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Description
Ordered mesoporous materials have tunable pore sizes between 2 and 50 nm and are characterized by ordered pore structures and high surface areas (~1000 m2/g). This makes them particularly favorable for a number of membrane applications such as protein separation, polymer extrusion, nanowire fabrication and membrane reactors. These membranes can be fabricated as top-layers on macroporous supports or as embedded membranes in a dense matrix. The first part of the work deals with the hydrothermal synthesis and water-vapor/oxygen separation properties of supported MCM-48 and a new Al-MCM-48 type membrane for potential use in air conditioning systems. Knudsen-type permeation is observed in these membranes. The combined effect of capillary condensation and the aluminosilicate matrix resulted in the highest separation factor (142) in Al-MCM-48 membranes, with a water vapor permeance of 6×10-8mol/m2Pas. The second part focuses on synthesis of embedded mesoporous silica membranes with helically ordered pores by a novel Counter Diffusion Self-Assembly (CDSA) method. This method is an extension of the interfacial synthesis method for fiber synthesis using tetrabutylorthosilicate (TBOS) and cetyltrimethylammonium bromide (CTAB) as the silica source and surfactant respectively. The initial part of this study determined the effect of TBOS height and humidity on fiber formation. From this study, the range of TBOS heights for best microscopic and macroscopic ordering were established. Next, the CDSA method was used to successfully synthesize membranes, which were characterized to have good support plugging and an ordered pore structure. Factors that influence membrane synthesis and plug microstructure were determined. SEM studies revealed the presence of gaps between the plugs and support pores, which occur due to shrinking of the plug on drying. Development of a novel liquid deposition method to seal these defects constituted the last part of this work. Post sealing, excess silica was removed by etching with hydrofluoric acid. Membrane quality was evaluated at each step using SEM and gas permeation measurements. After surfactant removal by liquid extraction, the membranes exhibited an O2 permeance of 1.65x10-6mol/m2.Pa.s and He/O2 selectivity of 3.30. The successful synthesis of this membrane is an exciting new development in the area of ordered mesoporous membrane technology.
ContributorsSeshadri, Shriya (Author) / Lin, Jerry Y. S. (Thesis advisor) / Dai, Lenore (Committee member) / Rege, Kaushal (Committee member) / Smith, David J. (Committee member) / Vogt, Bryan (Committee member) / Arizona State University (Publisher)
Created2011
Description
Locomotion of microorganisms is commonly observed in nature. Although microorganism locomotion is commonly attributed to mechanical deformation of solid appendages, in 1956 Nobel Laureate Peter Mitchell proposed that an asymmetric ion flux on a bacterium's surface could generate electric fields that drive locomotion via self-electrophoresis. Recent advances in nanofabrication have enabled the engineering of synthetic analogues, bimetallic colloidal particles, that swim due to asymmetric ion flux originally proposed by Mitchell. Bimetallic colloidal particles swim through aqueous solutions by converting chemical fuel to fluid motion through asymmetric electrochemical reactions. This dissertation presents novel bimetallic motor fabrication strategies, motor functionality, and a study of the motor collective behavior in chemical concentration gradients. Brownian dynamics simulations and experiments show that the motors exhibit chemokinesis, a motile response to chemical gradients that results in net migration and concentration of particles. Chemokinesis is typically observed in living organisms and distinct from chemotaxis in that there is no particle directional sensing. The synthetic motor chemokinesis observed in this work is due to variation in the motor's velocity and effective diffusivity as a function of the fuel and salt concentration. Static concentration fields are generated in microfluidic devices fabricated with porous walls. The development of nanoscale particles that swim autonomously and collectively in chemical concentration gradients can be leveraged for a wide range of applications such as directed drug delivery, self-healing materials, and environmental remediation.
