Zádor Judit, Zsély István Gy, Turányi Tamás, Ratto Marco, Tarantola Stefano, Saltelli Andrea
Department of Physical Chemistry, Eötvös University (ELTE), P.O. Box 32, H-1518 Budapest, Hungary.
J Phys Chem A. 2005 Nov 3;109(43):9795-807. doi: 10.1021/jp053270i.
Local and global uncertainty analyses of a flat, premixed, stationary, laminar methane flame model were carried out using the Leeds methane oxidation mechanism at lean (phi = 0.70), stoichiometric (phi = 1.00), and rich (phi = 1.20) equivalence ratios. Uncertainties of laminar flame velocity, maximal flame temperature, and maximal concentrations of radicals H, O, OH, CH, and CH(2) were investigated. Global uncertainty analysis methods included the Morris method, the Monte Carlo analysis with Latin hypercube sampling, and an improved version of the Sobol' method. Assumed probability density functions (pdf's) were assigned to the rate coefficients of all the 175 reactions and to the enthalpies of formation of the 37 species. The analyses provided the following answers: approximate pdf's and standard deviations of the model results, minimum and maximum values of the results at any physically realistic parameter combination, and the contribution of the uncertainty of each parameter to the uncertainty of the model result. The uncertainty of a few rate parameters and a few enthalpies of formation causes most of the uncertainty of the model results. Most uncertainty comes from the inappropriate knowledge of kinetic data, but the uncertainty caused by thermodynamic data is also significant.
使用利兹甲烷氧化机理，在贫燃（φ = 0.70）、化学计量比（φ = 1.00）和富燃（φ = 1.20）当量比条件下，对扁平、预混、静止、层流甲烷火焰模型进行了局部和全局不确定性分析。研究了层流火焰速度、最高火焰温度以及自由基H、O、OH、CH和CH₂的最大浓度的不确定性。全局不确定性分析方法包括莫里斯方法、采用拉丁超立方抽样的蒙特卡罗分析以及索博尔方法的改进版本。为所有175个反应的速率系数以及37种物质的生成焓指定了假设的概率密度函数（pdf）。分析给出了以下结果：模型结果的近似pdf和标准差、在任何实际物理参数组合下结果的最小值和最大值，以及每个参数的不确定性对模型结果不确定性的贡献。少数速率参数和少数生成焓的不确定性导致了模型结果的大部分不确定性。大部分不确定性来自动力学数据的了解不足，但热力学数据引起的不确定性也很显著。
