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- All Subjects: engineering
- All Subjects: nanotechnology
- Creators: Tamizhmani, Govindasamy
- Status: Published
Description
Nitrate is the most prevalent water pollutant limiting the use of groundwater as a potable water source. The overarching goal of this dissertation was to leverage advances in nanotechnology to improve nitrate photocatalysis and transition treatment to the full-scale. The research objectives were to (1) examine commercial and synthesized photocatalysts, (2) determine the effect of water quality parameters (e.g., pH), (3) conduct responsible engineering by ensuring detection methods were in place for novel materials, and (4) develop a conceptual framework for designing nitrate-specific photocatalysts. The key issues for implementing photocatalysis for nitrate drinking water treatment were efficient nitrate removal at neutral pH and by-product selectivity toward nitrogen gases, rather than by-products that pose a human health concern (e.g., nitrite). Photocatalytic nitrate reduction was found to follow a series of proton-coupled electron transfers. The nitrate reduction rate was limited by the electron-hole recombination rate, and the addition of an electron donor (e.g., formate) was necessary to reduce the recombination rate and achieve efficient nitrate removal. Nano-sized photocatalysts with high surface areas mitigated the negative effects of competing aqueous anions. The key water quality parameter impacting by-product selectivity was pH. For pH < 4, the by-product selectivity was mostly N-gas with some NH4+, but this shifted to NO2- above pH = 4, which suggests the need for proton localization to move beyond NO2-. Co-catalysts that form a Schottky barrier, allowing for localization of electrons, were best for nitrate reduction. Silver was optimal in heterogeneous systems because of its ability to improve nitrate reduction activity and N-gas by-product selectivity, and graphene was optimal in two-electrode systems because of its ability to shuttle electrons to the working electrode. "Environmentally responsible use of nanomaterials" is to ensure that detection methods are in place for the nanomaterials tested. While methods exist for the metals and metal oxides examined, there are currently none for carbon nanotubes (CNTs) and graphene. Acknowledging that risk assessment encompasses dose-response and exposure, new analytical methods were developed for extracting and detecting CNTs and graphene in complex organic environmental (e.g., urban air) and biological matrices (e.g. rat lungs).
ContributorsDoudrick, Kyle (Author) / Westerhoff, Paul (Thesis advisor) / Halden, Rolf (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2013
Description
The object of this study was a 26 year old residential Photovoltaic (PV) monocrystalline silicon (c-Si) power plant, called Solar One, built by developer John F. Long in Phoenix, Arizona (a hot-dry field condition). The task for Arizona State University Photovoltaic Reliability Laboratory (ASU-PRL) graduate students was to evaluate the power plant through visual inspection, electrical performance, and infrared thermography. The purpose of this evaluation was to measure and understand the extent of degradation to the system along with the identification of the failure modes in this hot-dry climatic condition. This 4000 module bipolar system was originally installed with a 200 kW DC output of PV array (17 degree fixed tilt) and an AC output of 175 kVA. The system was shown to degrade approximately at a rate of 2.3% per year with no apparent potential induced degradation (PID) effect. The power plant is made of two arrays, the north array and the south array. Due to a limited time frame to execute this large project, this work was performed by two masters students (Jonathan Belmont and Kolapo Olakonu) and the test results are presented in two masters theses. This thesis presents the results obtained on the north array and the other thesis presents the results obtained on the south array. The resulting study showed that PV module design, array configuration, vandalism, installation methods and Arizona environmental conditions have had an effect on this system's longevity and reliability. Ultimately, encapsulation browning, higher series resistance (potentially due to solder bond fatigue) and non-cell interconnect ribbon breakages outside the modules were determined to be the primary causes for the power loss.
ContributorsBelmont, Jonathan (Author) / Tamizhmani, Govindasamy (Thesis advisor) / Henderson, Mark (Committee member) / Rogers, Bradley (Committee member) / Arizona State University (Publisher)
Created2013
Description
Potential induced degradation (PID) due to high system voltages is one of the major degradation mechanisms in photovoltaic (PV) modules, adversely affecting their performance due to the combined effects of the following factors: system voltage, superstrate/glass surface conductivity, encapsulant conductivity, silicon nitride anti-reflection coating property and interface property (glass/encapsulant; encapsulant/cell; encapsulant/backsheet). Previous studies carried out at ASU's Photovoltaic Reliability Laboratory (ASU-PRL) showed that only negative voltage bias (positive grounded systems) adversely affects the performance of commonly available crystalline silicon modules. In previous studies, the surface conductivity of the glass surface was obtained using either conductive carbon layer extending from the glass surface to the frame or humidity inside an environmental chamber. This thesis investigates the influence of glass surface conductivity disruption on PV modules. In this study, conductive carbon was applied only on the module's glass surface without extending to the frame and the surface conductivity was disrupted (no carbon layer) at 2cm distance from the periphery of frame inner edges. This study was carried out under dry heat at two different temperatures (60 °C and 85 °C) and three different negative bias voltages (-300V, -400V, and -600V). To replicate closeness to the field conditions, half of the selected modules were pre-stressed under damp heat for 1000 hours (DH 1000) and the remaining half under 200 hours of thermal cycling (TC 200). When the surface continuity was disrupted by maintaining a 2 cm gap from the frame to the edge of the conductive layer, as demonstrated in this study, the degradation was found to be absent or negligibly small even after 35 hours of negative bias at elevated temperatures. This preliminary study appears to indicate that the modules could become immune to PID losses if the continuity of the glass surface conductivity is disrupted at the inside boundary of the frame. The surface conductivity of the glass, due to water layer formation in a humid condition, close to the frame could be disrupted just by applying a water repelling (hydrophobic) but high transmittance surface coating (such as Teflon) or modifying the frame/glass edges with water repellent properties.