ContributorsWheat, Philip Matthew (Author) / Posner, Jonathan D (Thesis advisor) / Phelan, Patrick (Committee member) / Chen, Kangping (Committee member) / Buttry, Daniel (Committee member) / Calhoun, Ronald (Committee member) / Arizona State University (Publisher)
Created2011
Description
III-nitride alloys are wide band gap semiconductors with a broad range of applications in optoelectronic devices such as light emitting diodes and laser diodes. Indium gallium nitride light emitting diodes have been successfully produced over the past decade. But the progress of green emission light emitting devices has been limited by the incorporation of indium in the alloy, mainly due to phase separation. This difficulty could be addressed by studying the growth and thermodynamics of these alloys. Knowledge of thermodynamic phase stabilities and of pressure - temperature - composition phase diagrams is important for an understanding of the boundary conditions of a variety of growth techniques. In this dissertation a study of the phase separation of indium gallium nitride is conducted using a regular solution model of the ternary alloy system. Graphs of Gibbs free energy of mixing were produced for a range of temperatures. Binodal and spinodal decomposition curves show the stable and unstable regions of the alloy in equilibrium. The growth of gallium nitride and indium gallium nitride was attempted by the reaction of molten gallium - indium alloy with ammonia at atmospheric pressure. Characterization by X-ray diffraction, photoluminescence, and secondary electron microscopy show that the samples produced by this method contain only gallium nitride in the hexagonal phase. The instability of indium nitride at the temperatures required for activation of ammonia accounts for these results. The photoluminescence spectra show a correlation between the intensity of a broad green emission, related to native defects, and indium composition used in the molten alloy. A different growth method was used to grow two columnar-structured gallium nitride films using ammonium chloride and gallium as reactants and nitrogen and ammonia as carrier gasses. Investigation by X-ray diffraction and spatially-resolved cathodoluminescence shows the film grown at higher temperature to be primarily hexagonal with small quantities of cubic crystallites, while the one grown at lower temperature to be pure hexagonal. This was also confirmed by low temperature photoluminescence measurements. The results presented here show that cubic and hexagonal crystallites can coexist, with the cubic phase having a much sharper and stronger luminescence. Controlled growth of the cubic phase GaN crystallites can be of use for high efficiency light detecting and emitting devices. The ammonolysis of a precursor was used to grow InGaN powders with different indium composition. High purity hexagonal GaN and InN were obtained. XRD spectra showed complete phase separation for samples with x < 30%, with ~ 9% indium incorporation in the 30% sample. The presence of InGaN in this sample was confirmed by PL measurements, where luminescence from both GaN and InGaN band edge are observed. The growth of higher indium compositions samples proved to be difficult, with only the presence of InN in the sample. Nonetheless, by controlling parameters like temperature and time may lead to successful growth of this III-nitride alloy by this method.
ContributorsHill, Arlinda (Author) / Ponce, Fernando A. (Thesis advisor) / Chamberlin, Ralph V (Committee member) / Sankey, Otto F (Committee member) / Smith, David J. (Committee member) / Tsen, Kong-Thon (Committee member) / Arizona State University (Publisher)
Created2011
Description
The demand for handheld portable computing in education, business and research has resulted in advanced mobile devices with powerful processors and large multi-touch screens. Such devices are capable of handling tasks of moderate computational complexity such as word processing, complex Internet transactions, and even human motion analysis. Apple's iOS devices, including the iPhone, iPod touch and the latest in the family - the iPad, are among the well-known and widely used mobile devices today. Their advanced multi-touch interface and improved processing power can be exploited for engineering and STEM demonstrations. Moreover, these devices have become a part of everyday student life. Hence, the design of exciting mobile applications and software represents a great opportunity to build student interest and enthusiasm in science and engineering. This thesis presents the design and implementation of a portable interactive signal processing simulation software on the iOS platform. The iOS-based object-oriented application is called i-JDSP and is based on the award winning Java-DSP concept. It is implemented in Objective-C and C as a native Cocoa Touch application that can be run on any iOS device. i-JDSP offers basic signal processing simulation functions such as Fast Fourier Transform, filtering, spectral analysis on a compact and convenient graphical user interface and provides a very compelling multi-touch programming experience. Built-in modules also demonstrate concepts such as the Pole-Zero Placement. i-JDSP also incorporates sound capture and playback options that can be used in near real-time analysis of speech and audio signals. All simulations can be visually established by forming interactive block diagrams through multi-touch and drag-and-drop. Computations are performed on the mobile device when necessary, making the block diagram execution fast. Furthermore, the extensive support for user interactivity provides scope for improved learning. The results of i-JDSP assessment among senior undergraduate and first year graduate students revealed that the software created a significant positive impact and increased the students' interest and motivation and in understanding basic DSP concepts.
