Simulated tropospheric NOx : Its evaluation, global distribution and individual source contributions
Simulated tropospheric NOx : Its evaluation, global distribution and individual source contributions
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模拟对流层氮氧化物：其评估、全球分布和单个源贡献
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发表时间：
1999
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通讯作者：
P. Kasibhatla
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作者：
H. Levy;W. Moxim;A. Klonecki;P. Kasibhatla
使用11级地球物理流体动力学实验室的全球化学传输模型，我们模拟全球对流层领域的氮氧化物，过氧乙酰硝酸盐（PAN），硝酸氢，和NO y，以及沉积的硝酸盐，广泛评估他们对现有的观测从地面站和飞机任务，并量化个人的自然和人为来源的贡献。模拟和观测到的HNO 3湿沉降的模式和量级在地球仪周围大体上是一致的。NOx和NO y的模型模拟与飞机观测的散点图发现，± 25%的点在± 25%范围内，± 75%在± 50%范围内，并且没有显示出系统的全局偏差。模拟和观测的垂直廓线形状相似，污染边界层（BL）中的水平较高（≥ 1ppbv），在遥远的BL中的值很低，从对流层中层到上层的值逐渐增加。模拟的NO y HNO 3和NOx + PAN也与莫纳罗亚天文台的广泛的低层自由对流层观测结果吻合得很好。在一般情况下，模拟和观测之间的协议的水平是一样好的协议之间的单独的，但同时，观测的NO，NOx或NO y如以前的研究表明，化石燃料燃烧和生物质燃烧控制NOx水平在对流层的下半部分的大部分与显着的贡献，从生物源排放。例外的是偏远的低氮氧化物的区域，BL和FT源作出可比的贡献。与大多数以前的研究，我们发现，小得多的原位FT源一般占主导地位的对流层上半部分。热带和夏季中纬度地区闪电占主导地位，平流层注入是夏季高纬度地区闪电的主要来源。唯一的例外是化石燃料燃烧产生的运输排放，这在冬季高纬度地区占主导地位。虽然飞机排放很少占主导地位，但对北方热带外的对流层上部和平流层下部确实有重大影响。
Using the 11-level Geophysical Fluid Dynamics Laboratory global chemical transport model, we simulate global tropospheric fields of NO x , peroxyacetyl nitrate (PAN), HNO 3 , and NO y , as well as the deposition of nitrate, extensively evaluate them against available observations from surface stations and aircraft missions, and quantify the contributions of individual natural and anthropogenic sources. The patterns and magnitudes of simulated and observed HNO 3 wet deposition are generally in good agreement around the globe. Scatterplots of model simulations versus aircraft observations for NO x and NO y find ∼50% of the points within ±25%, find -75% within ±50%, and show no systematic global biases. Both simulated and observed vertical profiles have similar shapes with high levels (∼1 ppbv or greater) in the polluted boundary layer (BL), very low values in the remote BL, and values increasing from the middle to the upper troposphere. Simulated NO y HNO 3 , and NO x + PAN are also in good agreement with extensive lower free tropospheric ( ) observations made at Mauna Loa Observatory. In general, the level of agreement between simulation and observation is as good as the agreement between separate, but simultaneous, observations of NO, NO x or NO y As previous studies have shown, fossil fuel combustion and biomass burning control NO x levels in most of the lower half of the troposphere with a significant contribution from biogenic emissions. The exceptions are the remote low-NO x regions where BL and FT sources make comparable contributions. Unlike most previous studies, we find that the much smaller in situ FT sources generally dominate in the upper half of the troposphere. Lightning dominates in the tropics and summertime midlatitudes, and stratospheric injection is the major source in the summer high latitudes. The exception is transported emissions from fossil fuel combustion, which dominate in winter high latitudes. Though seldom dominant, aircraft emissions do have a significant impact on the upper troposphere and lower stratosphere of the northern hemisphere extratropics.