ContributorsTatapudi, Sai Ravi Vasista (Author) / Tamizhmani, Govindasamy (Thesis advisor) / Srinivasan, Devarajan (Committee member) / Rogers, Bradley (Committee member) / Arizona State University (Publisher)
Created2012
Description
Filtration for microfluidic sample-collection devices is desirable for sample selection, concentration, preprocessing, and downstream manipulation, but microfabricating the required sub-micrometer filtration structure is an elaborate process. This thesis presents a simple method to fabricate polydimethylsiloxane (PDMS) devices with an integrated membrane filter that will sample, lyse, and extract the DNA from microorganisms in aqueous environments. An off-the-shelf membrane filter disc was embedded in a PDMS layer and sequentially bound with other PDMS channel layers. No leakage was observed during filtration. This device was validated by concentrating a large amount of cyanobacterium Synechocystis in simulated sample water with consistent performance across devices. After accumulating sufficient biomass on the filter, a sequential electrochemical lysing process was performed by applying 5VDC across the filter. This device was further evaluated by delivering several samples of differing concentrations of cyanobacterium Synechocystis then quantifying the DNA using real-time PCR. Lastly, an environmental sample was run through the device and the amount of photosynthetic microorganisms present in the water was determined. The major breakthroughs in this design are low energy demand, cheap materials, simple design, straightforward fabrication, and robust performance, together enabling wide-utility of similar chip-based devices for field-deployable operations in environmental micro-biotechnology.
ContributorsLecluse, Aurelie (Author) / Meldrum, Deirdre (Thesis advisor) / Chao, Joseph (Thesis advisor) / Westerhoff, Paul (Committee member) / Arizona State University (Publisher)
Created2011
Description
Photovoltaic (PV) systems are one of the next generation's renewable energy sources for our world energy demand. PV modules are highly reliable. However, in polluted environments, over time, they will collect grime and dust. There are also limited field data studies about soiling losses on PV modules. The study showed how important it is to investigate the effect of tilt angle on soiling. The study includes two sets of mini-modules. Each set has 9 PV modules tilted at 0, 5, 10, 15, 20, 23, 30, 33 and 40°. The first set called "Cleaned" was cleaned every other day. The second set called "Soiled" was never cleaned after the first day. The short circuit current, a measure of irradiance, and module temperature was monitored and recorded every two minutes over three months (January-March 2011). The data were analyzed to investigate the effect of tilt angle on daily and monthly soiling, and hence transmitted solar insolation and energy production by PV modules. The study shows that during the period of January through March 2011 there was an average loss due to soiling of approximately 2.02% for 0° tilt angle. Modules at tilt anlges 23° and 33° also have some insolation losses but do not come close to the module at 0° tilt angle. Tilt anlge 23° has approximately 1.05% monthly insolation loss, and 33° tilt angle has an insolation loss of approximately 0.96%. The soiling effect is present at any tilt angle, but the magnitude is evident: the flatter the solar module is placed the more energy it will lose.
