Critical kinetic uncertainties in modeling hydrogen/carbon monoxide, methane, methanol, formaldehyde, and ethylene combustion
Critical kinetic uncertainties in modeling hydrogen/carbon monoxide, methane, methanol, formaldehyde, and ethylene combustion
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DOI：
10.1016/j.combustflame.2018.02.006
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发表时间：
2018-09
影响因子：
4.4
通讯作者：
Yujie Tao;Gregory P Smith;Hai Wang
中科院分区：
文献类型：
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作者：
Yujie Tao;Gregory P Smith;Hai Wang
鉴于反应模型的潜在不确定性在燃烧化学建模未来进展中的关键作用，根据 H2、H2/CO、CH4、CH2O 和 C2H6 的现有基本燃烧数据，开发了基础燃料化学模型 1.0 (FFCM-1)，并进行了不确定性最小化。作为一个关键功能，FFCM-1不仅协调了大量的基本燃烧数据，还严格评估了速率系数的不确定性、用于模型优化和不确定性最小化的燃烧实验目标，最重要的是，具有量化不确定性的优化反应模型。在目前的工作中，使用完美搅拌反应器（PSR）作为相关模型平台来检查 FFCM-1 的剩余动力学不确定性，但在测试条件下无法进行可靠的实验。要解决的关键问题包括模型优化对熄灭和点火时 PSR 停留时间的预测不确定性的改进程度，以及必须改进的反应速率系数，以减少预测不确定性。对 H2/CO 单键、CH2O 单键、CH4 单键、CH3OH 单键和 C2H4-空气混合物进行计算测试，压力范围为 10-100 atm，PSR 入口温度将产生与实际燃烧器中燃料燃烧的典型时间尺度相当的停留时间。结果表明，虽然模型优化降低了熄灭和着火停留时间预测的不确定性，但剩余的不确定性仍然较大。已确定并详细讨论了降低速率不确定性将极大提高反应模型质量和准确性的关键反应。
In view of the critical role of the underlying uncertainties of the reaction model in future progress of combustion chemistry modeling, Foundational Fuel Chemistry Model 1.0 (FFCM-1) was developed with uncertainty minimization against available fundamental combustion data of H2, H2/CO, CH4, CH2O, and C2H6. As a critical feature, FFCM-1 not only reconciles a large body of fundamental combustion data, it also has rigorously evaluated uncertainties for the rate coefficients, the combustion experimental targets used for model optimization and uncertainty minimization, and most importantly, an optimized reaction model with quantified uncertainties. In the present work, the remaining kinetic uncertainties of FFCM-1 are examined using a perfectly stirred reactor (PSR) as the relevant model platform for which reliable experiments under the conditions tested are unavailable. The key questions to address include the level of improvement from model optimization in the prediction uncertainties of PSR residence times at extinction and ignition and the rate coefficients of reactions that must be improved in order to reduce the prediction uncertainties. Computational tests are made for H2/COsingle bond, CH2Osingle bond, CH4single bond, CH3OHsingle bond and C2H4–air mixtures over the pressure range of 10–100 atm and PSR inlet temperatures that would yield residence times comparable to the time scales typical of fuel combustion in practical combustors. The results show that although model optimization reduces the prediction uncertainties of residence time at extinction and ignition, the remaining uncertainties remain rather large. Key reactions for which reduced rate uncertainties would greatly improve the reaction model quality and accuracy have been identified and discussed in detail.