A dissertation submitted to the Faculty of Engineering and the Built Environment, University of the Witwatersrand, Johannesburg, in fulfilment of the requirements for the degree of Master of Science in Engineering
September, 2017 / South Africa emits large amounts of carbon dioxide (CO2) due to its reliance on coal. The emission of CO2 needs to be reduced for clean sustainable energy generation. Research efforts have therefore been devoted to reducing CO2 emissions by developing cost-effective methods for capturing and storing it. Amine-based absorption using monoethanolamine solvent is the most mature technique for CO2 capture despite its huge energy consumption, corrosiveness and difficulty in solvent regeneration. However, CO2 removal by solid adsorbents is a promising alternative because it consumes less energy, and can be operated at moderate temperature and pressure. Metal organic frameworks have received attention as a CO2 adsorbent because they have large surface areas, open metal sites, high porosity and they require less energy for regeneration.
This research was aimed at optimizing and scaling-up SOD-ZMOF through structural modification for enhanced CO2 adsorption by impregnating it with chitosan. Scaled-up SOD-ZMOF samples were prepared as described elsewhere and impregnated with Chitosan. Physiochemical properties obtained using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and Nitrogen physisorption showed that SOD-ZMOF and SOD-ZMOF-chitosan were successfully synthesized. Qualitatively, the surface area of the SOD-ZMOF synthesized using the scaled up protocol is lower than the one prepared using the non-scaled-up protocol
XRD pattern of SOD-ZMOF showed that it was crystalline and was in agreement with literature. The XRD peaks of the SOD-ZMOF decreased after chitosan impregnation showing that chitosan was impregnated on SOD-ZMOF. The FTIR spectrum of SOD-ZMOF showed functional groups present in organic linker used to synthesize SOD-ZMOF, and that of the SOD-ZMOF-chitosan revealed the same functional groups but with disappearance of carboxylic acid functional group. N2 physisorption showed a decrease in BET surface area and pore volume after chitosan impregnation on SOD-ZMOF as well.
Performance evaluation of the material was carried out with a demonstration adsorption set-up using a 15%/85% CO2/N2 mixture and as a thermal gravimetric analysis (TGA) using 100% CO2. For both the packed-bed column and the TGA experiments, evaluation was conducted on SOD-ZMOF and SOD-ZMOF with chitosan for comparison. About 50 mg of the adsorbent was used at 25 oC, 1 bar and 25 ml/min for the packed-bed column. For the adsorption with the TGA, 11 mg of adsorbent was used at 25 ℃, 1 bar and 60 ml/min.
SOD-ZMOF showed improved adsorption capacity after chitosan impregnation. CO2 adsorption capacity of SOD-ZMOF increased by 16% and 39% using packed-bed column and TGA, respectively, after chitosan impregnation. The increase in adsorption capacity was attributed to the impregnated chitosan that has amine groups that display a high affinity for CO2.
A traditional approach was used to investigate the effect of adsorption temperature and inlet gas flowrate on the CO2 adsorption capacity of SOD-ZMOF-chitosan. This was done using both the parked bed column and the TGA. Temperature range of 25-80 ℃ and inlet gas flowrate range of 25-90 ml/min were investigated. Adsorption capacity increased with a decrease in temperature and inlet gas flowrate. For the packed-bed column, maximum of 781 mg CO2/ g adsorbent was obtained at 25℃, 1 bar, 25 ml/min and for the TGA a maximum CO2 adsorption capacity of 23 mg/ g adsorbent at 25 ℃, 1 bar, and 60 ml/min was obtained. / MT2018
| Identifer | oai:union.ndltd.org:netd.ac.za/oai:union.ndltd.org:wits/oai:wiredspace.wits.ac.za:10539/24232 |
| Date | January 2017 |
| Creators | Singo, Muofhe Comfort |
| Source Sets | South African National ETD Portal |
| Language | English |
| Detected Language | English |
| Type | Thesis |
| Format | Online resource (xvi, 113 leaves), application/pdf, application/pdf |
Page generated in 0.0032 seconds