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Environmentally responsible use of nanomaterials for the photocatalytic reduction of nitrate in water

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

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).

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2013

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Development and characterization of gas diffusion layer using carbon slurry dispersed by ammonium lauryl sulfate for proton exchange member fuel cells

Description

Gas diffusion layers (GDLs) are a critical and essential part of proton exchange membrane fuel cells (PEMFCs). They carry out various important functions such as transportation of reactants to and from the reaction sites. The material properties and structural characteristics

Gas diffusion layers (GDLs) are a critical and essential part of proton exchange membrane fuel cells (PEMFCs). They carry out various important functions such as transportation of reactants to and from the reaction sites. The material properties and structural characteristics of the substrate and the microporous layer strongly influence fuel cell performance. The microporous layer of the GDLs was fabricated with the carbon slurry dispersed in water containing ammonium lauryl sulfate (ALS) using the wire rod coating method. GDLs were fabricated with different materials to compose the microporous layer and evaluated the effects on PEMFC power output performance. The consistency of the carbon slurry was achieved by adding 25 wt. % of PTFE, a binding agent with a 75:25 ratio of carbon (Pureblack and vapor grown carbon fiber). The GDLs were investigated in PEMFC under various relative humidity (RH) conditions using H2/O2 and H2/Air. GDLs were also fabricated with the carbon slurry dispersed in water containing sodium dodecyl sulfate (SDS) and multiwalled carbon nanotubes (MWCNTs) with isopropyl alcohol (IPA) based for fuel cell performance comparison. MWCNTs and SDS exhibits the highest performance at 60% and 70% RH with a peak power density of 1100 mW.cm-2 and 850 mW.cm-2 using air and oxygen as an oxidant. This means that the gas diffusion characteristics of these two samples were optimum at 60 and 70 % RH with high limiting current density range. It was also found that the composition of the carbon slurry, specifically ALS concentration has the highest peak power density of 1300 and 500mW.cm-2 for both H2/O2 and H2/Air at 100% RH. However, SDS and MWCNTs demonstrates the lowest power density using air and oxygen as an oxidants at 100% RH.

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Date Created
2012

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Comparison of four methods to assess silver release from nano impregnated reverse osmosis membranes

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,

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.

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Date Created
2017

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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

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.

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Date Created
2015

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Development of Hydrogel-based Porous Desiccants for Atmospheric Water Extraction

Description

Atmospheric water extraction (AWE) is an emerging technology to tackle water resource shortage challenges. One such approach to provide fresh water utilizes stimuli-responsive hydrogel-based desiccants to capture the moisture from the air and release it into the liquid form. Typical

Atmospheric water extraction (AWE) is an emerging technology to tackle water resource shortage challenges. One such approach to provide fresh water utilizes stimuli-responsive hydrogel-based desiccants to capture the moisture from the air and release it into the liquid form. Typical gel desiccants are composed of a hygroscopic agent for capturing and a hydrophilic gel matrix for storage. The desorption process can be completed by elevating the temperature above the upper or lower critical solution temperature point to initiate the volume phase transition of either thermo-responsive or photothermal types. This thesis focuses on investigating the structural effect of hydrogels on moisture uptake. Firstly, the main matrix of gel desiccant, poly(N-isopropylacrylamide) hydrogel, was optimized via tuning synthesis temperature and initial monomer concentration. Secondly, a series of hydrogel-based desiccants consisting of a hygroscopic material, vinyl imidazole, and optimized poly(N-isopropylacrylamide) gel matrix were synthesized with different network structures. The moisture uptake result showed that the gel desiccant with an interpenetrating polymeric network (IPN) resulted in the best-performing moisture capturing. The gel desiccant with the best performance will be used as a primary structural unit to evaluate the feasibility of developing a light-responsive gel desiccant to materialize light-trigger moisture desorption for AWE technology in the future.

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Date Created
2021

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Carbonaceous nanomaterials as flame retardant coating on fabric

Description

Flame retardants (FRs) are applied to variety of consumer products such as textiles and polymers for fire prevention and fire safety. Substantial research is ongoing to replace traditional FRs with alternative materials that are less toxic, present higher flame retardancy

