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ABSTRACT The heat recovery steam generator (HRSG) is a key component of Combined Cycle Power Plants (CCPP). The exhaust (flue gas) from the CCPP gas turbine flows through the HRSG − this gas typically contains a high concentration of NO and cannot be discharged directly to the atmosphere because of

ABSTRACT The heat recovery steam generator (HRSG) is a key component of Combined Cycle Power Plants (CCPP). The exhaust (flue gas) from the CCPP gas turbine flows through the HRSG − this gas typically contains a high concentration of NO and cannot be discharged directly to the atmosphere because of environmental restrictions. In the HRSG, one method of reducing the flue gas NO concentration is to inject ammonia into the gas at a plane upstream of the Selective Catalytic Reduction (SCR) unit through an injection grid (AIG); the SCR is where the NO is reduced to N2 and H2O. The amount and spatial distribution of the injected ammonia are key considerations for NO reduction while using the minimum possible amount of ammonia. This work had three objectives. First, a flow network model of the Ammonia Flow Control Unit (AFCU) was to be developed to calculate the quantity of ammonia released into the flue gas from each AIG perforation. Second, CFD simulation of the flue gas flow was to be performed to obtain the velocity, temperature, and species concentration fields in the gas upstream and downstream of the SCR. Finally, performance characteristics of the ammonia injection system were to be evaluated. All three objectives were reached. The AFCU was modeled using JAVA - with a graphical user interface provided for the user. The commercial software Fluent was used for CFD simulation. To evaluate the efficacy of the ammonia injection system in reducing the flue gas NO concentration, the twelve butterfly valves in the AFCU ammonia delivery piping (risers) were throttled by various degrees in the model and the NO concentration distribution computed for each operational scenario. When the valves were kept fully open, it was found that it led to a more uniform reduction in NO concentration compared to throttling the valves such that the riser flows were equal. Additionally, the SCR catalyst was consumed somewhat more uniformly, and ammonia slip (ammonia not consumed in reaction) was found lower. The ammonia use could be decreased by 10 percent while maintaining the NO concentration limit in the flue gas exhausting into the atmosphere.
ContributorsAdulkar, Sajesh (Author) / Roy, Ramendra (Thesis advisor) / Lee, Taewoo (Thesis advisor) / Phelan, Patrick (Committee member) / Arizona State University (Publisher)
Created2011
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Description
Nanoparticles are ubiquitous in various fields due to their unique properties not seen in similar bulk materials. Among them, core-shell composite nanoparticles are an important class of materials which are attractive for their applications in catalysis, sensing, electromagnetic shielding, drug delivery, and environmental remediation. This dissertation focuses on the study

Nanoparticles are ubiquitous in various fields due to their unique properties not seen in similar bulk materials. Among them, core-shell composite nanoparticles are an important class of materials which are attractive for their applications in catalysis, sensing, electromagnetic shielding, drug delivery, and environmental remediation. This dissertation focuses on the study of core-shell type of nanoparticles where a polymer serves as the core and inorganic nanoparticles are the shell. This is an interesting class of supramolecular building blocks and can "exhibit unusual, possibly unique, properties which cannot be obtained simply by co-mixing polymer and inorganic particles". The one-step Pickering emulsion polymerization method was successfully developed and applied to synthesize polystyrene-silica core-shell composite particles. Possible mechanisms of the Pickering emulsion polymerization were also explored. The silica nanoparticles were thermodynamically favorable to self-assemble at liquid-liquid interfaces at the initial stage of polymerization and remained at the interface to finally form the shells of the composite particles. More importantly, Pickering emulsion polymerization was employed to synthesize polystyrene/poly(N-isopropylacrylamide) (PNIPAAm)-silica core-shell nanoparticles with N-isopropylacrylamide incorporated into the core as a co-monomer. The composite nanoparticles were temperature sensitive and could be up-taken by human prostate cancer cells and demonstrated effectiveness in drug delivery and cancer therapy. Similarly, by incorporating poly-2-(N,N)-dimethylamino)ethyl methacrylate (PDMA) into the core, pH sensitive core-shell composite nanoparticles were synthesized and applied as effective carriers to release a rheological modifier upon a pH change. Finally, the research focuses on facile approaches to engineer the transition of the temperature-sensitive particles and develop composite core-shell nanoparticles with a metallic shell.
ContributorsSanyal, Sriya (Author) / Dai, Lenore L. (Thesis advisor) / Jiang, Hanqing (Committee member) / Lind, Mary L. (Committee member) / Phelan, Patrick (Committee member) / Rege, Kaushal (Committee member) / Arizona State University (Publisher)
Created2012
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Description
In this study, two novel sorbents (zeolite 4A and sodium polyacrylate) are tested to investigate if utilizing ultrasonic acoustic energy could decrease the amount of time and overall energy required to regenerate these materials for use in cooling applications. To do this, an experiment was designed employing a cartridge heater