ContributorsCano Valero, José (Author) / Tamizhmani, Govindasamy (Thesis advisor) / Madakannan, Arunachalanadar (Committee member) / Macia, Narciso (Committee member) / Arizona State University (Publisher)
Created2011
Description
As engineered nanomaterials (NMs) become used in industry and commerce their loading to sewage will increase. However, the fate of widely used NMs in wastewater treatment plants (WWTPs) remains poorly understood. In this research, sequencing batch reactors (SBRs) were operated with hydraulic (HRT) and sludge (SRT) retention times representative of full-scale biological WWTPs for several weeks. NM loadings at the higher range of expected environmental concentrations were selected. To achieve the pseudo-equilibrium state concentration of NMs in biomass, SBR experiments needed to operate for more than three times the SRT value, approximately 18 days. Under the conditions tested, NMs had negligible effects on ability of the wastewater bacteria to biodegrade organic material, as measured by chemical oxygen demand (COD). NM mass balance closure was achieved by measuring NMs in liquid effluent and waste biosolids. All NMs were well removed at the typical biomass concentration (1~2 gSS/L). However, carboxy-terminated polymer coated silver nanoparticles (fn-Ag) were removed less effectively (88% removal) than hydroxylated fullerenes (fullerols; >90% removal), nano TiO2 (>95% removal) or aqueous fullerenes (nC60; >95% removal). Although most NMs did not settle out of the feed solution without bacteria present, approximately 65% of the titanium dioxide was removed even in the absence of biomass simply due to self-aggregation and settling. Experiments conducted over 4 months with daily loadings of nC60 showed that nC60 removal from solution depends on the biomass concentration. Under conditions representative of most suspended growth biological WWTPs (e.g., activated sludge), most of the NMs will accumulate in biosolids rather than in liquid effluent discharged to surface waters. Significant fractions of fn-Ag were associated with colloidal material which suggests that efficient particle separation processes (sedimentation or filtration) could further improve removal of NM from effluent. As most NMs appear to accumulate in biosolids, future research should examine the fate of NMs during disposal of WWTP biosolids, which may occur through composting or anaerobic digestion and/or land application, incineration, or landfill disposal.
ContributorsWang, Yifei (Author) / Westerhoff, Paul (Thesis advisor) / Krajmalnik-Brown, Rosa (Committee member) / Rittmann, Bruce (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2012
Analysis and modeling of residual compounds in process streams from U.S. wastewater treatment plants
Description
The presence of compounds such as pharmaceuticals and personal care products (PPCPs) in the environment is a cause for concern as they exhibit secondary effects on non-target organisms and are also indicative of incomplete removal by wastewater treatment plants (WWTPs) during water reclamation. Analytical methods and predictive models can help inform on the rates at which these contaminants enter the environment via biosolids use or wastewater effluent release to estimate the risk of adverse effects. The goals of this research project were to integrate the results obtained from the two different methods of risk assessment, (a) in silico modeling and (b) experimental analysis. Using a previously published empirical model, influent and effluent concentration ranges were predicted for 10 sterols and validated with peer-reviewed literature. The in silico risk assessment analysis performed for sterols and hormones in biosolids concluded that hormones possess high leaching potentials and that particularly 17-α-ethinyl estradiol (EE2) can pose significant threat to fathead minnows (P. promelas) via leaching from terrestrial depositions of biosolids. Six mega-composite biosolids samples representative of 94 WWTPs were analyzed for a suite of 120 PPCPs using the extended U.S. EPA Method 1694 protocol. Results indicated the presence of 26 previously unmonitored PPCPs in the samples with estimated annual release rates of 5-15 tons yr-1 via land application of biosolids. A mesocosm sampling analysis that was included in the study concluded that four compounds amitriptyline, paroxetine, propranolol and sertraline warrant further monitoring due to their high release rates from land applied biosolids and their calculated extended half-lives in soils. There is a growing interest in the scientific community towards the development of new analytical protocols for analyzing solid matrices such as biosolids for the presence of PPCPs and other established and emerging contaminants of concern. The two studies presented here are timely and an important addition to the increasing base of scientific articles regarding environmental release of PPCPs and exposure risks associated with biosolids land application. This research study emphasizes the need for coupling experimental results with predictive analytical modeling output in order to more fully assess the risks posed by compounds detected in biosolids.