Flame retardants (FRs) are applied to variety of consumer products such as textiles and polymers for fire prevention and fire safety. Substantial research is ongoing to replace traditional FRs with alternative materials that are less toxic, present higher flame retardancy and result in lower overall exposure as there are potential health concerns in case of exposure to popular FRs. Carbonaceous nanomaterials (CNMs) such as carbon nanotubes (CNTs) and graphene oxide (GO) have been studied and applied to polymer composites and electronics extensively due to their remarkable properties. Hence CNMs are considered as potential alternative materials that present high flame retardancy. In this research, different kinds of CNMs coatings on polyester fabric are produced and evaluated for their use as flame retardants. To monitor the mass loading of CNMs coated on the fabric, a two-step analytical method for quantifying CNMs embedded in polymer composites was developed. This method consisted of polymer dissolution process using organic solvents followed by subsequent programmed thermal analysis (PTA). This quantification technique was applicable to CNTs with and without high metal impurities in a broad range of polymers. Various types of CNMs were coated on polyester fabric and the efficacy of coatings as flame retardant was evaluated. The oxygen content of CNMs emerged as a critical parameter impacting flame retardancy with higher oxygen content resulting in less FR efficacy. The most performant nanomaterials, multi-walled carbon nanotubes (MWCNTs) and amine functionalized multi-walled carbon nantoubes (NH2-MWCNT) showed similar FR properties to current flame retardants with low mass loading (0.18 g/m2) and hence are promising alternatives that warrant further investigation. Chemical/physical modification of MWCNTs was conducted to produce well-dispersed MWCNT solutions without involving oxygen for uniform FR coating. The MWCNTs coating was studied to evaluate the durability of the coating and the impact on the efficacy during use phase by conducting mechanical abrasion and washing test. Approximately 50% and 40% of MWCNTs were released from 1 set of mechanical abrasion and washing test respectively. The losses during simulated usage impacted the flame retardancy negatively.

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Date Created
2018

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Dependence of toxicity test results on sample removal methods of PV modules

Description

The volume of end-of-life photovoltaic (PV) modules is increasing as the global PV market increases, and the global PV waste streams are expected to reach 250,000 metric tons by the end of 2020. If the recycling processes are not in

The volume of end-of-life photovoltaic (PV) modules is increasing as the global PV market increases, and the global PV waste streams are expected to reach 250,000 metric tons by the end of 2020. If the recycling processes are not in place, there would be 60 million tons of end-of-life PV modules lying in the landfills by 2050, that may not become a not-so-sustainable way of sourcing energy since all PV modules could contain certain amount of toxic substances. Currently in the United States, PV modules are categorized as general waste and can be disposed in landfills. However, potential leaching of toxic chemicals and materials, if any, from broken end-of-life modules may pose health or environmental risks. There is no standard procedure to remove samples from PV modules for chemical toxicity testing in the Toxicity Characteristic Leaching Procedure (TCLP) laboratories as per EPA 1311 standard. The main objective of this thesis is to develop an unbiased sampling approach for the TCLP testing of PV modules. The TCLP testing was concentrated only for the laminate part of the modules, as they are already existing recycling technologies for the frame and junction box components of PV modules. Four different sample removal methods have been applied to the laminates of five different module manufacturers: coring approach, cell-cut approach, strip-cut approach, and hybrid approach. These removed samples were sent to two different TCLP laboratories, and TCLP results were tested for repeatability within a lab and reproducibility between the labs. The pros and cons of each sample removal method have been explored and the influence of sample removal methods on the variability of TCLP results has been discussed. To reduce the variability of TCLP results to an acceptable level, additional improvements in the coring approach, the best of the four tested options, are still needed.

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Date Created
2018

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Comparison of Encapsulant Degradation between Glass/Backsheet and Glass/Glass Field-aged Photovoltaic Modules

Description

Ethylene vinyl acetate (EVA) is the most commonly used encapsulant in photovoltaic modules. However, EVA degrades over time and causes performance losses in PV system. Therefore, EVA degradation is a matter of concern from a durability point of view.

This

Ethylene vinyl acetate (EVA) is the most commonly used encapsulant in photovoltaic modules. However, EVA degrades over time and causes performance losses in PV system. Therefore, EVA degradation is a matter of concern from a durability point of view.

This work compares EVA encapsulant degradation in glass/backsheet and glass/glass field-aged PV modules. EVA was extracted from three field-aged modules (two glass/backsheet and one glass/glass modules) from three different manufacturers from various regions (cell edges, cell centers, and non-cell region) from each module based on their visual and UV Fluorescence images. Characterization techniques such as I-V measurements, Colorimetry, Different Scanning Calorimetry, Thermogravimetric Analysis, Raman spectroscopy, and Fourier Transform Infrared Spectroscopy were performed on EVA samples.

The intensity of EVA discoloration was quantified using colorimetric measurements. Module performance parameters like Isc and Pmax degradation rates were calculated from I-V measurements. Properties such as degree of crystallinity, vinyl acetate content and degree of crosslinking were calculated from DSC, TGA, and Raman measurements, respectively. Polyenes responsible for EVA browning were identified in FTIR spectra.

The results from the characterization techniques confirmed that when EVA undergoes degradation, crosslinking in EVA increases beyond 90% causing a decrease in the degree of crystallinity and an increase in vinyl acetate content of EVA. Presence of polyenes in FTIR spectra of degraded EVA confirmed the occurrence of Norrish II reaction. However, photobleaching occurred in glass/backsheet modules due to the breathable backsheet whereas no photobleaching occurred in glass/glass modules because they were hermetically sealed. Hence, the yellowness index along with the Isc and Pmax degradation rates of EVA in glass/glass module is higher than that in glass/backsheet modules.

