Matching Items (3)
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- All Subjects: Adsorption
- All Subjects: CCS
- All Subjects: Las Vegas climate
- All Subjects: MOF
- Creators: Anderson, James
- Member of: ASU Electronic Theses and Dissertations
- Status: Published
Description
Post-combustion carbon capture is a viable option for reducing CO2 greenhouse gas emissions, and one potentially promising technology for this route is adsorption using chemically and physically based sorbents. A number of exceptional CO2 sorbents materials have been prepared including metal organic frameworks, zeolites, and carbon based materials. One particular group of capable materials are amine based solid sorbents that has shown to possess high adsorption capacities and favorable adsorption kinetics. A key variable in the synthesis of an amine based sorbent is the support which acts as the platform for the amine modification. Aerogels, due to their high porosities and surface areas, appear to be a promising support for an amine modified CO2 sorbent. Therefore, in order to develop a commercially viable CO2 sorbent, particulate aerogels manufactured by Cabot Corporation through an economical and proprietary ambient drying process were modified with amines using a variety of functionalization methods. Two methods of physical impregnation of the amino polymer TEPA were performed in order to observe the performance as well as understand the effects of how the TEPA distribution is affected by the method of introduction. Both samples showed excellent adsorption capacities but poor cyclic stability for lack of any covalent attachment. Furthermore the method of TEPA impregnation seems to be independent on how the polymer will be distributed in the pore space of aerogel. The last two methods utilized involved covalently attaching amino silanes to the surface silanols of the aerogel. One method was performed in the liquid phase under anhydrous and hydrous conditions. The materials developed through the hydrous method have much greater adsorption capacities relative to the anhydrous sample as a result of the greater amine content present in the hydrous sample. Water is another source of silylation where additional silanes can attach and polymerize. These samples also possessed stable cyclic stability after 100 adsorption/regeneration cycles. The other method of grafting was performed in the gas phase through ALD. These samples possessed exceptionally high amine efficiencies and levels of N content without damaging the microstructure of the aerogel in contrast to the liquid phase grafted sorbents.
ContributorsLinneen, Nick (Author) / Lin, Jerry (Thesis advisor) / Pfeffer, Robert (Thesis advisor) / Lind, Mary (Committee member) / Rege, Kaushal (Committee member) / Nielsen, David (Committee member) / Anderson, James (Committee member) / Arizona State University (Publisher)
Created2014
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
This study uses the Weather Research and Forecasting (WRF) model to simulate and predict the changes in local climate attributed to the urbanization for five desert cities. The simulations are performed in the fashion of climate downscaling, constrained by the surface boundary conditions generated from high resolution land-use maps. For each city, the land-use maps of 1985 and 2010 from Landsat satellite observation, and a projected land-use map for 2030, are used to represent the past, present, and future. An additional set of simulations for Las Vegas, the largest of the five cities, uses the NLCD 1992 and 2006 land-use maps and an idealized historical land-use map with no urban coverage for 1900.
The study finds that urbanization in Las Vegas produces a classic urban heat island (UHI) at night but a minor cooling during the day. A further analysis of the surface energy balance shows that the decrease in surface Albedo and increase effective emissivity play an important role in shaping the local climate change over urban areas. The emerging urban structures slow down the diurnal wind circulation over the city due to an increased effective surface roughness. This leads to a secondary modification of temperature due to the interaction between the mechanical and thermodynamic effects of urbanization.
The simulations for the five desert cities for 1985 and 2010 further confirm a common pattern of the climatic effect of urbanization with significant nighttime warming and moderate daytime cooling. This effect is confined to the urban area and is not sensitive to the size of the city or the detail of land cover in the surrounding areas. The pattern of nighttime warming and daytime cooling remains robust in the simulations for the future climate of the five cities using the projected 2030 land-use maps. Inter-city differences among the five urban areas are discussed.
The study finds that urbanization in Las Vegas produces a classic urban heat island (UHI) at night but a minor cooling during the day. A further analysis of the surface energy balance shows that the decrease in surface Albedo and increase effective emissivity play an important role in shaping the local climate change over urban areas. The emerging urban structures slow down the diurnal wind circulation over the city due to an increased effective surface roughness. This leads to a secondary modification of temperature due to the interaction between the mechanical and thermodynamic effects of urbanization.
The simulations for the five desert cities for 1985 and 2010 further confirm a common pattern of the climatic effect of urbanization with significant nighttime warming and moderate daytime cooling. This effect is confined to the urban area and is not sensitive to the size of the city or the detail of land cover in the surrounding areas. The pattern of nighttime warming and daytime cooling remains robust in the simulations for the future climate of the five cities using the projected 2030 land-use maps. Inter-city differences among the five urban areas are discussed.
ContributorsKamal, Samy (Author) / Huang, Huei-Ping (Thesis advisor) / Anderson, James (Thesis advisor) / Herrmann, Marcus (Committee member) / Calhoun, Ronald (Committee member) / Myint, Soe (Committee member) / Arizona State University (Publisher)
Created2015