Chemical Kinetics Study of the Autoignition of NH3/CH4 Mixtures
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摘要: 在当量比φ=0.5、压力为2~7 MPa以及温度从930 K到1 140 K的条件下,用快速压缩机研究氨气(NH3)和甲烷(CH4)混合气的着火延迟时间,其中CH4占总燃料的摩尔分数分别为0、5%、10%及50%.另外,在φ为1.0和2.0的条件下对掺入10%CH4的混合气进行着火延迟时间测试.CH4对NH3的着火过程具有非常明显的促进作用,随着CH4占总燃料的比例越来越高,混合气的着火延迟时间缩短,同时CH4对着火的促进作用趋于平缓.含10%CH4的NH3的着火延迟时间在φ为0.5和1.0的条件下变化很小,而当φ=2.0时着火延迟时间增加约50%.利用试验数据对6种不同的NH3氧化机理进行了验证,所开发的机理预测着火延迟时间最为准确,除了在最高温度,CH4摩尔分数为50%时试验与计算差异达到了50%,其他所有条件下机理的预测结果与试验结果差距都小于30%.利用开发的机理进行敏感性分析,结果表明:当CH4摩尔分数为5%和10%时,反应CH4+NH2=CH3+NH3对稀薄燃烧条件下混合气的着火延迟时间有显著的促进作用;但当CH4摩尔分数为50%时,该反应会表现出轻微的抑制作用.Abstract: Ignition delay times of NH3/CH4 mixtures with CH4 mole fractions of 0,5%,10% and 50% were measured in a rapid compression machine at equivalence ratio of 0.5,pressures from 2—7 MPa and temperatures from 930 K to 1 140 K. In addition,measurements were performed for NH3 mixtures with 10% CH4 at φ=1.0 and 2.0.Methane shows a strong ignition-enhancing effect on NH3,which levels off at higher CH4 fractions,as the ignition delay time approaches that of pure methane. Autoignition delay times at 10% CH4 at φ=0.5 and 1.0 are indistinguishable,while an increase of ignition delay times by factor of 1.5 was observed upon increasing φ to 2.0. The experimental data were used to evaluate six NH3 oxidation mechanisms capable of simulating NH3/CH4 mixtures. The mechanism previously used shows the best performance:generally,it predicts the measured ignition delay times to better than 30% for all conditions,except for 50% CH4 addition for which the differences increase up to 50% at the highest temperature. Sensitivity analysis based on the mechanism used indicates that under lean conditions the reaction CH4+NH2=CH3+NH3 significantly promotes ignition for CH4 addition(5% and 10%),but becomes modestly ignition-inhibiting at 50% CH4.
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