The results implied that more acetic acid was produced in the non-cell region due to its double layer of EVA compared to the front EVA from cell region. But, since glass/glass module is hermetically sealed, acetic acid gets entrapped inside the module further accelerating EVA degradation whereas it diffuses out through backsheet in glass/backsheet modules. Hence, it can be said that EVA might be a good encapsulant for glass/backsheet modules, but the same cannot be said for glass/glass modules.

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Date Created
2018

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Series resistance increase in field degraded PV modules in different climatic conditions

Description

Global photovoltaic (PV) module installation in 2018 is estimated to exceed 100 GW, and crystalline Si (c-Si) solar cell-based modules have a share more than 90% of the global PV market. To reduce the social cost of PV electricity, further

Global photovoltaic (PV) module installation in 2018 is estimated to exceed 100 GW, and crystalline Si (c-Si) solar cell-based modules have a share more than 90% of the global PV market. To reduce the social cost of PV electricity, further developments in reliability of solar panels are expected. These will lead to realize longer module lifetime and reduced levelized cost of energy. As many as 86 failure modes are observed in PV modules [1] and series resistance increase is one of the major durability issues of all. Series resistance constitutes emitter sheet resistance, metal-semiconductor contact resistance, and resistance across the metal-solder ribbon. Solder bond degradation at the cell interconnect is one of the primary causes for increase in series resistance, which is also considered to be an invisible defect [1]. Combination of intermetallic compounds (IMC) formation during soldering and their growth due to solid state diffusion over its lifetime result in formation of weak interfaces between the solar cell and the interconnect. Thermal cycling under regular operating conditions induce thermo-mechanical fatigue over these weak interfaces resulting in contact reduction or loss. Contact reduction or loss leads to increase in series resistance which further manifests into power and fill factor loss. The degree of intermixing of metallic interfaces and contact loss depends on climatic conditions as temperature and humidity (moisture ingression into the PV module laminate) play a vital role in reaction kinetics of these layers. Modules from Arizona and Florida served as a good sample set to analyze the effects of hot and humid climatic conditions respectively. The results obtained in the current thesis quantifies the thickness of IMC formation from SEM-EDS profiles, where similar modules obtained from different climatic conditions were compared. The results indicate the thickness of the IMC and detachment degree to be growing with age and operating temperatures of the module. This can be seen in CuxSny IMC which is thicker in the case of Arizona module. The results obtained from FL

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aged modules also show that humidity accelerates the formation of IMC as they showed thicker AgxSny layer and weak interconnect-contact interfaces as compared to Arizona modules. It is also shown that climatic conditions have different effects on rate at which CuxSny and AgxSny intermetallic compounds are formed.

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Date Created
2018

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Reliability of Photovoltaic Cells with Plated Copper Electrodes

Description

An ongoing effort in the photovoltaic (PV) industry is to reduce the major manufacturing cost components of solar cells, the great majority of which are based on crystalline silicon (c-Si). This includes the substitution of screenprinted silver (Ag) cell contacts

An ongoing effort in the photovoltaic (PV) industry is to reduce the major manufacturing cost components of solar cells, the great majority of which are based on crystalline silicon (c-Si). This includes the substitution of screenprinted silver (Ag) cell contacts with alternative copper (Cu)-based contacts, usually applied with plating. Plated Cu contact schemes have been under study for many years with only minor traction in industrial production. One of the more commonly-cited barriers to the adoption of Cu-based contacts for photovoltaics is long-term reliability, as Cu is a significant contaminant in c-Si, forming precipitates that degrade performance via degradation of diode character and reduction of minority carrier lifetime. Cu contamination from contacts might cause degradation during field deployment if Cu is able to ingress into c-Si. Furthermore, Cu contamination is also known to cause a form of light-induced degradation (LID) which further degrades carrier lifetime when cells are exposed to light.

Prior literature on Cu-contact reliability tended to focus on accelerated testing at the cell and wafer level that may not be entirely replicative of real-world environmental stresses in PV modules. This thesis is aimed at advancing the understanding of Cu-contact reliability from the perspective of quasi-commercial modules under more realistic stresses. In this thesis, c-Si solar cells with Cu-plated contacts are fabricated, made into PV modules, and subjected to environmental stress in an attempt to induce hypothesized failure modes and understand any new vulnerabilities that Cu contacts might introduce. In particular, damp heat stress is applied to conventional, p-type c-Si modules and high efficiency, n-type c-Si heterojunction modules. I present evidence of Cu-induced diode degradation that also depends on PV module materials, as well as degradation unrelated to Cu, and in either case suggest engineering solutions to the observed degradation. In a forensic search for degradation mechanisms, I present novel evidence of Cu outdiffusion from contact layers and encapsulant-driven contact corrosion as potential key factors. Finally, outdoor exposures to light uncover peculiarities in Cu-plated samples, but do not point to especially serious vulnerabilities.

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Date Created
2020