Theses and Dissertations
This collection includes both ASU Theses and Dissertations, submitted by graduate students, and the Barrett, Honors College theses submitted by undergraduate students.
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- Creators: Anderson, Matthew Brandon
- Creators: Carpenter, Ray
Description
Emission of CO2 into the atmosphere has become an increasingly concerning issue as we progress into the 21st century Flue gas from coal-burning power plants accounts for 40% of all carbon dioxide emissions. The key to successful separation and sequestration is to separate CO2 directly from flue gas (10-15% CO2, 70% N2), which can range from a few hundred to as high as 1000°C. Conventional microporous membranes (carbons/silicas/zeolites) are capable of separating CO2 from N2 at low temperatures, but cannot achieve separation above 200°C. To overcome the limitations of microporous membranes, a novel ceramic-carbonate dual-phase membrane for high temperature CO2 separation was proposed. The membrane was synthesized from porous La0.6Sr0.4Co0.8Fe0.2O3-d (LSCF) supports and infiltrated with molten carbonate (Li2CO3/Na2CO3/K2CO3). The CO2 permeation mechanism involves a reaction between CO2 (gas phase) and O= (solid phase) to form CO3=, which is then transported through the molten carbonate (liquid phase) to achieve separation. The effects of membrane thickness, temperature and CO2 partial pressure were studied. Decreasing thickness from 3.0 to 0.375 mm led to higher fluxes at 900°C, ranging from 0.186 to 0.322 mL.min-1.cm-2 respectively. CO2 flux increased with temperature from 700 to 900°C. Activation energy for permeation was similar to that for oxygen ion conduction in LSCF. For partial pressures above 0.05 atm, the membrane exhibited a nearly constant flux. From these observations, it was determined that oxygen ion conductivity limits CO2 permeation and that the equilibrium oxygen vacancy concentration in LSCF is dependent on the partial pressure of CO2 in the gas phase. Finally, the dual-phase membrane was used as a membrane reactor. Separation at high temperatures can produce warm, highly concentrated streams of CO2 that could be used as a chemical feedstock for the synthesis of syngas (H2 + CO). Towards this, three different membrane reactor configurations were examined: 1) blank system, 2) LSCF catalyst and 3) 10% Ni/y-alumina catalyst. Performance increased in the order of blank system < LSCF catalyst < Ni/y-alumina catalyst. Favorable conditions for syngas production were high temperature (850°C), low sweep gas flow rate (10 mL.min-1) and high methane concentration (50%) using the Ni/y-alumina catalyst.
ContributorsAnderson, Matthew Brandon (Author) / Lin, Jerry (Thesis advisor) / Alford, Terry (Committee member) / Rege, Kaushal (Committee member) / Anderson, James (Committee member) / Rivera, Daniel (Committee member) / Arizona State University (Publisher)
Created2011
Description
Soft magnetic alloys play a significant role for magnetic recording applications and highly sensitivity magnetic field sensors. In order to sustain the magnetic areal density growth, development of new synthesis techniques and materials is necessary. In this work, the effect of oxygen incorporation during electrodeposition of CoFe alloys on magnetic properties, magnetoresistance and structural properties has been studied. Understanding the magnetic properties often required knowledge of oxygen distribution and structural properties of the grown films. Transmission electron microscopy (TEM) was a powerful tool in this study to correlate the oxygen-distribution nanostructure to the magnetic properties of deposited films. Off-axis electron holography in TEM was used to measure magnetic domain wall width in the deposited films. Elemental depth profiles of Fe, Co, O were investigated by secondary ion mass spectroscopy (SIMS). Magnetic properties have been determined by superconducting quantum interference device (SQUID) measurements. Oxygen content in the CoFe deposited films was controlled by electrolyte composition. Films were deposited on Si 100 substrates and on other substrates such as Cu and Al. However, a good film quality was achieved on Si substrate. Electron energy loss and x-ray spectroscopies showed that the low oxygen films contained intragranular Fe2+ oxide (FeO) particles and that the high oxygen films contained intergranular Fe3+ (Fe2O3) along grain boundaries. The films with oxide present at the grain boundary had significantly increased coercivity, magnetoresistance and reduced saturation magnetization relative to the lower oxygen content films with intragranular oxide. The differences in magnetic properties between low oxygen and high oxygen concentration films were attributed to stronger mobile domain wall interactions with the grain boundary oxide layers. The very high magnetoresistance values were achieved for magnetic devices with nanocontact dimension < 100 nm and oxide incorporation in this nanoconfined geometry. The content of oxide phase in nanocontact was controlled by concentration of the Fe3+ ions in the electrodeposition solution. Magnetic device integrity was improved by varying amount of additive into plating solution. These results indicated that electrodeposited CoFe nanocontact is a novel class of materials with large application for magnetic field sensors.
ContributorsElhalawaty, Shereen (Author) / Carpenter, Ray (Thesis advisor) / Chamberlin, Ralph (Committee member) / McCartney, Martha (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2012