Absolute radical concentration measurements and modeling of low-pressure CH4/O2/NO flames

An experimental and theoretical investigation of CH and CN radical formation and destruction in a low-pressure 13.3-hPa (10 Torr) premixed stoichiometric CH₄/O₂ flame seeded with NO is presented. Relative concentration profiles of CH and CN are measured by linear unsaturated laser-induced fluorescence (LIF). An absolute calibration of the relative profiles is obtained by Rayleigh scattering. A computational study is performed to identify key uncertainties in the formation and destruction chemistry of the CH and CN radicals. It is shown that the reaction of the CH radical with molecular oxygen is of particular importance in the present flame. Prevailing uncertainties in the reactions of ³CH₂ with hydrogen atoms and molecular oxygen are also discussed. The present quantitative measurements of the CN radical also indicate that further attention should be given to the formation and oxidation chemistry of HCN. Nevertheless, computational results are encouraging and reasonable agreement is obtained for both the CH and CN radicals. It is further shown that the effects on CH concentration levels of introducing NO dopants may be reproduced. Comparisons of absolute concentration profiles of CH₃, OH, and CH radicals as well as NO are also made with computed results obtained using GRI Mech. 2.11 and a reaction mechanism developed by Warnatz. The computations highlight significant differences in reaction paths and rate selection. The major areas of uncertainty are outlined and tentative recommendations are made in relation to the key reaction paths.