Application of metal organic frameworks (MOFs) to capturing CO2 directly from air

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Darunte, Lalit A.
Jones, Christopher W.
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Increased CO2 concentration in the atmosphere is increasingly linked to climate change. With the aim of developing next-generation carbon capture technologies; this thesis focuses on the use of solid amine-functionalized metal-organic frameworks (MOFs) for CO2 capture from air. MOFs are promising because of their tunability and high porosity. However, many considerations are required for their practical utilization. 1. High equilibrium adsorption capacity at ultra-dilute CO2 concentrations, 2. Incorporation of MOFs into practical substrates that can provide low pressure drops at high flowrates of air, and 3. Process analysis that takes into account various thermodynamic and kinetic factors. This thesis studied MIL-101(Cr) and Mg2(dobpdc) frameworks functionalized with various amines for CO2 adsorption at direct air capture conditions. Additionally, diamine-appended Mg2(dobpdc) was immobilized on a practical honeycomb monolith substrate with an oriented MOF growth. This diamine-appended framework was further studied for CO2 adsorption in a packed bed experiment where different regimes of breakthrough profiles were identified using an equilibrium wave theory and the kinetics of CO2 adsorption was characterized using semi-empirical models. Overall, this thesis aims to further the understanding of the scientific community in various aspects that are critical for the use of novel adsorbents in a practical process.
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