ASU Electronic Theses and Dissertations
This collection includes most of the ASU Theses and Dissertations from 2011 to present. ASU Theses and Dissertations are available in downloadable PDF format; however, a small percentage of items are under embargo. Information about the dissertations/theses includes degree information, committee members, an abstract, supporting data or media.
In addition to the electronic theses found in the ASU Digital Repository, ASU Theses and Dissertations can be found in the ASU Library Catalog.
Dissertations and Theses granted by Arizona State University are archived and made available through a joint effort of the ASU Graduate College and the ASU Libraries. For more information or questions about this collection contact or visit the Digital Repository ETD Library Guide or contact the ASU Graduate College at gradformat@asu.edu.
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- All Subjects: nanotechnology
Description
In-situ environmental transmission electron microscopy (ETEM) is a powerful tool for following the evolution of supported metal nanoparticles under different reacting gas conditions at elevated temperatures. The ability to observe the events in real time under reacting gas conditions can provide significant information on the fundamental processes taking place in catalytic materials, from which the performance of the catalyst can be understood. The first part of this dissertation presents the application of in-situ ETEM studies in developing structure-activity relationship in supported metal nanoparticles. In-situ ETEM studies on nanostructures in parallel with ex-situ reactor studies of conversions and selectivities were performed for partial oxidation of methane (POM) to syngas (CO+H2) on Ni/SiO2, Ru/SiO2 and NiRu/SiO2 catalysts. During POM, the gas composition varies along the catalyst bed with increasing temperature. It is important to consider these variations in gas composition in order to design experiments for in-situ ETEM. In-situ ETEM experiments were performed under three different reacting gas conditions. First in the presence of H2, this represents the state of the fresh catalyst for the catalytic reaction. Later in the presence of CH4 and O2 in 2:1 ratio, this is the composition of the reacting gases for the POM reaction and this composition acts as an oxidizing environment. Finally in the presence of CH4, this is the reducing gas. Oxidation and reduction behavior of Ni, Ru and NiRu nanoparticles were followed in an in-situ ETEM under reacting gas conditions and the observations were correlated with the performance of the catalyst for POM. The later part of the dissertation presents a technique for determining the gas compositional analysis inside the in-situ ETEM using electron energy-loss spectroscopy. Techniques were developed to identify the gas composition using both inner-shell and low-loss spectroscopy of EELS. Using EELS, an "operando TEM" technique was successfully developed for detecting the gas phase catalysis inside the ETEM. Overall this research demonstrates the importance of in-situ ETEM studies in understanding the structure-activity relationship in supported-metal catalysts for heterogeneous catalysis application.
ContributorsChenna, Santhosh (Author) / Crozier, Peter A. (Thesis advisor) / Carpenter, Ray (Committee member) / Sieradzki, Karl (Committee member) / Petuskey, William (Committee member) / Arizona State University (Publisher)
Created2011
Description
Lithium-ion batteries can fail and catch fire when overcharged, exposed to high temperatures or short-circuited due to the highly flammable organic liquid used in the electrolyte. Using inorganic solid electrolyte materials can potentially improve the safety factor. Additionally, nanostructured electrolyte materials may further enhanced performance by taking advantage of their large aspect ratio. In this work, the synthesis of two promising nanostructured solid electrolyte materials was explored. Amorphous lithium niobate nanowires were synthesized through the decomposition of a niobium-containing complex in a structure-directing solvent using a reflux method. Lithium lanthanum titanate was obtained via solid state reaction with titanium oxide nanowires as the titanium precursor, but the nanowire morphology could not be preserved due to high temperature sintering. Hyperbranched potassium lanthanum titanate was synthesized through hydrothermal route. This was the first time that hyperbranched nanowires with perovskite structure were made without any catalyst or substrate. This result has the potential to be applied to other perovskite materials.
ContributorsYang, Ting (Author) / Chan, Candace K. (Thesis advisor) / Crozier, Peter A. (Committee member) / Sieradzki, Karl (Committee member) / Arizona State University (Publisher)
Created2012
Description
In recent years, the scientific community around the synthesis and processing of nanoporous metals is striving to integrate them into powder metallurgy processes such as additive manufacturing since it has a potential to fabricate 3D hierarchical high surface area electrodes for energy applications. Recent research in dealloying – a versatile method for synthesizing nanoporous metals – emphasized the need in understanding its process-structure relationships to independently control the relative density, ligament and pore sizes with good process reproducibly. In this dissertation, a new understanding of the dealloying process is presented for synthesizing (i) nanoporous gold thin-films and (ii) nanoporous Cu spherical powders with an emphasis on understanding variability in their process-structure relationships and process scalability. First, this work sheds the light on the nature of the dealloying front and its percolation along the grain boundaries in nanocrystalline gold-silver thin films by studying the early stages of ligament nucleation. Additionally, this work analyses its variability by investigating new process variables such as (i) equilibration time and (ii) precursor aging and their impacts in achieving process reproducibility. The correlation of relative density with ligament size is contextualized with state-of-the-art data mining research. Second, this work provides a new methodology for large scale production of nanoporous Cu powder and demonstrates its integration with powder casting to fabricate porous conductive electrode. By understanding the influence of etching solution concentration and titration methodology on the structure and composition of nanoporous Cu, it was possible to fabricate precipitate-free powders at high throughputs. Further, the nature of oxygen incorporation into porous Cu powder was studied as a function of surface-to-volume ratio of powder in atmospheric conditions. To consolidate powders into parts via open-die casting, this work harvests Ostwald Ripening phenomena associated with thermal coarsening in nanoporous metals to weld them at low temperatures (approximately one-third of its melting temperature). This work represents a major step towards the integration of nanoporous Cu feedstocks into additive manufacturing.
ContributorsNiauzorau, Stanislau (Author) / Azeredo, Bruno (Thesis advisor) / Sieradzki, Karl (Committee member) / Song, Kenan (Committee member) / Chawla, Nikhilesh (Committee member) / Arizona State University (Publisher)
Created2022