Energy & Fuels, Vol.33, No.4, 3339-3348, 2019
Evaluation of Operating and Design Parameters of Pressurized Flue Gas Systems with Integrated Removal of NOx and SOx
This study investigates the operating and design parameters of product gas compression and integrated control of nitrogen oxides (NOx) and sulfur oxides (SOx) in large-scale oxy-fuel and chemical looping combustion processes. A process model that includes a comprehensive description of nitrogen and sulfur chemistry and mass transfer is developed. The results show that the fraction of NO oxidation into NO2 will be 10-50% in a multistage compressor to 30 bars (1-4% O-2 in the gas) depending on the residence times in intercoolers and pressure levels. At lower O-2 concentrations (>0.1% O(2 )in the gas), the oxidation is limited but still active. Nitric acid formation in the compressor condensate is, thus, inevitable, although limited, as most water is condensed in the early stages, whereas the acid gases are formed in the later stages. The NO2/NOx ratio has an important effect on the total amount of NOx absorbed and extra residence time should be added after the compressor to increase this ratio. Evaluation of the process behavior in relation to simultaneous absorption of SO2 and NOx revealed that increased SO2/NOx ratio and bottom liquid recycling enhanced the total NOx absorption. In addition, maintaining the pH in the absorbing solution above 5 improves the removal efficiencies of NOx and SO2. NOx removal rates of up to around 95% can be achieved for SO2/NOx > 1 in the flue gas with appropriate design of the absorber. For SO2/NOx < 1, increasing the packing height or addition of S(IV) solutions could enhance the NOx removal rates to 95% or more. The model predictions are compared with the experimental data from a laboratory-scale absorber. The process model developed in this work enables design studies and techno-economic evaluation of absorption-based NOx and SOx removal concepts.