ContributorsLiu, Jinru (Author) / Spanias, Andreas (Thesis advisor) / Tsakalis, Kostas (Committee member) / Qian, Gang (Committee member) / Arizona State University (Publisher)
Created2011
Description
In this work, a novel method is developed for making nano- and micro- fibrous hydrogels capable of preventing the rejection of implanted materials. This is achieved by either (1) mimicking the native cellular environment, to exert fine control over the cellular response or (2) acting as a protective barrier, to camouflage the foreign nature of a material and evade recognition by the immune system. Comprehensive characterization and in vitro studies described here provide a foundation for developing substrates for use in clinical applications. Hydrogel dextran and poly(acrylic acid) (PAA) fibers are formed via electrospinning, in sizes ranging from nanometers to microns in diameter. While "as-electrospun" fibers are continuous in length, sonication is used to fragment fibers into short fiber "bristles" and generate nano- and micro- fibrous surface coatings over a wide range of topographies. Dex-PAA fibrous surfaces are chemically modified, and then optimized and characterized for non-fouling and ECM-mimetic properties. The non-fouling nature of fibers is verified, and cell culture studies show differential responses dependent upon chemical, topographical and mechanical properties. Dex-PAA fibers are advantageously unique in that (1) a fine degree of control is possible over three significant parameters critical for modifying cellular response: topography, chemistry and mechanical properties, over a range emulating that of native cellular environments, (2) the innate nature of the material is non-fouling, providing an inert background for adding back specific bioactive functionality, and (3) the fibers can be applied as a surface coating or comprise the scaffold itself. This is the first reported work of dex-PAA hydrogel fibers formed via electrospinning and thermal cross-linking, and unique to this method, no toxic solvents or cross-linking agents are needed to create hydrogels or for surface attachment. This is also the first reported work of using sonication to fragment electrospun hydrogel fibers, and in which surface coatings were made via simple electrostatic interaction and dehydration. These versatile features enable fibrous surface coatings to be applied to virtually any material. Results of this research broadly impact the design of biomaterials which contact cells in the body by directing the consequent cell-material interaction.
