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Source apportionment of submicron organic aerosol at an urban background and a road site in Barcelona (Spain) during SAPUSS

机译:在城市背景和苏贝纳(西班牙)的城市背景和一条路站点的亚微米有机气溶胶的来源分配

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This study investigates the contribution of potential sources to the submicron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September–October 2010). A total of 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by gas chromatography–mass spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by multivariate curve resolution–alternating least squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin and three of secondary OA origin, while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (urban primary organic aerosol, or POA Urban), mainly traffic emissions but also cigarette smoke, contributed 43% (1.5 μg OC m3) and 18% (0.4 μg OC m3) to OA at RS and UB, respectively. A secondary primary source – biomass burning (BBOA) – was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation (REG.). Three secondary organic aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO) – i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols – showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m?3, or 16% and 7%, at UB and RS, respectively). By contrast, a SOA biogenic component attributed to -pinene oxidation (SOA BIO PIN) presented average concentrations of 0.5 μg m?3 at UB (24% of OA) and 0.2 μg m3 at RS (7%), respectively, suggesting that this SOA component did not impact the two monitoring sites at the same level. A clear anti-correlation was observed between SOA ISO and SOA PIN during nucleation days, surprisingly suggesting that some of the growth of urban freshly nucleating particles may be driven by biogenic α-pinene oxidation products but inhibited by isoprene organic compounds. A third SOA component was formed by a mixture of aged anthropogenic and biogenic secondary organic compounds (SOA Aged) that accumulated under stagnant atmospheric conditions, contributing for 12% to OA at RS (0.4 μg OC m3) and for 18% at UB (0.4 μg OC m3). A sixth component, formed by C7–C9 dicarboxylic acids and detected especially during daytime, was called "urban oxygenated organic aerosol" (OOA Urban) due to its high abundance at urban RS (23%; 0.8 μg OCm3) vs. UB (10%; 0.2 μg OCm3), with a well-defined daytime maximum. This temporal trend and geographical differentiation suggests that local anthropogenic sources were determining this component. However, the changes of these organic molecules were also influenced by the air mass trajectories, indicating that atmospheric conditions have an influence on this component, although the specific origin on this component remains unclear. It points to a secondary organic component driven by primary urban sources including cooking and traffic (mainly gasoline) activities.
机译:本研究调查潜在来源在城市背景(UB)和巴塞罗那的30天内在城市背景(UB)和公路站点(RS)的亚微米(PM1)有机气溶胶(OA)的贡献(解决2010年9月至10月,使用协同策略来解决气溶胶问题。在两个站点都收集了12小时采样时间分辨率的103个过滤器。通过气相色谱 - 质谱(GC-MS)分析已知发射源和光学化学转化方法的三十六个中性和极性有机化合物。本文提出并讨论了分析的痕量化合物的浓度。另外,通过多变量曲线分辨率 - 交替的最小二乘(MCR-Al)和在两个位点鉴定出六种组分的OA源分数:两种是原发性人为OA起源和三个二次OA起源,而第六个是不是明确规定。来自局部人为活动排放(城市原发性有机气溶胶或POA城市)排放的初级有机体,主要是交通排放,也是卷烟烟雾,为RS和RS贡献了43%(1.5μg)和18%(0.4μgm3)至OA分别为UB。在所有样品中发现了次级主要源 - 生物量燃烧(BboA)(平均值7%Rs; 12%UB;0.3μgoc m3),但当当采样点受影响的情况下,该组分基本上才会有助于OA区域空气群众循环(REG。)。在城市环境PM1中观察到三次二次有机气溶胶(SOA)组分(描述总体60%的方差)。异戊二烯氧化产物(SOA ISO) - 即2-甲基甘氨酸,C5烯烃三醇和2-甲基四烯醇 - 当城市受到内陆空气群众的影响时,两种地方的最高丰富。 SOA ISO的总浓度在两个位点(0.4和0.3μgm≤3,或16%和7%,分别为UB和Rs)。相比之下,归因于 - 氧化氧化(SOA BIO引脚)的SOA生物成分呈现在UB(24%OA)下的平均浓度为0.5μgm≤3,分别为0.2μgm3,rs(7%),表明这一点SOA组件没有影响同一级别的两个监测网站。在成核天期间SOA ISO和SOA销之间观察到澄清的抗相关性,令人惊讶地表明城市新鲜成核颗粒的一些生长可以由生物α-焦烯氧化产品驱动,但是由异戊二烯有机化合物抑制。第三SOA组分由在停滞的大气条件下积聚的老年人的人为和生物学二次有机化合物(SOA老化)的混合物形成,在rs(0.4μgm3)下有助于12%至OA,在UB时为18%(0.4 μgoc m3)。由C7-C9二羧酸形成并尤其在白天检测到的第六组分,被称为“城市含氧有机气溶胶”(oOA城市),因为它在城市Rs(23%;0.8μgOCM3)与UB(10 %;0.2μgocm3),具有明确定义的日间最大值。这种时间趋势和地理分化表明局部人为源正在确定该组分。然而,这些有机分子的变化也受到空气质量轨迹的影响,表明大气条件对该组分有影响,尽管该组分上的特异性起源尚不清楚。它指向由主要城市来源驱动的二级有机成分,包括烹饪和交通(主要是汽油)活动。

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