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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- All Subjects: Carbon Dioxide
- All Subjects: MOS Capacitor
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
Of the potential technologies for pre-combustion capture, membranes offer the advantages of being temperature resistant, able to handle large flow rates, and having a relatively small footprint. A significant amount of research has centered on the use of polymeric and microporous inorganic membranes to separate CO2. These membranes, however, have limitations at high temperature resulting in poor permeation performance. To address these limitations, the use of a dense dual-phase membrane has been studied. These membranes are composed of conductive solid and conductive liquid phases that have the ability to selectively permeate CO2 by forming carbonate ions that diffuse through the membrane at high temperature. The driving force for transport through the membrane is a CO2 partial pressure gradient. The membrane provides a theoretically infinite selectivity. To address stability of the ceramic-carbonate dual-phase membrane for CO2 capture at high temperature, the ceramic phase of the membrane was studied and replaced with materials previously shown to be stable in harsh conditions. The permeation properties and stability of La0.6Sr0.4Co0.8Fe0.2O3-δ (LSCF)-carbonate, La0.85Ce0.1Ga0.3Fe0.65Al0.05O3-δ (LCGFA)-carbonate, and Ce0.8Sm0.2O1.9 (SDC)-carbonate membranes were examined under a wide range of experimental conditions at high temperature. LSCF-carbonate membranes were shown to be unstable without the presence of O2 due to reaction of CO2 with the ceramic phase. In the presence of O2, however, the membranes showed stable permeation behavior for more than one month at 900oC. LCGFA-carbonate membranes showed great chemical and permeation stability in the presence of various conditions including exposure to CH4 and H2, however, the permeation performance was quite low when compared to membranes in the literature. Finally, SDC-carbonate membranes showed great chemical and permeation stability both in a CO2:N2 environment for more than two weeks at 900oC as well as more than one month of exposure to simulated syngas conditions at 700oC. Ceramic phase chemical stability increased in the order of LSCF < LCGFA < SDC while permeation performance increased in the order of LCGFA < LSCF < SDC.
ContributorsNorton, Tyler (Author) / Lin, Jerry Y.S. (Thesis advisor) / Alford, Terry (Committee member) / Lind, Mary Laura (Committee member) / Smith, David (Committee member) / Torres, Cesar (Committee member) / Arizona State University (Publisher)
Created2013
Description
Total dose sensing systems (or radiation detection systems) have many applications,
ranging from survey monitors used to supervise the generated radioactive waste at
nuclear power plants to personal dosimeters which measure the radiation dose
accumulated in individuals. This dissertation work will present two different types of
novel devices developed at Arizona State University for total dose sensing applications.
The first detector technology is a mechanically flexible metal-chalcogenide glass (ChG)
based system which is fabricated on low cost substrates and are intended as disposable
total dose sensors. Compared to existing commercial technologies, these thin film
radiation sensors are simpler in form and function, and cheaper to produce and operate.
The sensors measure dose through resistance change and are suitable for applications
such as reactor dosimetry, radiation chemistry, and clinical dosimetry. They are ideal for
wearable devices due to the lightweight construction, inherent robustness to resist
breaking when mechanically stressed, and ability to attach to non-flat objects. Moreover,
their performance can be easily controlled by tuning design variables and changing
incorporated materials. The second detector technology is a wireless dosimeter intended
for remote total dose sensing. They are based on a capacitively loaded folded patch
antenna resonating in the range of 3 GHz to 8 GHz for which the load capacitance varies
as a function of total dose. The dosimeter does not need power to operate thus enabling
its use and implementation in the field without requiring a battery for its read-out. As a
result, the dosimeter is suitable for applications such as unattended detection systems
destined for covert monitoring of merchandise crossing borders, where nuclear material
tracking is a concern. The sensitive element can be any device exhibiting a known
variation of capacitance with total ionizing dose. The sensitivity of the dosimeter is
related to the capacitance variation of the radiation sensitive device as well as the high
frequency system used for reading. Both technologies come with the advantage that they
are easy to manufacture with reasonably low cost and sensing can be readily read-out.
ranging from survey monitors used to supervise the generated radioactive waste at
nuclear power plants to personal dosimeters which measure the radiation dose
accumulated in individuals. This dissertation work will present two different types of
novel devices developed at Arizona State University for total dose sensing applications.
The first detector technology is a mechanically flexible metal-chalcogenide glass (ChG)
based system which is fabricated on low cost substrates and are intended as disposable
total dose sensors. Compared to existing commercial technologies, these thin film
radiation sensors are simpler in form and function, and cheaper to produce and operate.
The sensors measure dose through resistance change and are suitable for applications
such as reactor dosimetry, radiation chemistry, and clinical dosimetry. They are ideal for
wearable devices due to the lightweight construction, inherent robustness to resist
breaking when mechanically stressed, and ability to attach to non-flat objects. Moreover,
their performance can be easily controlled by tuning design variables and changing
incorporated materials. The second detector technology is a wireless dosimeter intended
for remote total dose sensing. They are based on a capacitively loaded folded patch
antenna resonating in the range of 3 GHz to 8 GHz for which the load capacitance varies
as a function of total dose. The dosimeter does not need power to operate thus enabling
its use and implementation in the field without requiring a battery for its read-out. As a
result, the dosimeter is suitable for applications such as unattended detection systems
destined for covert monitoring of merchandise crossing borders, where nuclear material
tracking is a concern. The sensitive element can be any device exhibiting a known
variation of capacitance with total ionizing dose. The sensitivity of the dosimeter is
related to the capacitance variation of the radiation sensitive device as well as the high
frequency system used for reading. Both technologies come with the advantage that they
are easy to manufacture with reasonably low cost and sensing can be readily read-out.
ContributorsMahmud, Adnan, Ph.D (Author) / Barnaby, Hugh J. (Thesis advisor) / Kozicki, Michael N (Committee member) / Gonzalez-Velo, Yago (Committee member) / Goryll, Michael (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2017