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Description
Two-dimensional transition metal dichalcogenides (TMDCs) such as
molybdenum disulfide (MoS2), tungsten disulfide (WS2), molybdenum diselenide (MoSe2) and tungsten diselenide (WSe2) are attractive for use in biotechnology, optical and electronics devices due to their promising and tunable electrical, optical and chemical properties. To fulfill the variety of requirements for different applications, chemical treatment methods are developed to tune their properties. In this dissertation, plasma treatment, chemical doping and functionalization methods have been applied to tune the properties of TMDCs. First, plasma treatment of TMDCs results in doping and generation of defects, as well as the synthesis of transition metal oxides (TMOs) with rolled layers that have increased surface-to-volume ratio and are promising for electrochemical applications. Second, chemical functionalization is another powerful approach for tuning the properties of TMDCs for use in many applications. To covalently functionalize the basal planes of TMDCs, previous reports begin with harsh treatments like lithium intercalation that disrupt the structure and lead to a phase transformation from semiconducting to metallic. Instead, this work demonstrates the direct covalent functionalization of semiconducting MoS2 using aryl diazonium salts without lithium treatments. It preserves the structure and semiconducting nature of MoS2, results in covalent C-S bonds on basal planes and enables different functional groups to be tethered to the MoS2 surface via the diazonium salts. The attachment of fluorescent proteins has been used as a demonstration and it suggests future applications in biology and biosensing. The effects of the covalent functionalization on the electronic transport properties of MoS2 were then studied using field effect transistor (FET) devices.
molybdenum disulfide (MoS2), tungsten disulfide (WS2), molybdenum diselenide (MoSe2) and tungsten diselenide (WSe2) are attractive for use in biotechnology, optical and electronics devices due to their promising and tunable electrical, optical and chemical properties. To fulfill the variety of requirements for different applications, chemical treatment methods are developed to tune their properties. In this dissertation, plasma treatment, chemical doping and functionalization methods have been applied to tune the properties of TMDCs. First, plasma treatment of TMDCs results in doping and generation of defects, as well as the synthesis of transition metal oxides (TMOs) with rolled layers that have increased surface-to-volume ratio and are promising for electrochemical applications. Second, chemical functionalization is another powerful approach for tuning the properties of TMDCs for use in many applications. To covalently functionalize the basal planes of TMDCs, previous reports begin with harsh treatments like lithium intercalation that disrupt the structure and lead to a phase transformation from semiconducting to metallic. Instead, this work demonstrates the direct covalent functionalization of semiconducting MoS2 using aryl diazonium salts without lithium treatments. It preserves the structure and semiconducting nature of MoS2, results in covalent C-S bonds on basal planes and enables different functional groups to be tethered to the MoS2 surface via the diazonium salts. The attachment of fluorescent proteins has been used as a demonstration and it suggests future applications in biology and biosensing. The effects of the covalent functionalization on the electronic transport properties of MoS2 were then studied using field effect transistor (FET) devices.
ContributorsChu, Ximo (Author) / Wang, Qing Hua (Thesis advisor) / Sieradzki, Karl (Committee member) / Green, Alexander (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2018
Description
With the need to address the world's growing energy demand, many new
alternative and renewable energy sources are being researched and developed. Many
of these technologies are in their infancy, still being too inefficient or too costly to
implement on a large scale. This list of alternative energies include biofuels,
geothermal power, solar energy, wind energy and hydroelectric power. This thesis
focuses on developing a concentrating solar thermal energy unit for the application
of an on-demand hot water system with phase change material. This system already
has a prototype constructed and needs refinement in several areas in order to
increase its efficiency to determine if the system could ever reach a point of
feasibility in a residential application. Having put additional control refining
systems on the solar water heat collector, it can be deduced that the efficiency has
increased. However, due to limited testing and analysis it is undetermined just how
much the efficiency of the system has increased. At minimum, the capabilities of the
research platform have dramatically increased, allowing future research to more
accurately study the dynamics of the system as well as conduct studies in more
targeted areas of engineering. In this aspect, the thesis was successful.