ContributorsLouie, Katherine BoYook (Author) / Massia, Stephen P (Thesis advisor) / Bennett, Kevin (Committee member) / Garcia, Antonio (Committee member) / Pauken, Christine (Committee member) / Vernon, Brent (Committee member) / Arizona State University (Publisher)
Created2011
Description
Due to the growing concerns on the depletion of petroleum based energy resources and climate change; fuel cell technologies have received much attention in recent years. Proton exchange membrane fuel cell (PEMFCs) features high energy conversion efficiency and nearly zero greenhouse gas emissions, because of its combination of the hydrogen oxidation reaction (HOR) at anode side and oxygen reduction reaction (ORR) at cathode side. Synthesis of Pt nanoparticles supported on multi walled carbon nanotubes (MWCNTs) possess a highly durable electrochemical surface area (ESA) and show good power output on proton exchange membrane (PEM) fuel cell performance. Platinum on multi-walled carbon nanotubes (MWCNTs) support were synthesized by two different processes to transfer PtCl62- from aqueous to organic phase. While the first method of Pt/MWCNTs synthesis involved dodecane thiol (DDT) and octadecane thiol (ODT) as anchoring agent, the second method used ammonium lauryl sulfate (ALS) as the dispersion/anchoring agent. The particle size and distribution of platinum were examined by high-resolution transmission electron microscope (HRTEM). The TEM images showed homogenous distribution and uniform particle size of platinum deposited on the surface of MWCNTs. The single cell fuel cell performance of the Pt/MWCNTs synthesized thiols and ALS based electrode containing 0.2 (anode) and 0.4 mg (cathode) Pt.cm-2 were evaluated using Nafion-212 electrolyte with H2 and O2 gases at 80 oC and ambient pressure. The catalyst synthesis with ALS is relatively simple compared to that with thiols and also showed higher performance (power density reaches about 1070 mW.cm-2). The Electrodes with Pt/MWCNTs nanocatalysts synthesized using ALS were characterized by cyclic voltammetry (CV) for durability evaluation using humidified H2 and N2 gases at room temperature (21 oC) along with commercial Pt/C for comparison. The ESA measured by cyclic voltammetry between 0.15 and 1.2 V showed significant less degradation after 1000 cycles for ALS based Pt/MWCNTs.
ContributorsLiu, Xuan (Author) / Madakannan, Arunachalanadar (Thesis advisor) / Munukutla, Lakshmi (Committee member) / Tamizhmani, Govindasamy (Committee member) / Arizona State University (Publisher)
Created2011
Description
Microchannel heat sinks can possess heat transfer characteristics unavailable in conventional heat exchangers; such sinks offer compact solutions to otherwise intractable thermal management problems, notably in small-scale electronics cooling. Flow boiling in microchannels allows a very high heat transfer rate, but is bounded by the critical heat flux (CHF). This thesis presents a theoretical-numerical study of a method to improve the heat rejection capability of a microchannel heat sink via expansion of the channel cross-section along the flow direction. The thermodynamic quality of the refrigerant increases during flow boiling, decreasing the density of the bulk coolant as it flows. This may effect pressure fluctuations in the channels, leading to nonuniform heat transfer and local dryout in regions exceeding CHF. This undesirable phenomenon is counteracted by permitting the cross-section of the microchannel to increase along the direction of flow, allowing more volume for the vapor. Governing equations are derived from a control-volume analysis of a single heated rectangular microchannel; the cross-section is allowed to expand in width and height. The resulting differential equations are solved numerically for a variety of channel expansion profiles and numbers of channels. The refrigerant is R-134a and channel parameters are based on a physical test bed in a related experiment. Significant improvement in CHF is possible with moderate area expansion. Minimal additional manufacturing costs could yield major gains in the utility of microchannel heat sinks. An optimum expansion rate occurred in certain cases, and alterations in the channel width are, in general, more effective at improving CHF than alterations in the channel height. Modest expansion in height enables small width expansions to be very effective.
ContributorsMiner, Mark (Author) / Phelan, Patrick E (Thesis advisor) / Herrmann, Marcus (Committee member) / Chen, Kangping (Committee member) / Arizona State University (Publisher)
Created2011
Description
Residue number systems have gained significant importance in the field of high-speed digital signal processing due to their carry-free nature and speed-up provided by parallelism. The critical aspect in the application of RNS is the selection of the moduli set and the design of the conversion units. There have been several RNS moduli sets proposed for the implementation of digital filters. However, some are unbalanced and some do not provide the required dynamic range. This thesis addresses the drawbacks of existing RNS moduli sets and proposes a new moduli set for efficient implementation of FIR filters. An efficient VLSI implementation model has been derived for the design of a reverse converter from RNS to the conventional two's complement representation. This model facilitates the realization of a reverse converter for better performance with less hardware complexity when compared with the reverse converter designs of the existing balanced 4-moduli sets. Experimental results comparing multiply and accumulate units using RNS that are implemented using the proposed four-moduli set with the state-of-the-art balanced four-moduli sets, show large improvements in area (46%) and power (43%) reduction for various dynamic ranges. RNS FIR filters using the proposed moduli-set and existing balanced 4-moduli set are implemented in RTL and compared for chip area and power and observed 20% improvements. This thesis also presents threshold logic implementation of the reverse converter.
