Analysis of radical propagation efficiency to assess ozone sensitivity to hydrocarbons and NO x : 1. Local indicators of instantaneous odd oxygen production sensitivity
Analysis of radical propagation efficiency to assess ozone sensitivity to hydrocarbons and NO x : 1. Local indicators of instantaneous odd oxygen production sensitivity
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DOI：
10.1029/1999jd900371
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发表时间：
2000-04
影响因子：
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通讯作者：
G. Tonnesen;R. Dennis
中科院分区：
文献类型：
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作者：
G. Tonnesen;R. Dennis
我们使用了一个简单的轨迹模型和一个三维网格模型来评估几个指标，可以用来预测奇数氧生产（P（Ox））的人为非甲烷碳氢化合物（VOC）和氮氧化物（NOx = NO + NO2）的排放变化的敏感性。为了进行评估，我们增强了模型，包括新的诊断输出，如P（Ox）的速率，NOx转化为非反应性氮的速率和自由基链长。我们使用新的诊断输出来解释模型预测的P（Ox）对VOC和NOx排放变化的敏感性。我们发现，臭氧脊线，区分NOx限制和自由基限制的条件下，是由最大OH链长度的脊线。我们研究了影响OH链长的自由基增长反应，并提出了四个与自由基增长效率相关的指标：I（HC，NO_2），它近似于与烃反应的OH的分数; I（NO，RO_2），它近似于与NO反应的HO_2的分数;[HO 2]是P（H2 O2）/P（HNO 3）的主导项。这些指标中的每一个都区分了瞬时P（Ox）主要对NOx排放减少或VOC排放减少敏感的条件。
We used a simple trajectory model and a three-dimensional grid model to evaluate several indicators that can be used to predict the sensitivity of odd oxygen production (P(Ox)) to changes in emissions of anthropogenic nonmethane hydrocarbons (VOC) and nitrogen oxides (NOx = NO + NO2). To perform the evaluation, we augmented the model to include new diagnostic outputs such as rates of P(Ox), rates of conversion of NOx to unreactive nitrogen, and radical chain length. We used the new diagnostic outputs to explain the model-predicted sensitivity of P(Ox) to changes in VOC and NOx emissions. We found that the ozone ridgeline, which distinguishes between NOx-limited and radical-limited conditions, is determined by a ridgeline of maximum OH chain length. We examined the radical propagation reactions which affect OH chain length, and we developed four indicators related to radical propagation efficiency: I(HC,NO2) which approximates the fraction of OH that reacts with hydrocarbons; I(NO,RO2) which approximates the fraction of HO2 that reacts with NO; the ratio of [O3]/[NOx] which affects the balance between radical initiation and propagation; and [HO2] which is the dominant term in P(H2O2)/P(HNO3). Each of these indicators distinguishes conditions in which instantaneous P(Ox) is primarily sensitive to either NOx emissions reductions or VOC emissions reductions.