To mitigate the global greenhouse gases (GHGs) emissions, carbon dioxide (CO2) capture and storage (CCS) has the potential to play a significant role for reaching mitigation target. Oxy-fuel combustion is a promising technology for CO2 capture in power plants. Advantages compared to CCS with the conventional combustion technology are: high combustion efficiency, flue gas volume reduction, low fuel consumption, near zero CO2 emission, and less nitrogen oxides (NOx) formation can be reached simultaneously by using the oxy-fuel combustion technology. However, knowledge gaps relating to large scale coal based and natural gas based power plants with CO2 capture still exist, such as combustors and boilers operating at higher temperatures and design of CO2 turbines and compressors. To apply the oxy-fuel combustion technology on power plants, much work is focused on the fundamental and feasibility study regarding combustion characterization, process and system analysis, and economic evaluation etc. Further studies from system perspective point of view are highlighted, such as the impact of operating conditions on system performance and on advanced cycle integrated with oxy-fuel combustion for CO2 capture. In this thesis, the characterization for flue gas recycle (FGR) was theoretically derived based on mass balance of combustion reactions, and system modeling was conducted by using a process simulator, Aspen Plus. Important parameters such as FGR rate and ratio, flue gas composition, and electrical efficiency etc. were analyzed and discussed based on different operational conditions. An advanced evaporative gas turbine (EvGT) cycle with oxy-fuel combustion for CO2 capture was also studied. Based on economic indicators such as specific investment cost (SIC), cost of electricity (COE), and cost of CO2avoidance (COA), economic performance was evaluated and compared among various system configurations. The system configurations include an EvGT cycle power plant without CO2 capture, an EvGT cycle power plant with chemical absorption for CO2 capture, and a combined cycle power plant. The study shows that FGR ratio is of importance, which has impact not only on heat transfer but also on mass transfer in the oxy-coal combustion process. Significant reduction in the amount of flue gas can be achieved due to the flue gas recycling, particularly for the system with more prior upstream recycle options. Although the recycle options have almost no effect on FGR ratio, flue gas flow rate, and system electrical efficiency, FGR options have significant effects on flue gas compositions, especially the concentrations of CO2 and H2O, and heat exchanger duties. In addition, oxygen purity and water/gas ratio, respectively, have an optimum value for an EvGT cycle power plant with oxy-fuel combustion. Oxygen purity of 97 mol% and water/gas ratio of 0.133 can be considered as the optimum values for the studied system. For optional operating conditions of flue gas recycling, the exhaust gas recycled after condensing (dry recycle) results in about 5 percentage points higher electrical efficiency and about 45 % more cooling water consumption comparing with the exhaust gas recycled before condensing (wet recycle). The direct costs of EvGT cycle with oxy-fuel combustion are a little higher than the direct costs of EvGT cycle with chemical absorption. However, as plant size is larger than 60 MW, even though the EvGT cycle with oxy-fuel combustion has a higher COE than the EvGT cycle with chemical absorption, the EvGT cycle with oxy-fuel combustion has a lower COA. Further, compared with others studies of natural gas combined cycle (NGCC), the EvGT system has a lower COE and COA than the NGCC system no matter which CO2 capture technology is integrated. / QC 20111123

Nearly half of the electrical power produced in the United States is generated with coal. Coal power is inexpensive and reliable, but coal combustion releases harmful pollutants including NOx and SOx into the atmosphere if not controlled. CO2, a greenhouse gas, is also released during coal combustion and may contribute to global warming. A promising technology enabling carbon capture is oxy-coal combustion. During oxy-combustion, coal is burned in an atmosphere of O2 and recycled flue gas to eliminate nitrogen which makes up the majority of air-combustion flue gas. Oxy-combustion flue gas is mainly composed of CO2 and H2O. H2O can be condensed out of the gas, and the CO2 can then be captured and permanently stored relatively easily. The composition of the gas inside an oxy-fired boiler will be different due to the absence of nitrogen and the recycling of flue gas. Corrosive sulfur and chlorine gas species concentrations will be higher, and CO and NOx concentrations will be effected. An understanding of the differences in gas concentrations is critical to oxy-combustion boiler design. Four different pulverized coals were combusted in a reactor under staged and unstaged oxy-combustion conditions with warm recycled flue gas (420°F) to simulate conditions in an oxy-fired coal boiler. The gas composition was measured in the reducing and oxidizing zones for staged combustion, and in the same locations, 57 cm and 216 cm from the burner, for unstaged combustion. The results were compared to the results from similar staged air-combustion experiments using the same coals and burner. CO concentrations were higher for staged oxy-combustion compared to air-combustion, and the increase was more substantial for lower rank coals. H2S concentrations in the reducing regions were also higher, and the fraction of gas phase sulfur measured as H2S was higher for oxy-combustion. SO2 concentrations were 2.9 to 3.8 times as high as air-combustion concentrations. The measured conversion of coal sulfur to SO3 was lower for oxy-combustion, and ranged from 0.61% to 0.98%. The average fraction of coal sulfur measured in the gas phase was 84%, 80%, and 85% for staged oxy-combustion, unstaged oxy-combustion, and staged air-combustion respectively. HCl concentrations were 2.8 to 3.1 times higher in the staged oxy-combustion oxidizing zone, and a smaller fraction of coal chlorine was measured in the reducing zone. On average 70.8%, 79.5%, and 71.1% of the coal chlorine was measured as HCl for staged oxy-combustion, unstaged oxy-combustion, and staged air-combustion respectively. The fractions of coal chlorine and sulfur measured in the gas phase for staged combustion were not significantly affected by combustion media. Some staged oxy-combustion NO concentrations were lower than air-combustion concentrations while others were slightly higher, and NO emission rates were much lower due to recycling NO through the burner.