In this study, two novel sorbents (zeolite 4A and sodium polyacrylate) are tested to investigate if utilizing ultrasonic acoustic energy could decrease the amount of time and overall energy required to regenerate these materials for use in cooling applications. To do this, an experiment was designed employing a cartridge heater and a piezoelectric element to be simultaneously providing heat and acoustic power to a custom designed desorption bed while measuring the bed mass and sorbent temperature at various locations. The results prove to be promising showing that early in the desorption process ultrasound may expedite the desorption process in zeolite by as much as five times and in sodium polyacrylate as much as three times in comparison to providing heat alone. The results also show that in zeolite desorption utilizing ultrasound may be particularly beneficial to initiate desorption whereas in sodium polyacrylate ultrasound appears most promising in the after a temperature threshold is met. These are exciting results and may prove to be significant in the future as more novel heat-based cooling cycles are developed.
ContributorsBertrand, Weston Kyle (Author) / Phelan, Patrick (Thesis advisor) / Bocanegra, Luis (Committee member) / Wang, Liping (Committee member) / Devasenathipathy, Shankar (Committee member) / Arizona State University (Publisher)
Created2018
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Description
Hydrogel polymers have been the subject of many studies, due to their fascinating ability to alternate between being hydrophilic and hydrophobic, upon the application of appropriate stimuli. In particular, thermo-responsive hydrogels such as N-Isopropylacrylamide (NIPAM), which possess a unique lower critical solution temperature (LCST) of 32°C, have been leveraged for

Hydrogel polymers have been the subject of many studies, due to their fascinating ability to alternate between being hydrophilic and hydrophobic, upon the application of appropriate stimuli. In particular, thermo-responsive hydrogels such as N-Isopropylacrylamide (NIPAM), which possess a unique lower critical solution temperature (LCST) of 32°C, have been leveraged for membrane-based processes such as using NIPAM as a draw agent for forward osmosis (FO) desalination. The low LCST temperature of NIPAM ensures that fresh water can be recovered, at a modest energy cost as compared to other thermally based desalination processes which require water recovery at higher temperatures. This work studies by experimentation, key process parameters involved in desalination by FO using NIPAM and a copolymer of NIPAM and Sodium Acrylate (NIPAM-SA). It encompasses synthesis of the hydrogels, development of experiments to effectively characterize synthesized products, and the measuring of FO performance for the individual hydrogels. FO performance was measured using single layers of NIPAM and NIPAM-SA respectively. The values of permeation flux obtained were compared to relevant published literature and it was found to be within reasonable range. Furthermore, a conceptual design for future large-scale implementation of this technology is proposed. It is proposed that perhaps more effort should focus on physical processes that have the ability to increase the low permeation flux of hydrogel driven FO desalination systems, rather than development of novel classes of hydrogels
ContributorsAbdullahi, Adnan None (Author) / Phelan, Patrick (Thesis advisor) / Wang, Robert (Committee member) / Dai, Lenore (Committee member) / Arizona State University (Publisher)
Created2019
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Description
Thermodynamic development and balance of plant study is completed for a 30 MW solar thermochemical water splitting process that generates hydrogen gas and electric power. The generalized thermodynamic model includes 23 components and 45 states. Quasi-steady state simulations are completed for design point system sizing, annual performance analysis and sensitivity

