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Coal-fired power plants are the largest anthropogenic point sources of CO2 emissions worldwide. About 40% of the world's electricity comes from coal. Approximately 49% of the US electricity in 2008 and 23% of the total electricity generation of Canada in 2000 came from coal-fired power plant (World Coal Association, and Statistic Canada). It is likely that in the near future there might be some form of CO2 regulation. Therefore, it is highly probable that CO2 capture will need to be implemented at many US and Canadian coal fired power plants at some point. Several technologies are available for CO2 capture from coal-fired power plants. One option is to separate CO2 from the combustion products using conventional approach such as chemical absorption/stripping with amine solvents, which is commercially available. Another potential alternative, membrane gas separation, involves no moving parts, is compact and modular with a small footprint, is gaining more and more attention. Both technologies can be retrofitted to existing power plants, but they demands significant energy requirement to capture, purify and compress the CO2 for transporting to the sequestration sites. This thesis is a techno-economical evaluation of the two approaches mentioned above along with another approach known as hybrid. This evaluation is based on the recent advancement in membrane materials and properties, and the adoption of systemic design procedures and optimization approach with the help of a commercial process simulator. Comparison of the process performance is developed in AspenPlus process simulation environment with a detailed multicomponent gas separation membrane model, and several rigorous rate-based absorption/stripping models. Fifteen various single and multi-stage membrane process configurations with or without recycle streams are examined through simulation and design study for industrial scale post-combustion CO2 capture. It is found that only two process configurations are capable to satisfy the process specifications i.e., 85% CO2 recovery and 98% CO2 purity for EOR. The power and membrane area requirement can be saved by up to 13% and 8% respectively by the optimizing the base design. A post-optimality sensitivity analysis reveals that any changes in any of the factors such as feed flow rate, feed concentration (CO2), permeate vacuum and compression condition have great impact on plant performance especially on power consumption and product recovery. Two different absorption/stripping process configurations (conventional and Fluor concept) with monoethanolamine (30 wt% MEA) solvent were simulated and designed using same design basis as above with tray columns. Both the rate-based and the equilibrium-stage based modeling approaches were adopted. Two kinetic models for modeling reactive absorption/stripping reactions of CO2 with aqueous MEA solution were evaluated. Depending on the options to account for mass transfer, the chemical reactions in the liquid film/phase, film resistance and film non-ideality, eight different absorber/stripper models were categorized and investigated. From a parametric design study, the optimum CO2 lean solvent loading was determined with respect to minimum reboiler energy requirement by varying the lean solvent flow rate in a closed-loop simulation environment for each model. It was realized that the success of modeling CO2 capture with MEA depends upon how the film discretization is carried out. It revealed that most of the CO2 was reacted in the film not in the bulk liquid. This insight could not be recognized with the traditional equilibrium-stage modeling. It was found that the
optimum/or minimum lean solvent loading ranges from 0.29 to 0.40 and the reboiler energy ranges from 3.3 to 5.1 (GJ/ton captured CO2) depending on the model considered. Between the two process alternatives, the Fluor concept process performs well in terms of plant operating (i.e., 8.5% less energy) and capital cost (i.e., 50% less number of strippers). The potentiality of hybrid processes which combines membrane permeation and conventional gas absorption/stripping using MEA were also examined for postcombustion CO2 capture in AspenPlus. It was found that the hybrid process may not be a promising alternative for post-combustion CO2 capture in terms of energy requirement for capture and compression. On the other hand, a stand-alone membrane gas separation process showed the lowest energy demand for CO2 capture and compression, and could save up to 15 to 35% energy compare to the MEA capture process depending on the absorption/stripping model used