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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:有机气溶胶老化的见解及煤炭燃烧对中东地区受体遗址的影响

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In order to understand the aging and processing of organic aerosols (OA), an intensive field campaign (Campaign of Air Pollution at Typical Coastal Areas IN Eastern China, CAPTAIN) was conducted March–April at a receptor site (a Changdao island) in central eastern China. Multiple fast aerosol and gas measurement instruments were used during the campaign, including a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) that was applied to measure mass concentrations and non-refractory chemical components of submicron particles (PM1nr). The average mass concentration of PM1(PM1nr+black carbon) was 47 ± 36 μg m?3 during the campaign and showed distinct variation, depending on back trajectories and their overlap with source regions. Organic aerosol (OA) is the largest component of PM1 (30%), followed by nitrate (28%), sulfate (19%), ammonium (15%), black carbon (6%), and chloride (3%). Four OA components were resolved by positive matrix factorization (PMF) of the high-resolution spectra, including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA (CCOA). The mass spectrum of CCOA had high abundance of fragments from polycyclic aromatic hydrocarbons (PAHs) (m/z 128, 152, 178, etc.). The average atomic ratio of oxygen to carbon in OA (O / C) at Changdao was 0.59, which is comparable to other field studies reported at locations downwind of large pollution sources, indicating the oxidized nature of most OA during the campaign. The evolution of OA elemental composition in the van Krevelen diagram (H / C vs. O / C) showed a slope of ?0.63; however, the OA influenced by coal combustion exhibits a completely different evolution that appears dominated by physical mixing. The aging of organic aerosols vs. photochemical age was investigated. It was shown that OA / ΔCO, as well as LV-OOA / ΔCO and SV-OOA / ΔCO, positively correlated with photochemical age. LV-OOA accounted for 73% of the OA secondary formation (SOA) in the oldest plumes (photochemical age of 25 h). The kOH at Changdao, by assuming SOA formation and aging as a first-order process proportional to OH, was calculated to be 5.2 1012 cm3 molec.?1 s?1, which is similar to those determined in recent studies of polluted air in other continents.
机译:为了了解有机气溶胶(OA)的衰老和加工,一个密集的野外运动(中国东部典型沿海地区的空气污染,船长)于3月至4月在中央的一个受体网站(长岛岛)进行了中国东部。在活动期间使用多种快速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),用于测量亚微米颗粒的质量浓度和非耐火材料组分(PM1NR )。在活动期间PM1(PM1NR +黑碳)的平均质量浓度为47±36μgm≤3,并显示出不同的变化,取决于背面轨迹及其与源区的重叠。有机气溶胶(OA)是PM1(30%)的最大成分,其次是硝酸盐(28%),硫酸盐(19%),铵(15%),黑碳(6%)和氯(3%)。通过高分辨率光谱的正基质分解(PMF)解决了四种OA组分,包括低挥发性含氧有机气溶胶(LV-OOA),半挥发性含氧OA(SV-OOA),烃类OA(HOA)和煤炭燃烧OA(CCOA)。 CCOA的质谱具有来自多环芳烃(PAH)(M / Z 128,152,178等)的高丰度。常德OA(O / C)中氧对碳的平均原子比为0.59,与大型污染源下风沿着大型污染源的地点报告的其他场研究相当,表明在活动期间大多数OA的氧化性质。 van Krevelen图中OA元素组成的演变(H / C与O / C)显示出0.63的斜率。然而,受煤燃烧影响的OA具有完全不同的进化,其出现在物理混合中占主导地位。研究了有机气溶胶的老化与光化学时代进行了研究。结果表明,OA /ΔCo,以及LV-OOA /ΔCO和SV-OOA /ΔCo,与光化学时期正相关。 LV-OOA在最古老的羽毛中占OA二级形成(SOA)的73%(25小时的光化学龄)。通过假设SOA形成和老化作为与OH成比例的一阶工艺,常常的KOH被计算为5.21012cm3分子。1 S?1,其类似于在近期污染空气中确定的那些大洲。

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