ContributorsPrakash Chari, Bipin (Author) / Halden, Rolf U. (Thesis advisor) / Westerhoff, Paul (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2012
Description
Nanotechnology is becoming increasingly present in our environment. Engineered nanoparticles (ENPs), defined as objects that measure less than 100 nanometers in at least one dimension, are being integrated into commercial products because of their small size, increased surface area, and quantum effects. These special properties have made ENPs antimicrobial agents in clothing and plastics, among other applications in industries such as pharmaceuticals, renewable energy, and prosthetics. This thesis incorporates investigations into both application of nanoparticles into polymers as well as implications of nanoparticle release into the environment. First, the integration of ENPs into polymer fibers via electrospinning was explored. Electrospinning uses an external electric field applied to a polymer solution to produce continuous fibers with large surface area and small volume, a quality which makes the fibers ideal for water and air purification purposes. Indium oxide and titanium dioxide nanoparticles were embedded in polyvinylpyrrolidone and polystyrene. Viscosity, critical voltage, and diameter of electrospun fibers were analyzed in order to determine the effects of nanoparticle integration into the polymers. Critical voltage and viscosity of solution increased at 5 wt% ENP concentration. Fiber morphology was not found to change significantly as a direct effect of ENP addition, but as an effect of increased viscosity and surface tension. These results indicate the possibility for seamless integration of ENPs into electrospun polymers. Implications of ENP release were investigated using phase distribution functional assays of nanoscale silver and silver sulfide, as well as photolysis experiments of nanoscale titanium dioxide to quantify hydroxyl radical production. Functional assays are a means of screening the relevant importance of multiple processes in the environmental fate and transport of ENPs. Four functional assays – water-soil, water-octanol, water-wastewater sludge and water-surfactant – were used to compare concentrations of silver sulfide ENPs (Ag2S-NP) and silver ENPs (AgNP) capped by four different coatings. The functional assays resulted in reproducible experiments which clearly showed variations between nanoparticle phase distributions; the findings may be a product of the effects of the different coatings of the ENPs used. In addition to phase distribution experiments, the production of hydroxyl radical (HO•) by nanoscale titanium dioxide (TiO2) under simulated solar irradiation was investigated. Hydroxyl radical are a short-lived, highly reactive species produced by solar radiation in aquatic environments that affect ecosystem function and degrades pollutants. HO• is produced by photolysis of TiO2 and nitrate (NO3-); these two species were used in photolysis experiments to compare the relative loads of hydroxyl radical which nanoscale TiO2 may add upon release to natural waters. Para-chlorobenzoic acid (pCBA) was used as a probe. Measured rates of pCBA oxidation in the presence of various concentrations of TiO2 nanoparticles and NO3- were utilized to calculate pseudo first order rate constants. Results indicate that, on a mass concentration basis in water, TiO2 produces hydroxyl radical steady state concentrations at 1.3 times more than the equivalent amount of NO3-; however, TiO2 concentrations are generally less than one order of magnitude lower than concentrations of NO3-. This has implications for natural waterways as the amount of nanoscale TiO2 released from consumer products into natural waterways increases in proportion to its use.
ContributorsHoogesteijn von Reitzenstein, Natalia (Author) / Westerhoff, Paul (Thesis advisor) / Herckes, Pierre (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2015
Characterization and analysis of long term field aged photovoltaic modules and encapsulant materials
Description
Photovoltaic (PV) module degradation is a well-known issue, however understanding the mechanistic pathways in which modules degrade is still a major task for the PV industry. In order to study the mechanisms responsible for PV module degradation, the effects of these degradation mechanisms must be quantitatively measured to determine the severity of each degradation mode. In this thesis multiple modules from three climate zones (Arizona, California and Colorado) were investigated for a single module glass/polymer construction (Siemens M55) to determine the degree to which they had degraded, and the main factors that contributed to that degradation. To explain the loss in power, various nondestructive and destructive techniques were used to indicate possible causes of loss in performance. This is a two-part thesis. Part 1 presents non-destructive test results and analysis and Part 2 presents destructive test results and analysis.
ContributorsChicca, Matthew (Author) / Tamizhmani, Govindasamy (Thesis advisor) / Rogers, Bradley (Committee member) / Srinivasan, Devarajan (Committee member) / Arizona State University (Publisher)
Created2015
Description
Arsenic (As) is a naturally occurring element that poses a health risk when continually consumed at levels exceeding the Environmental Protection Agencies (EPA) maximum contaminant level (MCL) of 10 ppb. With the Arizona Department of Water Resources considering reliance on other sources of water other than just solely surface water, groundwater proves a reliable, supplemental source. The Salt River Project (SRP) wants to effectively treat their noncompliance groundwater sources to meet EPA compliance. Rapid small-scale column tests (RSSCTs) of two SRP controlled groundwater wells along the Eastern Canal and Consolidated Canal were designed to assist SRP in selection and future design of full-scale packed bed adsorbent media. Main concerns for column choice is effectiveness, design space at groundwater wells, and simplicity. Two adsorbent media types were tested for effective treatment of As to below the MCL: a synthetic iron oxide, Bayoxide E33, and a strong base anion exchange resin, SBG-1. Both media have high affinity toward As and prove effective at treating As from these groundwater sources. Bayoxide E33 RSSCT performance indicated that As treatment lasted to near 60,000 bed volumes (BV) in both water sources and still showed As adsorption extending past this operation ranging from several months to a year. SBG-1 RSSCT performance indicated As, treatment lasted to 500 BV, with the added benefit of being regenerated. At 5%, 13%, and 25% brine regeneration concentrations, regeneration showed that 5% brine is effective, yet would complicate overall design and footprint. Bayoxide E33 was selected as the best adsorbent media for SRP use in full-scale columns at groundwater wells due to its simplistic design and high efficiency.
ContributorsLesan, Dylan (Author) / Westerhoff, Paul (Thesis advisor) / Hristovski, Kiril (Committee member) / Fraser, Matthew (Committee member) / Arizona State University (Publisher)
Created2015