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Quantitative NH measurements by using laser-based diagnostics in low-pressure flames
Proceedings of the Combustion Institute ( IF 5.3 ) Pub Date : 2018-09-18 , DOI: 10.1016/j.proci.2018.09.007
Nathalie Lamoureux , Laurent Gasnot , Pascale Desgroux

NH is a key short-lived radical involved in the prompt-NO formation. Quantification of NH is thus particularly important for testing the NO kinetic mechanisms. However, quantitative measurements of native NH in hydrocarbon/oxygen/nitrogen flames remain very scarce. Therefore, in this work, the mole fractions of native NH were obtained using a combination of laser-based diagnostics; Laser Induced Fluorescence (LIF) and Cavity Ring-Down Spectroscopy (CRDS). The NH species was probed after exciting the transition R1(6) in the A3Π-X3Σ (0-0) system at 333.9 nm. The mole fraction profiles of NH were successfully obtained in premixed low-pressure flames of CH4/O2/N2 and C2H2/O2/N2 at two equivalence ratios of 1.00 and 1.25. The estimated detection limit for the NH radical was around 4.5 × 108 molecule cm−3 (i.e. 2 ppb in mole fraction at 1600 K), which is nearly 2 orders of magnitude lower than previous values reported in the literature. These new experimental results were compared with predictions by a recently developed NO model (namely NOMecha2.0). In the case of the CH4 flames, a satisfying agreement between the experiment and model was observed. However, in the case of the C2H2 flames, some discrepancies were observed. Model analysis has highlighted the importance of the HCCO radicals in the NH formation through the HCNO→HNCO→NH2 reactions pathway. Modification of the rate constant values of the reactions C2H2+ O and HCCO + O2, which are key reactions for both the acetylene laminar flame speed and the HCCO predictions, has enabled the model to satisfactorily predict the experimental NH and NO profiles also in the C2H2 flames.



中文翻译:

通过在低压火焰中使用基于激光的诊断程序进行定量NH测量

NH是参与NO迅速形成的关键短命自由基。因此,NH的定量对于测试NO动力学机理尤为重要。然而,烃/氧/氮火焰中天然NH的定量测量仍然非常稀少。因此,在这项工作中,天然NH的摩尔分数是结合使用基于激光的诊断方法获得的。激光诱导荧光(LIF)和腔衰荡光谱(CRDS)。的NH物种激发过渡后R探测1在A(6)3 Π-X 3 Σ -在333.9纳米(0-0)系统。在CH 4 / O 2 / N 2的预混合低压火焰中成功获得了NH的摩尔分数分布和C 2 H 2 / O 2 / N 2的两个当量比为1.00和1.25。NH自由基的估计检出限约为4.5×10 8分子cm -3(即,在1600 K下摩尔分数为2 ppb),比文献中报道的先前值低了近2个数量级。将这些新的实验结果与最近开发的NO模型(即NOMecha2.0)的预测结果进行了比较。在CH 4火焰的情况下,观察到实验与模型之间的令人满意的一致性。但是,在C 2 H 2的情况下火焰,观察到一些差异。模型分析突出了HCCO自由基通过HCNO→HNCO→NH 2反应途径在NH形成中的重要性。反应C 2 H 2的速率常数值的修改+ O和HCCO + O 2是乙炔层流火焰速度和HCCO预测的关键反应,已使模型能够令人满意地预测C 2 H 2火焰中的实验NH和NO分布。

更新日期:2018-09-18
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