Thermodynamic development and balance of plant study is completed for a 30 MW solar thermochemical water splitting process that generates hydrogen gas and electric power. The generalized thermodynamic model includes 23 components and 45 states. Quasi-steady state simulations are completed for design point system sizing, annual performance analysis and sensitivity analysis. Detailed consideration is given to water splitting reaction kinetics with governing equations generalized for use with any redox-active metal oxide material. Specific results for Ceria illustrate particle reduction in two solar receivers for target oxygen partial pressure of 10 Pa and particle temperature of 1773 K at a design point DNI of 900 W/m2. Sizes of the recuperator, steam generator and hydrogen separator are calculated at the design point DNI to achieve 100,000 kg of hydrogen production per day from the plant. The total system efficiency of 39.52% is comprised of 50.7% hydrogen fraction and 19.62% electrical fraction. Total plant capital costs and operating costs are estimated to equate a hydrogen production cost of $4.40 per kg for a 25-year plant life. Sensitivity analysis explores the effect of environmental parameters and design parameters on system performance and cost. Improving recuperator effectiveness from 0.7 to 0.8 is a high-value design modification resulting in a 12.1% decrease in hydrogen cost for a modest 2.0% increase in plant $2.85M. At the same time, system efficiency is relatively inelastic to recuperator effectiveness because 81% of excess heat is recovered from the system for electricity production 39 MWh/day and revenue is $0.04 per kWh. Increasing water inlet pressure up to 20 bar reduces the size and cost of super heaters but further pressure rises increasing pump at a rate that outweighs super heater cost savings.
ContributorsBudama, Vishnu Kumar (Author) / Johnson, Nathan (Thesis advisor) / Stechel, Ellen (Committee member) / Rykaczewski, Konrad (Committee member) / Phelan, Patrick (Committee member) / Wang, Robert (Committee member) / Arizona State University (Publisher)
Created2018
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Description
The large-scale anthropogenic emission of carbon dioxide into the atmosphere leads to many unintended consequences, from rising sea levels to ocean acidification. While a clean energy infrastructure is growing, mid-term strategies that are compatible with the current infrastructure should be developed. Carbon capture and storage in fossil-fuel power plants is

The large-scale anthropogenic emission of carbon dioxide into the atmosphere leads to many unintended consequences, from rising sea levels to ocean acidification. While a clean energy infrastructure is growing, mid-term strategies that are compatible with the current infrastructure should be developed. Carbon capture and storage in fossil-fuel power plants is one way to avoid our current gigaton-scale emission of carbon dioxide into the atmosphere. However, for this to be possible, separation techniques are necessary to remove the nitrogen from air before combustion or from the flue gas after combustion. Metal-organic frameworks (MOFs) are a relatively new class of porous material that show great promise for adsorptive separation processes. Here, potential mechanisms of O2/N2 separation and CO2/N2 separation are explored.

First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
ContributorsMcIntyre, Sean (Author) / Mu, Bin (Thesis advisor) / Green, Matthew (Committee member) / Lind, Marylaura (Committee member) / Arizona State University (Publisher)
Created2019
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Description
Reactive inkjet printing (RIJP) is a direct-write deposition technique that synthesizes and patterns functional materials simultaneously. It is a route to cheap fabrication of highly conductive features on a versatile range of substrates. Silver reactive inks have become a staple of conductive inkjet printing for application in printed and flexible

Reactive inkjet printing (RIJP) is a direct-write deposition technique that synthesizes and patterns functional materials simultaneously. It is a route to cheap fabrication of highly conductive features on a versatile range of substrates. Silver reactive inks have become a staple of conductive inkjet printing for application in printed and flexible electronics, photovoltaic metallization, and more. However, the high cost of silver makes these less effective for disposable and low-cost applications.

This work aimed to develop a particle-free formulation for a nickel reactive ink capable of metallizing highly pure nickel at temperatures under 100 °C to facilitate printing on substrates like paper or plastic. Nickel offers a significantly cheaper alternative to silver at slightly reduced bulk conductivity.

