The characteristics and mechanism NO formation during hydroxylated fuels/NH3 oxidation in oxy-fuel atmospheres

Abstract

Oxy-fuel combustion, as an important technology to realize CCUS in the field of combustion, needs to control the generation of pollutants such as NOx while realizing CO2 capture, and the conversion of fuel-N to N2 is crucial. Previous experiments have provided insights into the influence of different atmospheres on NO during oxy-fuel combustion of alcohols. However, the specific reaction mechanism underlying how the atmosphere and hydroxyl fuels impact NO generation through the free radical pool remains unclear. In this study, the formation and reduction of NO during the oxidation of CH3OH/NH3 and C2H5OH/NH3 in O2/CO2, O2/H2O and O2/CO2/H2O atmospheres with oxy-fuel condition were investigated by simulation. In the NO generation stage, different H2O, CO2, O2 and fuel types have little effect on the peak of NO although they change the NH3→NO reaction path. In the process of NO reduction, stage 1 is the main reaction phase of NO→N2, and both CO2 and H2O are beneficial for the reduction of NO. But the reduction of NO by H2O was more pronounced. In the case of simultaneous addition of H2O and CO2, the reducing effect of H2O and CO2 alone on NO was attenuated. On the other hand, the reduction effect exerted by H2O and CO2 was stronger in high than in low oxygen-fuel ratio, stronger in C2H5OH than in CH3OH. The reduction of NO by H2O and CO2 is based on the general equation NO→N2+O2. H2O is used to promote the reaction in the positive direction by consuming O2 to convert it to H and OH, so that more of the element O is converted to OH than O2 to inhibit the production of NO. The CO2 contributes to the formation of less O2 during the reduction of N2 from NO by promoting reaction NO + N→O + N2, while the additional OH increases the "capacity" of O2 in the NO→N2+O2 reaction.