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Insights on organic aerosol aging and the influence of coal combustion at a regional receptor site of central eastern China

机译:中国中部东部区域受体点对有机气溶胶老化和燃煤影响的见解

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摘要

In order to understand the aging and processing of organic aerosols (OA), anintensive field campaign (ampaign of irollution at ypical oastalreas Eastern China, CAPTAIN) was conductedMarch–April at a receptor site (a Changdao island) in central eastern China.Multiple fast aerosol and gas measurement instruments were used during thecampaign, including a high resolution time-of-flight aerosol massspectrometer (HR-ToF-AMS) that was applied to measure mass concentrations andnon-refractory chemical components of submicron particles (PM).The average mass concentration of PM(PM+blackcarbon) was 47 ± 36 μg m during the campaign and showeddistinct variation, depending on back trajectories and their overlap withsource regions. Organic aerosol (OA) is the largest component of PM(30%), followed by nitrate (28%), sulfate (19%), ammonium (15%),black carbon (6%), and chloride (3%). Four OA components were resolvedby positive matrix factorization (PMF) of the high-resolution spectra,including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatileoxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA(CCOA). The mass spectrum of CCOA had high abundance of fragments frompolycyclic aromatic hydrocarbons (PAHs) ( 128, 152, 178, etc.). The averageatomic ratio of oxygen to carbon in OA (O / C) at Changdao was 0.59, which iscomparable to other field studies reported at locations downwind of largepollution sources, indicating the oxidized nature of most OA during thecampaign. The evolution of OA elemental composition in the van Krevelendiagram (H / C vs. O / C) showed a slope of −0.63; however, the OA influenced bycoal combustion exhibits a completely different evolution that appearsdominated by physical mixing. The aging of organic aerosols vs.photochemical age was investigated. It was shown that OA / ΔCO, as wellas LV-OOA / ΔCO and SV-OOA / ΔCO, positively correlated withphotochemical age. LV-OOA accounted for 73% of the OA secondary formation(SOA) in the oldest plumes (photochemical age of 25 h). The atChangdao, by assuming SOA formation and aging as a first-order processproportional to OH, was calculated to be 5.2 × 10 cm molec. s, which is similar to those determinedin recent studies of polluted air in other continents.
机译:为了了解有机气溶胶(OA)的老化和加工过程,于3月至4月在中国东部中部的一个接收点(一个长岛)进行了一次密集的野战(典型的中国东部绿洲喷水活动,CAPTAIN)。在活动期间使用了气溶胶和气体测量仪器,包括高分辨率飞行时间气溶胶质谱仪(HR-ToF-AMS),用于测量质量浓度和亚微米颗粒(PM)的非难熔化学成分。竞选期间PM(PM +炭黑)的浓度为47±36μgm,并且表现出明显的变化,具体取决于后向轨迹及其与源区的重叠。有机气溶胶(OA)是PM的最大成分(30%),其次是硝酸盐(28%),硫酸盐(19%),铵(15%),黑碳(6%)和氯化物(3%)。通过高分辨率光谱的正矩阵分解(PMF)解决了四个OA成分,包括低挥发性氧化有机气溶胶(LV-OOA),半挥发性加氧OA(SV-OOA),类烃OA(HOA)和燃煤OA(CCOA)。 CCOA的质谱具有高丰度的多环芳烃(PAHs)碎片(128、152、178等)。长岛的OA中氧气与碳的平均原子比(O / C)为0.59,这与大型污染源顺风处的其他田间研究报告相当,表明大多数OA在活动期间具有氧化性。 van Krevelendendgram中的OA元素组成的演变(H / C与O / C)显示为-0.63的斜率;然而,受煤燃烧影响的OA表现出完全不同的演变,似乎是由物理混合主导的。研究了有机气溶胶的老化与光化学年龄的关系。结果表明,OA /ΔCO,LV-OOA /ΔCO和SV-OOA /ΔCO与光化学年龄呈正相关。 LV-OOA占最老羽(光化学年龄25 h)中OA次要形成(SOA)的73%。通过假设SOA的形成和老化是与OH成比例的一阶过程,在长岛计算得出的摩尔数为5.2×10 cm摩尔。 s,这与最近在其他大洲的空气污染研究中确定的结果相似。

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