Quantitative assessment of uncertainties for a model of tropospheric ethene oxidation using the European Photoreactor (EUPHORE)
Quantitative assessment of uncertainties for a model of tropospheric ethene oxidation using the European Photoreactor (EUPHORE)
复制标题
使用欧洲光反应器 (EUPHORE) 对对流层乙烯氧化模型的不确定性进行定量评估
DOI：
10.1016/j.atmosenv.2004.06.052
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发表时间：
2005
影响因子：
5
通讯作者：
M. Pilling
中科院分区：
文献类型：
--
作者：
J. Zádor;V. Wagner;K. Wirtz;M. Pilling
使用不确定度分析方法将主化学机制第3版(MCMv3)与在西班牙巴伦西亚的欧洲光反应堆(EUPHORE)中进行的测量进行了比较，以调查模型测量的差异并获得关于墙效应重要性的信息。用以下方法分析了在高NOx和低NOx条件下乙烯氧化的两个EUPHORE烟雾室测量结果：(I)局部不确定度分析，(Ii)Morris全局筛选方法和(Iii)拉丁超立方体采样的蒙特卡罗(MC)分析。对于这两个实验，臭氧(分别增加了25%和30%)和甲醛(分别增加了34%和40%)被模型计算大大高估了，而对其他物种的不一致就不那么明显了。根据局部不确定度分析和Morris方法，在低NOx条件下，臭氧不确定度的最主要贡献因素是HOCH2CH2O2+NO→HOCH2CH2O+NO2，而在高NOx条件下，主要贡献因素是OH+NO2→HNO3。MC模拟给出了在实验结束时两种情况下臭氧的2σ不确定度估计为∼20%。结果表明，测量和模型计算之间存在系统性的不一致，尽管这种差异的来源尚不清楚。似乎腔效应本身并不是观察到的差异的原因。
Methods of uncertainty analysis were used for comparison of the Master Chemical Mechanism version 3 (MCMv3) with measurements made in the European Photoreactor (EUPHORE) at Valencia (Spain) to investigate model–measurement discrepancies and to obtain information on the importance of wall effects. Two EUPHORE smog chamber measurements of ethene oxidation, under high and low NOxconditions were analysed by the following methods: (i) local uncertainty analysis, (ii) the global screening method of Morris and (iii) Monte Carlo (MC) analysis with Latin hypercube sampling. For both experiments, ozone (by 25% and 30%, respectively) and formaldehyde (by 34% and 40%, respectively) are significantly over-predicted by the model calculations, while the disagreement for other species is less substantial. According to the local uncertainty analysis and the Morris method, the most important contributor to ozone uncertainty under low NOxconditions is HOCH2CH2O2+NO→HOCH2CH2O+NO2, while under high NOxconditions OH+NO2→HNO3is the main contributor. The MC simulations give an estimate of the 2σ uncertainty for ozone as ∼20% in both scenarios at the end of the experiment. The results suggest systematic disagreement between measurements and model calculations, although the origin of this is not clear. It seems that chamber effects alone are not responsible for the observed discrepancies.