alternative and renewable energy sources are being researched and developed. Many
of these technologies are in their infancy, still being too inefficient or too costly to
implement on a large scale. This list of alternative energies include biofuels,
geothermal power, solar energy, wind energy and hydroelectric power. This thesis
focuses on developing a concentrating solar thermal energy unit for the application
of an on-demand hot water system with phase change material. This system already
has a prototype constructed and needs refinement in several areas in order to
increase its efficiency to determine if the system could ever reach a point of
feasibility in a residential application. Having put additional control refining
systems on the solar water heat collector, it can be deduced that the efficiency has
increased. However, due to limited testing and analysis it is undetermined just how
much the efficiency of the system has increased. At minimum, the capabilities of the
research platform have dramatically increased, allowing future research to more
accurately study the dynamics of the system as well as conduct studies in more
targeted areas of engineering. In this aspect, the thesis was successful.
ContributorsDonovan, Benjamin (Author) / Rajadas, John (Thesis advisor) / Kannan, Arunachala (Committee member) / Rogers, Bradley (Committee member) / Arizona State University (Publisher)
Created2016
Description
There was a growing trend in the automotive market on the adoption of Hybrid Electric Vehicles (HEVs) for consumers to purchase. This was partially due to external pressures such as the effects of global warming, cost of petroleum, governmental regulations, and popularity of the vehicle type. HEV technology relied on a variety of factors which included the powertrain (PT) of the system, external driving conditions, and the type of driving pattern being driven. The core foundation for HEVs depended heavily on the battery pack and chemistry being adopted for the vehicle performance and operations. This paper focused on the effects of hot and arid temperatures on the performance of LiFePO4 (LFP) battery packs and presented a possible modeling method for overall performance.
Lithium-ion battery (LIB) packs were subjected to room and high temperature settings while being cycled under a current profile created from a drive cycle. The Federal Urban Driving Schedule (FUDS) was selected and modified to simulate normal city driving situation using an electric only drive mode. Capacity and impedance fade of the LIB packs were monitored over the lifetime of the pack to determine the overall performance through the variables of energy and power fade. Regression analysis was done on the energy and power fade of the LIB pack to determine the duration life of LIB packs for HEV applications. This was done by comparing energy and power fade with the average lifetime mileage of a vehicle.
The collected capacity and impedance data was used to create an electrical equivalent model (EEM). The model was produced through the process of a modified Randles circuit and the creation of the inverse constant phase element (ICPE). Results indicated the model had a potential for high fidelity as long as a sufficient amount of data was gathered. X-ray powder diffraction (XRD) and a scanning electron microscope (SEM) was performed on a fresh and cycled LFP battery. SEM results suggested a dramatic growth on LFP crystals with a reduction in carbon coating after cycling. XRD effects showed a slight uniformed strain and decrease in size of LFP olivine crystals after cycling.
Lithium-ion battery (LIB) packs were subjected to room and high temperature settings while being cycled under a current profile created from a drive cycle. The Federal Urban Driving Schedule (FUDS) was selected and modified to simulate normal city driving situation using an electric only drive mode. Capacity and impedance fade of the LIB packs were monitored over the lifetime of the pack to determine the overall performance through the variables of energy and power fade. Regression analysis was done on the energy and power fade of the LIB pack to determine the duration life of LIB packs for HEV applications. This was done by comparing energy and power fade with the average lifetime mileage of a vehicle.
The collected capacity and impedance data was used to create an electrical equivalent model (EEM). The model was produced through the process of a modified Randles circuit and the creation of the inverse constant phase element (ICPE). Results indicated the model had a potential for high fidelity as long as a sufficient amount of data was gathered. X-ray powder diffraction (XRD) and a scanning electron microscope (SEM) was performed on a fresh and cycled LFP battery. SEM results suggested a dramatic growth on LFP crystals with a reduction in carbon coating after cycling. XRD effects showed a slight uniformed strain and decrease in size of LFP olivine crystals after cycling.
