Carbon Dioxide Capture Conversion via Calgary Framework CALF-20: Catalytic Process design and Optimization
Date
2021-11-02
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Abstract
The main goal of this study is to explore the integration of Calgary Framework CALF20, [Zn2(1,2,4-triazolate)2(oxalate)], that was developed in Dr. Shimzu’s lab in three catalytic conversion processes. Each process was implemented in this project as a separate objective. Chapter 3 included developing an integrated device at Dr. Kibria’s lab, wherein MOF-based porous materials served as CO? concentrators, and subsequently, a Cu-based nanostructured catalyst electrochemically converts CO? to ethylene C2H4. Carbon fiber sheet Gas-Diffusion Layer (GDL) was used as a platform to conduct the current and support the MOF and Cu catalyst for CO? capture and electrochemical reduction reaction, respectively. One side of the GDL was coated with Zinc-based MOF. The MOF layer served as a CO? concentrator and a screening stage, where it allows a higher percentage of CO? molecules to pass through the fiber to the other side. The other side of the GDL was coated with Cu?O particles to catalyze the electrochemical reduction reaction. The spray coating technique was used to spray coat MOF and Cu?O onto the carbon fiber. Binary gas feed N? 90%/CO? 10% at a relative humidity (RH%) of 10%, 30%, and 70% was used for the electrochemical reduction experiments in a flow-cell configuration. The results showed high C2H4 selectivity, conversion efficiency, and catalyst stability at RH 10% and 30%. Chapter 4 included the use of metal-organic frameworks (MOFs) and combining the desirable features of homogeneous and heterogeneous catalysts for boosting the activity of CO?RR. Zn-based MOFs involving two different azolate functional ligands, i.e., 1,2,4-triazolate (Calgary Framework-20, CALF20) and 2-methylimidazole (zeolitic imidazolate framework-8, ZIF-8), were investigated for CO?RR in an alkaline flow cell electrolyzer. In Chapter 5, we synthesized a composite of photoactive TiO?/MOF material for CO? capture and photoconversion. The TiO?/MOF composites were implemented in a photocatalytic reactor set-up to corroborate the CO? capture and photocatalytic conversion process. CO product was identified. The composite proved its ability to increase the CO yield up to 4.51 ?mol g-1h-1 with 70% CALF20 in the composite compared to 2.98 and 1.88 ?mol g-1h-1 for TiO? and CALF20 separately.
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Keywords
Carbon Capture, Carbon Conversion, CO2, MOF, Catalysis, CO2 reduction, CALF20
Citation
Marei, N. N. I. (2021). Carbon Dioxide Capture Conversion via Calgary Framework CALF-20: Catalytic Process design and Optimization (Doctoral thesis). University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca .