrode surface per volume treated might become a reality. This dissertation encompasses the successful fabrication of flexible nanocomposite electrodes for electrocatalysis and electroanalysis applications.First, nano boron-doped diamond electrodes (BDD) were prepared as an inexpensive alternative to commercial boron-doped diamond electrodes. Comparative detailed surface and electrochemical characterization was conducted. Empirical study showed that replacing commercial BDD electrodes with nano-BDD electrodes can result in a cost reduction of roughly 1000x while maintaining the same electrochemical performance.
Next, self-standing electrodes were fabricated through the electropolymerization of conducing polymer, polypyrrole. Surface characterizations, such as SEM, FTIR and XPS proved the successful fabrication of these self-standing electrodes. High mechanical stability and bending flexibility demonstrated the ability to use these electrodes in different designs, such as roll-to-roll membranes. Electrochemical nitrite reduction was employed to demonstrate the viability of using self-standing nanocomposite electrodes for electrocatalytic applications reducing hazardous nitrogen oxyanions (i.e., nitrite) towards innocuous species such as nitrogen gas. A high faradaic efficiency of 78% was achieved, with high selectivity of 91% towards nitrogen gas.
To further enhance the conductivity and charge transfer properties of self-standing polypyrrole electrodes, three different nanoparticles, including copper (Cu), gold (Au), and platinum (Pt), were incorporated in the polypyrrole matrix. Effect of nanoparticle wt% and interaction between metal nanoparticles and polypyrrole matrix was investigated for electroanalytical applications, specifically dopamine sensing. Flexible nanocomposite electrodes showed outstanding performance as electrochemical sensors with PPy-Cu 120s exhibiting a low limit of detection (LOD) of 1.19 µM and PPy-Au 120s exhibiting a high linear range of 5 µM - 300 µM.
This dissertation outlines a method of fabricating self-standing electrodes and provides a pathway of using self-standing electrodes based on polypyrrole and polypyrrole-metal nanocomposites for various applications in wastewater treatment and electroanalytical sensing.
ContributorsBansal, Rishabh (Author) / Garcia-Segura, Sergio (Thesis advisor) / Westerhoff, Paul (Committee member) / Perreault, Francois (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2023
Description
Nitrate leaching from agricultural systems poses a threat to ecosystems and human health. Integrating 2D carbon-based graphite nano additive (GNA) soil amendments previously demonstrated potential in mitigating nitrate loss, yet the responsible mechanism was unclear. To clarify the causal mechanism, this dissertation aimed to identify and understand mechanisms of how addition of graphite nano-additive (GNA) soil amendment reduces N leaching through agricultural soil by sequential investigation employing laboratory soil incubation tests, batch adsorption experiments, soil column experiments, and greenhouse pot study. Soil incubation tests were conducted with four commercially available graphene nanomaterials to establish that soil microbial activity indicated by respiration was significantly enhanced when soil was amended with graphene (e.g., GNA). Additionally, gene abundance assessment from the same incubation tests indicated a potentially slowed soil nitrification (ammonium to nitrate conversion) by GNA. Separate batch absorption tests indicated that GNA was unlikely to retain nitrate through adsorption. Soil column experiments were designed to probe the dependency of N retention in GNA-amended soil primarily due to altered microbial activity from assessing the impact of temperature, soil saturation, sterility, hydraulic retention time, GNA dose, and soil organic carbon. Finally, a greenhouse plant growth study was designed to assess how GNA impacts soil biology. Enzyme activity indicated GNA could stimulate soil carbon mineralization and improve soil bioavailable carbon. Gene abundance assessment showed total bacterial community size was unimpacted but selected and suppressed certain bacterial groups (e.g., suppressed bacterial amoA gene abundance).16S bacterial community sequencing showed that GNA significantly altered the bulk and rhizosphere soil microbiome composition. GNA-induced selection of certain bacterial classes (e.g., Bacilli) holds significant implications in aspects of plant growth and nutrient acquisition. This dissertation revealed mechanisms behind GNA-induced decrease of nitrate leaching in agricultural soil, aiding progress to its integration into conventional agriculture to improve nitrogen fertilizer efficiency for a food-secure future.
ContributorsDas, Partho (Author) / Westerhoff, Paul (Thesis advisor) / Penton, Christopher Ryan (Committee member) / Perreault, Francois (Committee member) / Arizona State University (Publisher)
Created2024