Experimental and kinetic modeling study of NO formation in premixed CH4+O2+N2 flames

Abstract

The nitric oxide (NO) formation in methane (CH 4 ) flames has been widely investigated, with quite a few kinetic mechanisms available in the literature. However, studies have shown that there are often discrepancies between the simulations using various mechanisms and the experimental results. To elucidate reactions leading to these discrepancies, experiments were designed to measure the NO formation in the post flame zone of CH 4 +O 2 +N 2 flames with the oxygen ratio, x O 2 = O 2 /(O 2 +N 2 ), varying from 0.2 to 0.27. The experiments were carried out on a heat flux burner at atmospheric pressure and 298 K using saturated Laser-induced fluorescence. The equivalence ratio, ϕ , was changed from 0.7 to 1.6. The corresponding laminar burning velocity, S L , for each condition was also measured using the heat flux method. A comparison was made for the present experimental data and simulation results using the Konnov, Glarborg, NOMecha 2.0, and San Diego mechanisms, and none of them well reproduced the new NO experimental data for all investigated conditions. Numerical analyses show that the increment of NO mole fraction in stoichiometric and fuel-lean flames when the x O 2 increases is mostly defined by the thermal-NO production, which is found to be over-predicted, especially by the Konnov and San Diego mechanisms. The rate constant of reaction NO+N = N 2 +O was derived as k = 1.529 × 10 13 T − 0.0027 exp ( 185.41 [ c a l / m o l e ] R T ) cm 3 / mol s over 225–2400 K temperature range. The rate constants of four reactions controlling CH mole fraction profiles and prompt-NO formation were updated based on the analysis of the literature data that yields an improved performance of the Konnov mechanism.