To meet these aims, three archetypes of inks were formulated. First were a set of glycerol-based inks temperature ink containing nickel acetate, hydrazine, and ammonia in a mixture of water and glycerol. This ink reduced between 115 – 200 °C to produce slightly oxidized deposits of nickel with carbon content around 10 wt %.

The high temperature was addressed in a second series, which replaced glycerol with lower boiling glycols and added sodium hydroxide as a strong base to enhance thermodynamics and kinetics of reduction. These inks reduced between 60 and 100 °C but sodium salts contaminated the final deposits.

In a third set of inks, sodium hydroxide was replaced with tetramethylammonium hydroxide (TMAH), a strong organic base, to address contamination. These inks also reduced between 60 and 100 °C. Pipetting or printing onto gold coated substrates produce metallic flakes coated in a clear, thick residue. EDS measured carbon and oxygen content up to 70 wt % of deposits. The residue was hypothesized to be a non-volatile byproduct of TMAH and acetate.

Recommendations are provided to address the residue. Ultimately the formulated reactive inks did not meet design targets. However, this thesis sets the framework to design an optimal nickel reactive ink in future work.
ContributorsDebruin, Dylan Jerome (Author) / Torres, Cesar (Thesis advisor) / Rykaczewski, Konrad (Thesis advisor) / Hildreth, Owen (Committee member) / Arizona State University (Publisher)
Created2019
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Description
Portable devices rely on battery systems that contribute largely to the overall device form factor and delay portability due to recharging. Membraneless microfluidic fuel cells are considered as the next generation of portable power sources for their compatibility with higher energy density reactants. Microfluidic fuel cells are potentially cost effective

Portable devices rely on battery systems that contribute largely to the overall device form factor and delay portability due to recharging. Membraneless microfluidic fuel cells are considered as the next generation of portable power sources for their compatibility with higher energy density reactants. Microfluidic fuel cells are potentially cost effective and robust because they use low Reynolds number flow to maintain fuel and oxidant separation instead of ion exchange membranes. However, membraneless fuel cells suffer from poor efficiency due to poor mass transport and Ohmic losses. Current microfluidic fuel cell designs suffer from reactant cross-diffusion and thick boundary layers at the electrode surfaces, which result in a compromise between the cell's power output and fuel utilization. This dissertation presents novel flow field architectures aimed at alleviating the mass transport limitations. The first architecture provides a reactant interface where the reactant diffusive concentration gradients are aligned with the bulk flow, mitigating reactant mixing through diffusion and thus crossover. This cell also uses porous electro-catalysts to improve electrode mass transport which results in higher extraction of reactant energy. The second architecture uses porous electrodes and an inert conductive electrolyte stream between the reactants to enhance the interfacial electrical conductivity and maintain complete reactant separation. This design is stacked hydrodynamically and electrically, analogous to membrane based systems, providing increased reactant utilization and power. These fuel cell architectures decouple the fuel cell's power output from its fuel utilization. The fuel cells are tested over a wide range of conditions including variation of the loads, reactant concentrations, background electrolytes, flow rates, and fuel cell geometries. These experiments show that increasing the fuel cell power output is accomplished by increasing reactant flow rates, electrolyte conductivity, and ionic exchange areas, and by decreasing the spacing between the electrodes. The experimental and theoretical observations presented in this dissertation will aid in the future design and commercialization of a new portable power source, which has the desired attributes of high power output per weight and volume and instant rechargeability.
ContributorsSalloum, Kamil S (Author) / Posner, Jonathan D (Thesis advisor) / Adrian, Ronald (Committee member) / Christen, Jennifer (Committee member) / Phelan, Patrick (Committee member) / Chen, Kangping (Committee member) / Arizona State University (Publisher)
Created2010
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Description
The conversion of H2S enables the recycling of a waste gas into a potential source of hydrogen at a lower thermodynamic energy cost as compared to water splitting. However, studies on the photocatalytic decomposition of H2S focus on traditional deployment of catalyst materials to facilitate this conversion, and operation only