ContributorsOpitz, Andrew (Author) / Kannan, Arunachala (Thesis advisor) / Mayyas, Abdel (Committee member) / Nam, Changho (Committee member) / Arizona State University (Publisher)
Created2016
Description
Lithium ion batteries have emerged as the most popular energy storage system, but they pose safety issues under extreme temperatures or in the event of a thermal runaway. Lithium ion batteries with inorganic separators offer the advantage of safer operation. An inorganic separator for lithium ion battery was prepared by an improved method of blade coating α-Al2O3 slurry directly on the electrode followed by drying. The improved separator preparation involves a twice-coating process instead of coating the slurry all at once in order to obtain a thin (~40 µm) and uniform coat. It was also found that α-Al2O3 powder with particle size greater than the pore size in the electrode is preferable for obtaining a separator with 40 µm thickness and consistent cell performance. Unlike state-of-the-art polyolefin separators such as polypropylene (PP) which are selectively wettable with only certain electrolytes, the excellent electrolyte solvent wettability of α-Al2O3 allows the coated alumina separator to function with different electrolytes. The coated α-Al2O3 separator has a much higher resistance to temperature effects than its polyolefin counterparts, retaining its dimensional integrity at temperatures as high as 200ºC. This eliminates the possibility of a short circuit during thermal runaway. Lithium ion batteries assembled as half-cells and full cells with coated α-Al2O3 separator exhibit electrochemical performance comparable with that of polyolefin separators at room temperature. However, the cells with coated alumina separator shows better cycling performance under extreme temperatures in the temperature range of -30°C to 60°C. Therefore, the coated α-Al2O3 separator is very promising for application in safe lithium-ion batteries.
ContributorsSharma, Gaurav (Author) / Lin, Jerry Y.S. (Thesis advisor) / Chan, Candace (Committee member) / Kannan, Arunachala (Committee member) / Arizona State University (Publisher)
Created2016
Description
Determining the thermal conductivity of carbon gas diffusion layers used in hydrogen fuel cells is a very active topic of research. The primary driver behind this research is due to the need for development of proton exchange membrane fuels with longer usable life cycles before failure. As heat is a byproduct of the oxygen-hydrogen reaction an optimized pathway to remove the excess heat is needed to prevent thermal damage to the fuel cell as both mechanical and chemical degradation is accelerated under elevated temperatures. Commercial systems used for testing thermal conductivity are readily available, but are prohibitively expensive, ranging from just over $10,000 to $80,000 for high-end systems. As this cost can exclude some research labs from experimenting with thermal conductivity, a low cost alternative system is a desirable product. The development of a low cost system that maintained typical accuracy levels of commercials systems was carried out successfully at a significant cost reduction. The end product was capable of obtaining comparable accuracy to commercial systems at a cost reduction of more than 600% when compared to entry level commercial models. Combined with a system design that only required some basic fabrication equipment, this design will allow many research labs to expand their testing capabilities without straining departmental budgets. As expected with the development of low cost solutions, the reduction in cost came at the loss in other aspects of system performance, mainly run time. While the developed system requires a significate time investment to obtain useable results, the system can be improved by the used of RTDs in place of thermocouples or incorporation of an isothermal cold plate. These improvements would reduce the runtime to less than that of a standard work day while maintaining an approximate reduction in cost of 350%.
ContributorsSucher, Brent (Author) / Kannan, Arunachala (Thesis advisor) / Hsu, Keng (Committee member) / Nam, Changho (Committee member) / Arizona State University (Publisher)
Created2016
Description
Zinc oxide nanowires ( NWs) have broad applications in various fields such as nanoelectronics, optoelectronics, piezoelectric nanogenerators, chemical/biological sensors, and heterogeneous catalysis. To meet the requirements for broader applications, the growth of high-quality ZnO NWs and functionalization of ZnO NWs are critical. In this work, specific types of functionalized ZnO NWs have been synthesized and correlations between specific structures and properties have been investigated. Deposition of δ-Bi2O3 (narrow band gap) epilayers onto ZnO (wide band gap) NWs improves the absorption efficiency of the visible light spectrum by 70%. Furthermore, the deposited δ-Bi2O3 grows selectively and epitaxially on the {11-20} but not on the {10-10} facets of the ZnO NWs. The selective epitaxial deposition and the interfacial structure were thoroughly investigated. The morphology and structure of the Bi2O3/ZnO nanocomposites can be tuned by controlling the deposition conditions.
