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- Genre: Academic theses
- Creators: Green, Matthew
- Creators: McIntyre, Sean
- 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
The cost of capturing carbon dioxide (CO2) from ambient air needs to be greatly reduced if it is to contribute significantly to mitigating climate change. Ion-exchange resin (IER) with quaternary ammonium cation binds CO2 when dry and releases it when wet without supplemental energy, making the process attractive for economical Direct Air Capture (DAC). In this study, a design case basis was developed for a system of collectors capable of capturing 1000 tons/day of CO2 via moisture swing sorption. The model uses varying weather parameters such as temperature, wind speed, and relative humidity to understand the impact of weather on the sorbent loading, cycle time (capture and regeneration), and net water loss. Two independent isotherm models, namely Flory Huggins and the modified Langmuir isotherm model were used to estimate the water and CO2 loading of the resin respectively as a function of relative humidity. The capture model suggests a higher capture rate during the summer and daytime (in a diurnal cycle) as the relative humidity is lower. A design optimization model was developed to minimize the capture time and maximize the sorbent loading. The crude rate production and the net water loss can help conduct an economic analysis to determine the cost of carbon capture.
ContributorsTalha, Mohammad Abu (Author) / Green, Matthew (Thesis advisor) / Lackner, Klaus (Committee member) / Cirucci, John (Committee member) / Arizona State University (Publisher)
Created2023