The conversion of H2S enables the recycling of a waste gas into a potential source of hydrogen at a lower thermodynamic energy cost as compared to water splitting. However, studies on the photocatalytic decomposition of H2S focus on traditional deployment of catalyst materials to facilitate this conversion, and operation only when a light source is available. In this study, the efficacy of Direct Ink Written (DIW) luminous structures for H2S conversion has been investigated, with the primary objective of sustaining H2S conversion when a light source has been terminated. Additionally, as a secondary objective, improving light distribution within monoliths for photocatalytic applications is desired. The intrinsic illumination of the 3D printed monoliths developed in this work could serve as an alternative to monolith systems that employ light transmitting fiber optic cables that have been previously proposed to improve light distribution in photocatalytic systems. The results that were obtained demonstrate that H2S favorable adsorbents, a wavelength compatible long afterglow phosphor, and a photocatalyst can form viscoelastic inks that are printable into DIW luminous monolithic contactors. Additionally, rheological, optical and porosity analyses conducted, provide design guidelines for future studies seeking to develop DIW luminous monoliths from compatible catalyst-phosphor pairs. The monoliths that were developed demonstrate not only improved conversion when exposed to light, but more significantly, extended H2S conversion from the afterglow of the monoliths when an external light source was removed. Lastly, considering growing interests in attaining a global circular economy, the techno-economic feasibility of a H2S-CO2 co-utilization plant leveraging hydrogen from H2S photocatalysis as a feed source for a downstream CO2 methanation plant has been assessed. The work provides preliminary information to guide future chemical kinetic design characteristics that are important to strive for if using H2S as a source of hydrogen in a CO2 methanation facility.
ContributorsAbdullahi, Adnan (Author) / Andino, Jean (Thesis advisor) / Phelan, Patrick (Thesis advisor) / Bhate, Dhruv (Committee member) / Wang, Robert (Committee member) / Huang, Huei-Ping (Committee member) / Arizona State University (Publisher)
Created2023
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Description
As experiencing hot months and thermal stresses is becoming more common, chemically protective fabrics must adapt and provide protections while reducing the heat stress to the body. These concerns affect first responders, warfighters, and workers regularly surrounded by hazardous chemical agents. While adapting traditional garments with cooling devices provides one

As experiencing hot months and thermal stresses is becoming more common, chemically protective fabrics must adapt and provide protections while reducing the heat stress to the body. These concerns affect first responders, warfighters, and workers regularly surrounded by hazardous chemical agents. While adapting traditional garments with cooling devices provides one route to mitigate this issue, these cooling methods add bulk, are time limited, and may not be applicable in locations without logistical support. Here I take inspiration from nature to guide the development of smart fabrics that have high breathability, but self-seal on exposure to target chemical(s), providing a better balance between cooling and protection.

Natural barrier materials were explored as a guide, focusing specifically on prickly pear cacti. These cacti have a natural waxy barrier that provides protection from dehydration and physically changes shape to modify surface wettability and water vapor transport. The results of this study provided a basis for a shape changing polymer to be used to respond directly to hazardous chemicals, swelling to contain the agent.

To create a stimuli responsive material, a novel superabsorbent polymer was synthesized, based on acrylamide chemistry. The polymer was tested for swelling properties in a wide range of organic liquids and found to highly swell in moderately polar organic liquids. To help predict swelling in untested liquids, the swelling of multiple test liquids were compared with their thermodynamic properties to observe trends. As the smart fabric needs to remain breathable to allow evaporative cooling, while retaining functionality when soaked with sweat, absorption of water, as well as that of an absorbing liquid in the presence of water were tested.

Micron sized particles of the developed polymer were deposited on a plastic mesh with pore size and open area similar to common clothing fabric to establish the proof of concept of using a breathable barrier to provide chemical protection. The polymer coated mesh showed minimal additional resistance to water vapor transport, relative to the mesh alone, but blocked more than 99% of a xylene aerosol from penetrating the barrier.
ContributorsManning, Kenneth (Author) / Rykaczewski, Konrad (Thesis advisor) / Burgin, Timothy (Committee member) / Emady, Heather (Committee member) / Green, Matthew (Committee member) / Thomas, Marylaura (Committee member) / Arizona State University (Publisher)
Created2020