Impacts of Humidity and Degradation on Adsorbents for CO2 Capture

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HOLMES-DISSERTATION-2024.pdf (62.47 MB)
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Holmes, Hannah Elisabeth
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School of Chemical and Biomolecular Engineering
School established in 1901 as the School of Chemical Engineering; in 2003, renamed School of Chemical and Biomolecular Engineering
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https://hdl.handle.net/1853/77711
Abstract
Carbon capture technologies are critical for mitigating the global temperature increase and its associated consequences. Advancements in solid adsorbents can reduce the cost of carbon capture technologies, particularly in three key areas: degradation, interactions with humidity, and integration into structured contactors. First, economic models were developed to assess the impact of sorbent degradation on the cost of direct air capture (DAC) and bioenergy with carbon capture and storage (BECCS). The results emphasize that increasing the lifetime of adsorbents should be prioritized. As a preliminary investigation into which adsorbents will be stable in BECCS, adsorbents were directly exposed to biomass combustion flue gas. Pre- and post-exposure characterization highlighted the range of possible degradation mechanisms due to structural differences in adsorbents. The second focus was on developing carbon capture materials that can adsorb appreciable amounts of carbon dioxide from humid feed streams. The addition of guanidine groups to the backbone of polymer of intrinsic microporosity (PIM)-1 was shown to mitigate amine impregnation issues and further enhance carbon dioxide chemisorption in the presence of humidity. Then, an optimum feed humidity range was identified for a diamine-appended metal-organic framework (MOF), in which a humidity-promoted sorption mechanism leads to a significant enhancement in capacity. Finally, fabrication methods were developed to translate the powder materials into scalable contactors. Fiber sorbents and monoliths containing the diamine-appended MOF exhibited the unique stepped adsorption behavior of the MOF. All-polymer hollow fibers containing PIM-guanidine were also fabricated, addressing the energy and productivity consequences of inactive support materials in contactors. By lowering the cost of carbon capture technologies, the insights facilitate the rapid and widescale deployment that is necessary for limiting the global temperature increase. The results also provide a foundation for further advancements in understanding, controlling, and utilizing the impacts of humidity and degradation on carbon dioxide adsorption processes, which is crucial for their success.
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2024-04-27
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Dissertation
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