Various deposition methods, both physical and chemical, were used to functionalize the ZnO NWs with metal or alloy nanoparticles (NPs) for catalytic transformations of important molecules which are relevant to energy and environment. Cu and PdZn NPs were epitaxially grown on ZnO NWs to make them resistant to sintering at elevated temperatures and thus improved the stability of such catalytic systems for methanol steam reforming (MSR) to produce hydrogen. A series of Pd/ZnO catalysts with different Pd loadings were synthesized and tested for MSR reaction. The CO selectivity was found to be strongly dependent on the size of the Pd: Both PdZn alloy and single Pd atoms yield low CO selectivity while Pd clusters give the highest CO selectivity.
By dispersing single Pd atoms onto ZnO NWs, Pd1/ZnO single-atom catalysts (SACs) was synthesized and their catalytic performance was evaluated for selected catalytic reactions. The experimental results show that the Pd1/ZnO SAC is active for CO oxidation and MSR but is not desirable other reactions. We further synthesized ZnO NWs supported noble metal (M1/ZnO; M=Rh, Pd, Pt, Ir) SACs and studied their catalytic performances for CO oxidation. The catalytic test data shows that all the fabricated noble metal SACs are active for CO oxidation but their activity are significantly different. Structure-performance relationships were investigated.
Various deposition methods, both physical and chemical, were used to functionalize the ZnO NWs with metal or alloy nanoparticles (NPs) for catalytic transformations of important molecules which are relevant to energy and environment. Cu and PdZn NPs were epitaxially grown on ZnO NWs to make them resistant to sintering at elevated temperatures and thus improved the stability of such catalytic systems for methanol steam reforming (MSR) to produce hydrogen. A series of Pd/ZnO catalysts with different Pd loadings were synthesized and tested for MSR reaction. The CO selectivity was found to be strongly dependent on the size of the Pd: Both PdZn alloy and single Pd atoms yield low CO selectivity while Pd clusters give the highest CO selectivity.
By dispersing single Pd atoms onto ZnO NWs, Pd1/ZnO single-atom catalysts (SACs) was synthesized and their catalytic performance was evaluated for selected catalytic reactions. The experimental results show that the Pd1/ZnO SAC is active for CO oxidation and MSR but is not desirable other reactions. We further synthesized ZnO NWs supported noble metal (M1/ZnO; M=Rh, Pd, Pt, Ir) SACs and studied their catalytic performances for CO oxidation. The catalytic test data shows that all the fabricated noble metal SACs are active for CO oxidation but their activity are significantly different. Structure-performance relationships were investigated.
ContributorsXu, Jia, Ph.D (Author) / Liu, Jingyue (Thesis advisor) / Smith, David (Committee member) / Chan, Candace (Committee member) / Mu, Bin (Committee member) / Arizona State University (Publisher)
Created2017
Description
Delamination of solar module interfaces often occurs in field-tested solar modules after decades of service due to environmental stressors such as humidity. In the presence of water, the interfaces between the encapsulant and the cell, glass, and backsheet all experience losses of adhesion, exposing the module to accelerated degradation. Understanding the relation between interfacial adhesion and water content inside photovoltaic modules can help mitigate detrimental power losses. Water content measurements via water reflectometry detection combined with 180° peel tests were used to study adhesion of module materials exposed to damp heat and dry heat conditions. The effect of temperature, cumulative water dose, and water content on interfacial adhesion between ethylene vinyl acetate and (1) glass, (2) front of the cell, and (3) backsheet was studied. Temperature and time decreased adhesion at all these interfaces. Water content in the sample during the measurement showed significant decreases in adhesion for the Backsheet/Ethylene vinyl acetate interface. Water dose showed little effect for the Glass/ Ethylene vinyl acetate and Backsheet/ Ethylene vinyl acetate interfaces, but there was significant adhesion loss with water dose at the front cell busbar/encapsulant interface. Initial tensile test results to monitor the effects of the mechanical properties ethylene vinyl acetate and backsheet showed water content increasing the strength of ethylene vinyl acetate during plastic deformation but no change in the strength of the backsheet properties. This mechanical property change is likely inducing variation along the peel interface to possibly convolute the adhesion measurements conducted or to explain the variation seen for the water saturated and dried peel test sample types.
ContributorsTheut, Nicholas (Author) / Bertoni, Mariana (Thesis advisor) / Holman, Zachary (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2020