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Impact of intercontinental pollution transport on North American ozone air pollution: an HTAP phase 2 multi-model study

机译:洲际污染运输对北美臭氧空气污染的影响:HTAP阶段2多模型研究

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The recent update on the US National Ambient Air Quality Standards (NAAQS) of the ground-level ozone (O3) can benefit from a better understanding of its source contributions in different US regions during recent years. In the Hemispheric Transport of Air Pollution experiment phase?1 (HTAP1), various global models were used to determine the O3 source–receptor (SR) relationships among three continents in the Northern Hemisphere in 2001. In support of the HTAP phase?2 (HTAP2) experiment that studies more recent years and involves higher-resolution global models and regional models' participation, we conduct a number of regional-scale Sulfur Transport and dEposition Model (STEM) air quality base and sensitivity simulations over North America during May–June?2010. STEM's top and lateral chemical boundary conditions were downscaled from three global chemical transport models' (i.e., GEOS-Chem, RAQMS, and ECMWF C-IFS) base and sensitivity simulations in which the East Asian (EAS) anthropogenic emissions were reduced by 20?%. The mean differences between STEM surface O3 sensitivities to the emission changes and its corresponding boundary condition model's are smaller than those among its boundary condition models, in terms of the regional/period-mean (?10?%) and the spatial distributions. An additional STEM simulation was performed in which the boundary conditions were downscaled from a RAQMS (Realtime Air Quality Modeling System) simulation without EAS anthropogenic emissions. The scalability of O3 sensitivities to the size of the emission perturbation is spatially varying, and the full (i.e., based on a 100?% emission reduction) source contribution obtained from linearly scaling the North American mean O3 sensitivities to a 20?% reduction in the EAS anthropogenic emissions may be underestimated by at least 10?%. The three boundary condition models' mean O3 sensitivities to the 20?% EAS emission perturbations are ~?8?% (May–June?2010)/~?11?% (2010 annual) lower than those estimated by eight global models, and the multi-model ensemble estimates are higher than the HTAP1 reported 2001 conditions. GEOS-Chem sensitivities indicate that the EAS anthropogenic NOx emissions matter more than the other EAS O3 precursors to the North American O3, qualitatively consistent with previous adjoint sensitivity calculations. In addition to the analyses on large spatial–temporal scales relative to the HTAP1, we also show results on subcontinental and event scales that are more relevant to the US air quality management. The EAS pollution impacts are weaker during observed O3?exceedances than on all days in most US regions except over some high-terrain western US rural/remote areas. Satellite O3 (TES, JPL–IASI, and AIRS) and carbon monoxide (TES and AIRS) products, along with surface measurements and model calculations, show that during certain episodes stratospheric O3 intrusions and the transported EAS pollution influenced O3 in the western and the eastern US differently. Free-running (i.e., without chemical data assimilation) global models underpredicted the transported background O3 during these episodes, posing difficulties for STEM to accurately simulate the surface O3 and its source contribution. Although we effectively improved the modeled O3 by incorporating satellite O3 (OMI and MLS) and evaluated the quality of the HTAP2 emission inventory with the Royal Netherlands Meteorological Institute–Ozone Monitoring Instrument (KNMI–OMI) nitrogen dioxide, using observations to evaluate and improve O3 source attribution still remains to be further explored.
机译:最近关于地面臭氧(O3)的美国国家环境空气质量标准(NAAQ)的最新情况可以从近年来更好地了解不同美国地区的源贡献。在空气污染实验期的半球运输中?1(HTAP1),2001年北半球三大洲的各种全局模型用于确定O3源 - 受体(SR)关系。支持HTAP阶段?2( HTAP2)实验,研究更近年来并涉及更高分辨率的全球模型和区域模型的参与,我们在5月6月期间开展了许多区域规模的硫运输和沉积模型(Stem)空气质量基础和敏感性模拟?2010年。茎的顶部和横向化学边界条件是从三个全球化学输送模型(即Geos-Chem,Raqms和EcmWF C-Ifs)底座和敏感性模拟的级联,其中东亚(EAS)人为的排放量减少了20? %。茎表面O3敏感性对发射变化的平均差异及其对应的边界条件模型小于其边界条件模型的差异,就区域/周期 - 平均值(?10?%)和空间分布而言。进行额外的茎模拟,其中边界条件从RAQMS(实时空气质量建模系统)模拟中逐渐缩小,没有EAS人为排放。 O3敏感性对发射扰动的尺寸的可扩展性在空间上变化,并且完全(即,基于100?%的排放减少)从线性缩放北美平均O3敏感性的源贡献到20?% EAS人为排放可能低估至少10μl%。三个边界条件模型的平均敏感性为20?%EAS排放扰动是〜?8?%(五月六月?2010)/〜?11?%(2010年度年度)低于八个全球模型的估计,多模型集合估计高于HTAP1报告的2001条条件。 Geos-Chem敏感性表明,EAS人为NOx排放量多于其他EAS O3前体对北美O3,与先前的伴随敏感性计算定性一致。除了相对于HTAP1的大型空间尺度上的分析外,我们还显示出与美国空气质量管理更相关的子加管和事件秤的结果。在观察到的O3期间,EAS污染影响较弱?除了在大多数美国地区的所有日子外,除了一些高地形西部美国农村/偏远地区。卫星O3(TES,JPL-IASI和AIRS)和一氧化碳(TES和AIRS)产品以及表面测量和模型计算,表明在某些发作流程图中的侵入性和在西方的S3不同于东方的不同。自由运行(即,没有化学数据同化)全球模型在这些剧集期间造成了运输的背景O3,使茎难以精确地模拟表面O3及其源贡献。虽然我们通过掺入卫星O3(OMI和MLS)来有效改善了模型的O3,并使用荷兰皇家气象学研究所 - 臭氧监测仪(KNMI-OMI)氮素二氧化氮,评价和改善O3,评估HTAP2排放清单的质量。源归因仍有待进一步探索。
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