Reduced Mechanism for Nitrogen and Sulfur Chemistry in Pressurized Flue Gas Systems

The gas- and liquid-phase chemistry of nitrogen and sulfur species under pressurized conditions is of high importance to the design and performance of the pressurized flue gas systems in carbon capture and storage (CCS) schemes. Yet, the available description of this chemistry is complex and difficult to apply in design studies for removal of NOx and SOx during the compression. This work proposes a reduced mechanism for engineering calculations of pressurized flue gas systems, a mechanism that is able to describe the relevant gas and liquid-phase chemistry as well as the S/N-product distribution. The reduced mechanism is derived by identifying the rate-limiting reactions using sensitivity analysis. The performance of the mechanism subsets are compared with results of a detailed mechanism. The identified rate-limiting reactions for the formation of key products form the basis for two different types of reduced mechanisms. The sets include one general reduced mechanism (valid for all pH conditions) and sets of pH-specific mechanisms. The general reduced mechanism and the pH-specific mechanisms perform satisfactorily compared to the detailed mechanism under different pH conditions. The results show that depending on the purpose of the modeling, whether it is to predict the pollutant removal (where sulfurous acid and nitrogen acids are mainly important) or capture the liquid composition, for which the N-S chemistry products are also important, different levels of simplification can be made. The number of reactions is reduced from 34 reactions (39 species) in the detailed mechanism to 12 reactions (20 species) in the general reduced mechanism and 7-8 (14-17 species) in the pH-specific mechanisms.