ContributorsChalivendra, Gayathri (Author) / Vrudhula, Sarma (Thesis advisor) / Shrivastava, Aviral (Committee member) / Bakkaloglu, Bertan (Committee member) / Arizona State University (Publisher)
Created2011
Description
Ge1-ySny alloys represent a new class of photonic materials for integrated optoelectronics on Si. In this work, the electrical and optical properties of Ge1-ySny alloy films grown on Si, with concentrations in the range 0 ≤ y ≤ 0.04, are studied via a variety of methods. The first microelectronic devices from GeSn films were fabricated using newly developed CMOS-compatible protocols, and the devices were characterized with respect to their electrical properties and optical response. The detectors were found to have a detection range that extends into the near-IR, and the detection edge is found to shift to longer wavelengths with increasing Sn content, mainly due to the compositional dependence of the direct band gap E0. With only 2 % Sn, all of the telecommunication bands are covered by a single detector. Room temperature photoluminescence was observed from GeSn films with Sn content up to 4 %. The peak wavelength of the emission was found to shift to lower energies with increasing Sn content, corresponding to the decrease in the direct band gap E0 of the material. An additional peak in the spectrum was assigned to the indirect band gap. The separation between the direct and indirect peaks was found to decrease with increasing Sn concentration, as expected. Electroluminescence was also observed from Ge/Si and Ge0.98Sn0.02 photodiodes under forward bias, and the luminescence spectra were found to match well with the observed photoluminescence spectra. A theoretical expression was developed for the luminescence due to the direct band gap and fit to the data.
ContributorsMathews, Jay (Author) / Menéndez, Jose (Thesis advisor) / Kouvetakis, John (Thesis advisor) / Drucker, Jeffery (Committee member) / Chizmeshya, Andrew (Committee member) / Ponce, Fernando (Committee member) / Arizona State University (Publisher)
Created2011
Description
Proton exchange membrane fuel cells (PEMFCs) run on pure hydrogen and oxygen (or air), producing electricity, water, and some heat. This makes PEMFC an attractive option for clean power generation. PEMFCs also operate at low temperature which makes them quick to start up and easy to handle. PEMFCs have several important limitations which must be overcome before commercial viability can be achieved. Active areas of research into making them commercially viable include reducing the cost, size and weight of fuel cells while also increasing their durability and performance. A growing and important part of this research involves the computer modeling of fuel cells. High quality computer modeling and simulation of fuel cells can help speed up the discovery of optimized fuel cell components. Computer modeling can also help improve fundamental understanding of the mechanisms and reactions that take place within the fuel cell. The work presented in this thesis describes a procedure for utilizing computer modeling to create high quality fuel cell simulations using Ansys Fluent 12.1. Methods for creating computer aided design (CAD) models of fuel cells are discussed. Detailed simulation parameters are described and emphasis is placed on establishing convergence criteria which are essential for producing consistent results. A mesh sensitivity study of the catalyst and membrane layers is presented showing the importance of adhering to strictly defined convergence criteria. A study of iteration sensitivity of the simulation at low and high current densities is performed which demonstrates the variance in the rate of convergence and the absolute difference between solution values derived at low numbers of iterations and high numbers of iterations.
ContributorsArvay, Adam (Author) / Madakannan, Arunachalanadar (Thesis advisor) / Peng, Xihong (Committee member) / Liang, Yong (Committee member) / Subach, James (Committee member) / Arizona State University (Publisher)
Created2011