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Ozone source apportionment during peak summer events over southwestern Europe

机译：欧洲西南部夏季高峰事件中的臭氧源分配

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It is well established that in Europe, high Osub3/sub concentrations are most pronounced in southern/Mediterranean countries due to the more favourable climatological conditions for its formation. However, the contribution of the different sources of precursors to Osub3/sub formation within each country relative to the imported (regional and hemispheric) Osub3/sub is poorly quantified. This lack of quantitative knowledge prevents local authorities from effectively designing plans that reduce the exceedances of the Osub3/sub target value set by the European air quality directive. Osub3/sub source attribution is a challenge because the concentration at each location and time results not only from local biogenic and anthropogenic precursors, but also from the transport of Osub3/sub and precursors from neighbouring regions, Osub3/sub regional and hemispheric transport and stratospheric Osub3/sub injections. The main goal of this study is to provide a first quantitative estimation of the contribution of the main anthropogenic activity sectors to peak Osub3/sub events in Spain relative to the contribution of imported (regional and hemispheric) Osub3/sub . We also assess the potential of our source apportionment method to improve Osub3/sub modelling. Our study applies and thoroughly evaluates a countrywide Osub3/sub source apportionment method implemented in the CALIOPE air quality forecast system for Spain at high resolution (4 × 4?km sup2/sup ) over a 10-day period characterized by typical summer conditions in the Iberian Peninsula (IP). The method tags both Osub3/sub and its gas precursor emissions from source sectors within one simulation, and each tagged species is subject to the typical physico-chemical processes (advection, vertical mixing, deposition, emission and chemistry) as the actual conditions remain unperturbed. We quantify the individual contributions of the largest NOsubx/sub local sources to high Osub3/sub concentrations compared with the contribution of imported Osub3/sub . We show, for the first time, that imported Osub3/sub is the largest input to the ground-level Osub3/sub concentration in the IP, accounting for 46?%–68?% of the daily mean Osub3/sub concentration during exceedances of the European target value. The hourly imported Osub3/sub increases during typical northwestern advections (70?%–90?%, 60–80 μ g?m sup?3/sup ), and decreases during typical stagnant conditions (30?%–40?%, 30–60 μ g?m sup?3/sup ) due to the local NO titration. During stagnant conditions, the local anthropogenic precursors control the Osub3/sub peaks in areas downwind of the main urban and industrial regions (up to 40?% in hourly peaks). We also show that ground-level Osub3/sub concentrations are strongly affected by vertical mixing of Osub3/sub -rich layers present in the free troposphere, which result from local/regional layering and accumulation, and continental/hemispheric transport. Indeed, vertical mixing largely explains the presence of imported Osub3/sub at ground level in the IP. Our results demonstrate the need for detailed quantification of the local and remote contributions to high Osub3/sub concentrations for local Osub3/sub management, and show Osub3/sub source apportionment to be an essential analysis prior to the design of Osub3/sub mitigation plans in any non-attainment area. Achieving the European Osub3/sub objectives in southern Europe requires not only ad hoc local actions but also decided national and European-wide strategies.
机译：众所周知，在欧洲，南部/地中海国家的O 3 浓度最高，这是由于其形成的气候条件更为有利。但是，相对于进口的（区域和半球形）O 3 ，每个国家内不同前体来源对O 3 形成的贡献都难以量化。由于缺乏定量知识，地方当局无法有效设计计划，以减少超出欧洲空气质量指令设定的O 3 目标值的情况。 O 3 的来源归因是一个挑战，因为每个位置和时间的浓度不仅来自本地生物和人为前体，而且还来自O 3 和来自邻区，O 3 区域和半球运输以及平流层O 3 注入。这项研究的主要目的是相对于进口（区域和半球）O 3 事件高峰的贡献进行首次定量估算。 > 3 。我们还评估了源分配方法改善O 3 建模的潜力。我们的研究应用并彻底评估了西班牙CALIOPE空气质量预报系统中在高分辨率（4×4？km 2 ）上实施的全国O 3 源分配方法。以伊比利亚半岛（IP）典型的夏季条件为特征的10天时段。该方法在一次模拟中同时标记了O 3 及其源部门的气体前体排放，并且每个标记的物种都经受典型的物理化学过程（对流，垂直混合，沉积，排放和化学作用）因为实际情况保持稳定。与进口的O 3 的贡献相比，我们量化了最大的NO x 本地来源对高O 3 浓度的单个贡献。我们首次显示，进口的O 3 是IP中地面O 3 浓度的最大输入，占46％-68％。超出欧洲目标值期间的每日平均O 3 浓度的百分比。每小时输入的O 3 在典型的西北平流期间增加（70？％– 90？％，60–80μg？m ？3 ），在典型的停滞条件下减少（30 %% – 40％，30–60μg？m ？3 ）归因于局部NO滴定。在停滞状态下，当地人为活动的前兆控制着主要城市和工业区顺风地区的O 3 高峰（每小时高峰可达40％）。我们还表明，自由对流层中存在的富含O 3 的层的垂直混合强烈地影响了地面O 3 的浓度，这是由于局部/区域分层和积累和大陆/半球运输。的确，垂直混合在很大程度上解释了IP地面上是否存在导入的O 3 。我们的结果表明，需要对本地O 3 管理中O 3 浓度高的本地和远程贡献进行详细量化，并显示O 3 在任何非达标区域设计O 3 缓解计划之前，源头分配是必不可少的分析。要在南欧实现欧洲的O 3 目标，不仅需要临时采取局部行动，还需要制定国家和整个欧洲范围的战略。

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