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- All Subjects: Mechanical Engineering
- Member of: ASU Electronic Theses and Dissertations
- Status: Published
Description
The large-scale anthropogenic emission of carbon dioxide into the atmosphere leads to many unintended consequences, from rising sea levels to ocean acidification. While a clean energy infrastructure is growing, mid-term strategies that are compatible with the current infrastructure should be developed. Carbon capture and storage in fossil-fuel power plants is one way to avoid our current gigaton-scale emission of carbon dioxide into the atmosphere. However, for this to be possible, separation techniques are necessary to remove the nitrogen from air before combustion or from the flue gas after combustion. Metal-organic frameworks (MOFs) are a relatively new class of porous material that show great promise for adsorptive separation processes. Here, potential mechanisms of O2/N2 separation and CO2/N2 separation are explored.
First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
ContributorsMcIntyre, Sean (Author) / Mu, Bin (Thesis advisor) / Green, Matthew (Committee member) / Lind, Marylaura (Committee member) / Arizona State University (Publisher)
Created2019
Description
Deformable heat exchangers could provide a multitude of previously untapped advantages ranging from adaptable performance via macroscale, dynamic shape change (akin to dilation/constriction seen in blood vessels) to enhanced heat transfer at thermal interfaces through microscale, surface deformations. So far, making deformable, ‘soft heat exchangers’ (SHXs) has been limited by the low thermal conductivity of materials with suitable mechanical properties. The recent introduction of liquid-metal embedded elastomers by Bartlett et al1 has addressed this need. Specifically, by remaining soft and stretchable despite the addition of filler, these thermally conductive composites provide an ideal material for the new class of “soft thermal systems”, which is introduced in this work. Understanding such thermal systems will be a key element in enabling technology that require high levels of stretchability, such as thermoregulatory garments, soft electronics, wearable electronics, and high-powered robotics. Shape change inherent to SHX operation has the potential to violate many conventional assumptions used in HX design and thus requires the development of new theoretical approaches to predict performance. To create a basis for understanding these devices, this work highlights two sequential studies. First, the effects of transitioning to a surface deformable, SHX under steady state static conditions in the setting of a liquid cooling device for thermoregulation, electronics and robotics applications was explored. In this study, a thermomechanical model was built and validated to predict the thermal performance and a system wide analysis to optimize such devices was carried out. Second, from a more fundamental perspective, the effects of SHXs undergoing transient shape deformation during operation was explored. A phase shift phenomenon in cooling performance dependent on stretch rate, stretch extent and thermal diffusivity was discovered and explained. With the use of a time scale analysis, the extent of quasi-static assumption viability in modeling such systems was quantified and multiple shape modulation regime limits were defined. Finally, nuance considerations and future work of using liquid metal-silicone composites in SHXs were discussed.
ContributorsKotagama, Praveen (Author) / Rykaczewski, Konrad (Thesis advisor) / Wang, Robert (Committee member) / Phelan, Patrick (Committee member) / Herrmann, Marcus (Committee member) / Green, Matthew (Committee member) / Arizona State University (Publisher)
Created2020
Description
As experiencing hot months and thermal stresses is becoming more common, chemically protective fabrics must adapt and provide protections while reducing the heat stress to the body. These concerns affect first responders, warfighters, and workers regularly surrounded by hazardous chemical agents. While adapting traditional garments with cooling devices provides one route to mitigate this issue, these cooling methods add bulk, are time limited, and may not be applicable in locations without logistical support. Here I take inspiration from nature to guide the development of smart fabrics that have high breathability, but self-seal on exposure to target chemical(s), providing a better balance between cooling and protection.
Natural barrier materials were explored as a guide, focusing specifically on prickly pear cacti. These cacti have a natural waxy barrier that provides protection from dehydration and physically changes shape to modify surface wettability and water vapor transport. The results of this study provided a basis for a shape changing polymer to be used to respond directly to hazardous chemicals, swelling to contain the agent.
To create a stimuli responsive material, a novel superabsorbent polymer was synthesized, based on acrylamide chemistry. The polymer was tested for swelling properties in a wide range of organic liquids and found to highly swell in moderately polar organic liquids. To help predict swelling in untested liquids, the swelling of multiple test liquids were compared with their thermodynamic properties to observe trends. As the smart fabric needs to remain breathable to allow evaporative cooling, while retaining functionality when soaked with sweat, absorption of water, as well as that of an absorbing liquid in the presence of water were tested.
Micron sized particles of the developed polymer were deposited on a plastic mesh with pore size and open area similar to common clothing fabric to establish the proof of concept of using a breathable barrier to provide chemical protection. The polymer coated mesh showed minimal additional resistance to water vapor transport, relative to the mesh alone, but blocked more than 99% of a xylene aerosol from penetrating the barrier.
Natural barrier materials were explored as a guide, focusing specifically on prickly pear cacti. These cacti have a natural waxy barrier that provides protection from dehydration and physically changes shape to modify surface wettability and water vapor transport. The results of this study provided a basis for a shape changing polymer to be used to respond directly to hazardous chemicals, swelling to contain the agent.
To create a stimuli responsive material, a novel superabsorbent polymer was synthesized, based on acrylamide chemistry. The polymer was tested for swelling properties in a wide range of organic liquids and found to highly swell in moderately polar organic liquids. To help predict swelling in untested liquids, the swelling of multiple test liquids were compared with their thermodynamic properties to observe trends. As the smart fabric needs to remain breathable to allow evaporative cooling, while retaining functionality when soaked with sweat, absorption of water, as well as that of an absorbing liquid in the presence of water were tested.
Micron sized particles of the developed polymer were deposited on a plastic mesh with pore size and open area similar to common clothing fabric to establish the proof of concept of using a breathable barrier to provide chemical protection. The polymer coated mesh showed minimal additional resistance to water vapor transport, relative to the mesh alone, but blocked more than 99% of a xylene aerosol from penetrating the barrier.
ContributorsManning, Kenneth (Author) / Rykaczewski, Konrad (Thesis advisor) / Burgin, Timothy (Committee member) / Emady, Heather (Committee member) / Green, Matthew (Committee member) / Thomas, Marylaura (Committee member) / Arizona State University (Publisher)
Created2020