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首页> 外文期刊>Atmospheric Chemistry and Physics Discussions >Modeling uncertainties for tropospheric nitrogen dioxide columns affecting satellite-based inverse modeling of nitrogen oxides emissions
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Modeling uncertainties for tropospheric nitrogen dioxide columns affecting satellite-based inverse modeling of nitrogen oxides emissions

机译:影响氮氧化物排放卫星逆建模的对流层氮二氧化柱的不确定性

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摘要

Errors in chemical transport models (CTMs) interpreting the relation between space-retrieved tropospheric column densities of nitrogen dioxide (NO2) and emissions of nitrogen oxides (NOx) have important consequences on the inverse modeling. They are however difficult to quantify due to lack of adequate in situ measurements, particularly over China and other developing countries. This study proposes an alternate approach for model evaluation over East China, by analyzing the sensitivity of modeled NO2 columns to errors in meteorological and chemical parameters/processes important to the nitrogen abundance. As a demonstration, it evaluates the nested version of GEOS-Chem driven by the GEOS-5 meteorology and the INTEX-B anthropogenic emissions and used with retrievals from the Ozone Monitoring Instrument (OMI) to constrain emissions of NOx. The CTM has been used extensively for such applications. Errors are examined for a comprehensive set of meteorological and chemical parameters using measurements and/or uncertainty analysis based on current knowledge. Results are exploited then for sensitivity simulations perturbing the respective parameters, as the basis of the following post-model linearized and localized first-order modification. It is found that the model meteorology likely contains errors of various magnitudes in cloud optical depth, air temperature, water vapor, boundary layer height and many other parameters. Model errors also exist in gaseous and heterogeneous reactions, aerosol optical properties and emissions of non-nitrogen species affecting the nitrogen chemistry. Modifications accounting for quantified errors in 10 selected parameters increase the NO2 columns in most areas with an average positive impact of 18% in July and 8% in January, the most important factor being modified uptake of the hydroperoxyl radical (HO2) on aerosols. This suggests a possible systematic model bias such that the top-down emissions will be overestimated by the same magnitude if the model is used for emission inversion without corrections. The modifications however cannot eliminate the large model underestimates in cities and other extremely polluted areas (particularly in the north) as compared to satellite retrievals, likely pointing to underestimates of the a priori emission inventory in these places with important implications for understanding of atmospheric chemistry and air quality. Note that these modifications are simplified and should be interpreted with caution for error apportionment.
机译:化学传输模型(CTMS)中的误差解释空间检索到二氧化氮(NO2)和氮氧化物排放(NOx)对阳性建模的重要后果。然而,由于缺乏足够的原位测量,特别是在中国和其他发展中国家,它们难以量化。本研究提出了一种替代方法,用于在华东地区的模型评估方法,通过分析模拟的NO2列对气象和化学参数/流程的误差的敏感性,对氮积累的流程进行了敏感性。作为演示,它评估了由Geos-5气象和Intex-B人类发射驱动的Geos-Chem的嵌套版本,并与臭氧监测仪器(OMI)的检索用于约束NOx的排放。 CTM已广泛用于此类应用。使用基于当前知识的测量和/或不确定性分析,检查误差是一套全面的气象和化学参数。结果被利用,然后用于扰动相应参数的灵敏度模拟,作为以下模型后线性化和局部大订单修改的基础。结果发现,模型气象可能在云光学深度,空气温度,水蒸气,边界层高度和许多其他参数中包含各种大小的误差。模型误差也存在于影响氮化学的非氮物质的气溶胶光学性质和非氮物质的排放中存在。修改10所选参数中量化误差的核算增加了大多数区域的NO2列,在7月平均阳性影响为18%和1月份的8%,最重要的因素正在改变氢过氧化氢基团(HO2)气溶胶上的最重要因素。这表明可能的系统模型偏置,使得如果模型用于没有校正的发射反转,则自上而下的排放将受到相同的幅度。然而,与卫星检索相比,该修改不能消除城市和其他极度污染的区域(特别是北方)的大型模型(特别是在北方),可能指向这些地方的先验排放量度低估了对大气化学的重要意义和空气质量。请注意,这些修改都是简化的,并且应该谨慎地解释错误,以便分配。

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