Chemical speciation and soot measurements in laminar counterflow diffusion flames of ethylene and ammonia mixtures

Ammonia is considered as one of the most promising alternative fuels due to its carbon neutrality and the existing infrastructure for its mass production and delivery. However, burning neat ammonia has the issue of poor flame stability and high NOx emissions, making co-firing ammonia with conventional fuel a more feasible approach. The present work investigated the sooting characteristics of counterflow diffusion flames of ethylene/ammonia mixtures. Experimentally, soot volume fraction (SVF) and average soot particle diameter in the neat ethylene, ammonia- and nitrogen- doped flames were non-intrusively measured. Both SVF and average soot particles diameter were found to decrease with the addition of ammonia. Flame temperature were measured with tunable diode laser absorption spectroscopy and the results suggested that the inhibiting effect of ammonia on soot formation was chemical instead of thermal. For further kinetic insights, numerical simulation with newly-constructed reaction mechanisms were performed and the results were compared against chemical speciation data from gas chromatography (GC) measurements; the results showed that ammonia doping would lead to more significant reduction of benzene concentration than nitrogen doping. Kinetic pathways of the chemical suppressing effect of ammonia addition on soot and its precursor formation were then explained based on numerical results. The major contribution of the present work can be summarized in the following aspects: 1) New comprehensive experimental data on sooting characteristics, important intermediate species concentrations of diffusion counterflow flames of ethylene/ammonia mixtures were provided for model validation; 2) One coupled mechanism with detailed hydrocarbon-nitrogen interactions was established to predict PAHs formation and soot formation; 3) Detailed chemical kinetics insight of ammonia effect on soot formation was presented in the counterflow flame.