Post combustion capture of carbon dioxide through hydrate formation in silica gel column

Carbon dioxide CO₂capture through hydrate formation is a novel technology under consideration as an efficient means of separating CO₂from flue/fuel gas mixtures for sequestration and enhanced oil recovery operations. This thesis examines post-combustion capture of CO₂from fossil-fuel power plant flue-gas streams through hydrate formation in a silica gel column. Power plant flue-gas contains essentially CO₂and nitrogen (N2) after suitable pre-treatment steps, thus a model flue-gas comprising 17% co₂and 83% N2 was used in the study. Previous studies employed a stirred-tank reactor to achieve water-gas contact for formation of hydrates; recent microscopic studies involved using water dispersed in silica gel to react with gas, showing potential for improved hydrate formation rates without the need for agitation. This study focuses on macroscopic kinetics of hydrate formation in silica gel to evaluate hydrate formation rates, CO₂separation efficiency and determining optimal silica gel properties as a basis for a CO2 capture process. Spherical silica gels with 30.0 and 100.0 nm pore sizes and 40-75 and 75-200 μm particle sizes were studied to determine pore size and particle size effects on hydrate formation. 100.0 nm pores achieved higher gas uptake and CO₂recovery over the 30.0 nm case. Improved CO₂separation was obtained when 75-200 μm particles with 100.0 nm pores were used. The two effects observed are due to improved gas diffusion occurring with larger pore and particle size, favouring increased hydrate formation. Compared to stirred-tank experiments, results in this study show a near four-fold increase in moles of gas incorporated in the hydrate per mole of water, showing that improved water-to-hydrate conversion is obtained with pore-dispersed water. At similar experimental conditions, CO₂recovery improved from 42% for stirred-tank studies to 51% for the optimum silica (100.0 nm 75-200 μm) determined in this study. Finally, effects of tetrahydrofuran (THF) - an additive that reduces operating pressure were evaluated. Experiments with 1 mol% THF, the optimum determined from previous stirred tank studies, showed improved gas consumption in silica but reduced CO₂recovery, indicating that the optimum concentration for use in silica is different from that in stirred-tank experiments.Applied Science, Faculty ofChemical and Biological Engineering, Department ofGraduat