| Summary: | Doctoral Degree. University of KwaZulu-Natal, Durban. Coal mining and petroleum refining processes face extreme pressure under climate change and global warming threats. Hence alternative sustainable and renewable energy sources must be made available for the rising energy demands. Natural gas found in permafrost and seabed areas in the form of gas hydrates possess vast amounts of low-carbon methane gas, which can replace fossil-based energy sources. The capture and storage of carbon dioxide gas in natural gas hydrate beds with the release of methane gas is a sustainable route under intense research. This study investigates the methane-carbon dioxide (CH4-CO2) replacement reaction mechanisms and the improvement of the process using different techniques, namely, additives, secondary gas, and thermal stimulation. Firstly, the gas hydrate dissociation measurements for the former gases utilized in the study were performed. This was followed by kinetic measurements with nanoparticles (aluminum oxide, copper oxide, and graphene nanoplatelets) and chemical additives (zinc oxide powder, graphite powder, and magnesium nitrate hexahydrate crystals) in the presence of sodium dodecyl sulfate (SDS) to affect kinetic or thermodynamic improvement in hydrate formation. The kinetic parameters investigated were induction time, hydrate storage capacity, water consumed in hydrate formation, fugacity of the gaseous phase, and the ratio of gas consumed to moles of water. Graphene nanoplatelets were selected for replacement reaction based on promising results obtained from the kinetic studies. The CH4-CO2 replacement process was performed in a 52 cm3 equilibrium cell using deionized water and nanoparticles. Also, a new experimental setup with a 300 cm3 reaction vessel was designed and assembled for CH4-CO2 replacement in the presence of synthetic silica sand. The results from kinetic studies showed an improvement in the hydrate formation kinetics due to the presence of nanoparticles. The CO2 hydrate formation kinetics obtained a ...
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