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首页> 外文期刊>Journal of Geophysical Research. Biogeosciences >Quantitative constraints on the atmospheric chemistry of nitrogen oxides: An analysis along chemical coordinates
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Quantitative constraints on the atmospheric chemistry of nitrogen oxides: An analysis along chemical coordinates

机译：氮氧化物对大气化学的定量约束：沿化学坐标的分析

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In situ observations of NO2, NO, NOy, ClONO2, OH, O-3, aerosol surface area, spectrally resolved solar radiation, pressure and temperature obtained from the ER-2 aircraft during the Photochemistry of Ozone Loss in the Arctic Region in Summer (POLARIS) experiments are used to examine the factors controlling the fast photochemistry connecting NO and NO2 and the slower chemistry connecting NOx and HNO3. Our analysis uses "chemical coordinates" to examine gradients of the difference between a model and precisely calibrated measurements to provide a quantitative assessment of the accuracy of current photochemical models. The NO/NO2 analysis suggests that reducing the activation energy for the NO+O-3 reaction by 1.7 kJ/mol will improve model representation of the temperature dependence of the NO/NO2 ratio in the range 215-235 K. The NOx/HNO3 analysis shows that systematic errors in the relative rate coefficients used to describe NOx loss by the reaction OH + NO2 --> HNO3 and by the reaction set NO2+O-3-->NO3; NO2+NO3 --> N2O5; N2O5+H2O --> 2HNO(3) are in error by +8.4% (+30/-45%) (OH + NO2 too fast) in models using the Jet Propulsion Laboratory 1997 recommendations [DeMore et al., 1997]. Models that use recommendations for OH+NO2 and OH+HNO3 based on reanalysis of recent and past laboratory measurements are in error by 1.2% (+30/-45%) (OH + NO2 too slow). The +30%/-45% error limit reflects systematic uncertainties, while the statistical uncertainty is 0.65%. This analysis also shows that the POLARIS observations only modestly constrain the relative rates of the major NOx production reactions HNO3 + OH --> H2O + NO3 and HNO3 + hv --> OH + NO2. Even under the assumption that all other aspects of the model are perfect, the POLARIS observations only constrain the rate coefficient for OH+HNO3 to a range of 65% around the currently recommended value. [References: 80]
机译：在夏季北极地区臭氧损失光化学过程中从ER-2飞机获得的NO2，NO，NOy，ClONO2，OH，O-3，气溶胶表面积，光谱分辨太阳辐射，压力和温度的原位观测（ POLARIS实验用于检查控制连接NO和NO2的快速光化学和连接NOx和HNO3的较慢化学的因素。我们的分析使用“化学坐标”来检查模型与精确校准的测量值之间的差异的梯度，以定量评估当前光化学模型的准确性。 NO / NO2分析表明，将NO + O-3反应的活化能降低1.7 kJ / mol将改善NO / NO2比的温度依赖性在215-235 K范围内的模型表示。NOx / HNO3分析表明，用于描述OH + NO2-> HNO3反应和反应组NO2 + O-3-> NO3的NOx损失的相对速率系数存在系统误差; NO2 + NO3-> N2O5;使用Jet Propulsion Laboratory 1997建议[DeMore et al。，1997]的模型中，N2O5 + H2O-> 2HNO（3）的误差为+ 8.4％（+ 30 / -45％）（OH + NO2太快）。根据对最近和过去实验室测量值的重新分析，使用推荐用于OH + NO2和OH + HNO3的模型的误差为1.2％（+ 30 / -45％）（OH + NO2太慢）。 +30％/-45％的误差极限反映了系统的不确定性，而统计不确定性为0.65％。该分析还表明，POLARIS观测值仅适度限制了主要NOx生成反应的相对速率HNO3 + OH-> H2O + NO3和HNO3 + hv-> OH + NO2。即使在模型的所有其他方面都完美的假设下，POLARIS观测值也仅将OH + HNO3的速率系数限制在当前推荐值的65％范围内。 [参考：80]

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