Matching Items (4)
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- All Subjects: Adsorption
- All Subjects: Climate Change
- All Subjects: CCS
- All Subjects: MOF
- Creators: Anderson, James
- Member of: ASU Electronic Theses and Dissertations
- Status: Published
Description
The implications of a changing climate have a profound impact on human life, society, and policy making. The need for accurate climate prediction becomes increasingly important as we better understand these implications. Currently, the most widely used climate prediction relies on the synthesis of climate model simulations organized by the Coupled Model Intercomparison Project (CMIP); these simulations are ensemble-averaged to construct projections for the 21st century climate. However, a significant degree of bias and variability in the model simulations for the 20th century climate is well-known at both global and regional scales. Based on that insight, this study provides an alternative approach for constructing climate projections that incorporates knowledge of model bias. This approach is demonstrated to be a viable alternative which can be easily implemented by water resource managers for potentially more accurate projections. Tests of the new approach are provided on a global scale with an emphasis on semiarid regional studies for their particular vulnerability to water resource changes, using both the former CMIP Phase 3 (CMIP3) and current Phase 5 (CMIP5) model archives. This investigation is accompanied by a detailed analysis of the dynamical processes and water budget to understand the behaviors and sources of model biases. Sensitivity studies of selected CMIP5 models are also performed with an atmospheric component model by testing the relationship between climate change forcings and model simulated response. The information derived from each study is used to determine the progressive quality of coupled climate models in simulating the global water cycle by rigorously investigating sources of model bias related to the moisture budget. As such, the conclusions of this project are highly relevant to model development and potentially may be used to further improve climate projections.
ContributorsBaker, Noel C (Author) / Huang, Huei-Ping (Thesis advisor) / Trimble, Steve (Committee member) / Anderson, James (Committee member) / Clarke, Amanda (Committee member) / Calhoun, Ronald (Committee member) / Arizona State University (Publisher)
Created2013
Description
The numerical climate models have provided scientists, policy makers and the general public, crucial information for climate projections since mid-20th century. An international effort to compare and validate the simulations of all major climate models is organized by the Coupled Model Intercomparison Project (CMIP), which has gone through several phases since 1995 with CMIP5 being the state of the art. In parallel, an organized effort to consolidate all observational data in the past century culminates in the creation of several "reanalysis" datasets that are considered the closest representation of the true observation. This study compared the climate variability and trend in the climate model simulations and observations on the timescales ranging from interannual to centennial. The analysis focused on the dynamic climate quantity of zonal-mean zonal wind and global atmospheric angular momentum (AAM), and incorporated multiple datasets from reanalysis and the most recent CMIP3 and CMIP5 archives. For the observation, the validation of AAM by the length-of-day (LOD) and the intercomparison of AAM revealed a good agreement among reanalyses on the interannual and the decadal-to-interdecadal timescales, respectively. But the most significant discrepancies among them are in the long-term mean and long-term trend. For the simulations, the CMIP5 models produced a significantly smaller bias and a narrower ensemble spread of the climatology and trend in the 20th century for AAM compared to CMIP3, while CMIP3 and CMIP5 simulations consistently produced a positive trend for the 20th and 21st century. Both CMIP3 and CMIP5 models produced a wide range of the magnitudes of decadal and interdecadal variability of wind component of AAM (MR) compared to observation. The ensemble means of CMIP3 and CMIP5 are not statistically distinguishable for either the 20th- or 21st-century runs. The in-house atmospheric general circulation model (AGCM) simulations forced by the sea surface temperature (SST) taken from the CMIP5 simulations as lower boundary conditions were carried out. The zonal wind and MR in the CMIP5 simulations are well simulated in the AGCM simulations. This confirmed SST as an important mediator in regulating the global atmospheric changes due to GHG effect.
ContributorsPaek, Houk (Author) / Huang, Huei-Ping (Thesis advisor) / Adrian, Ronald (Committee member) / Wang, Zhihua (Committee member) / Anderson, James (Committee member) / Herrmann, Marcus (Committee member) / Arizona State University (Publisher)
Created2013
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