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Origins and composition of fine atmospheric carbonaceous aerosol in the Sierra Nevada Mountains, California

机译:塞拉尼达山脉山脉塞拉尼达山脉的精细大气碳质气溶胶的起源和组成

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In this paper we report chemically resolved measurements of organic aerosol (OA) and related tracers during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX) at the Blodgett Forest Research Station, California from 15 August–10 October 2007. OA contributed the majority of the mass to the fine atmospheric particles and was predominately oxygenated (OOA). The highest concentrations of OA were during sporadic wildfire influence when aged plumes were impacting the site. In situ measurements of particle phase molecular markers were dominated by secondary compounds and along with gas phase compounds could be categorized into six factors or sources: (1) aged biomass burning emissions and oxidized urban emissions, (2) oxidized urban emissions (3) oxidation products of monoterpene emissions, (4) monoterpene emissions, (5) anthropogenic emissions and (6) local methyl chavicol emissions and oxidation products. There were multiple biogenic components that contributed to OA at this site whose contributions varied diurnally, seasonally and in response to changing meteorological conditions, e.g. temperature and precipitation events. Concentrations of isoprene oxidation products were larger when temperatures were higher during the first half of the campaign (15 August–12 September) due to more substantial emissions of isoprene and enhanced photochemistry. The oxidation of methyl chavicol, an oxygenated terpene emitted by ponderosa pine trees, contributed similarly to OA throughout the campaign. In contrast, the abundances of monoterpene oxidation products in the particle phase were greater during the cooler conditions in the latter half of the campaign (13 September–10 October), even though emissions of the precursors were lower, although the mechanism is not known. OA was correlated with the anthropogenic tracers 2-propyl nitrate and carbon monoxide (CO), consistent with previous observations, while being comprised of mostly non-fossil carbon (75%). The correlation between OA and an anthropogenic tracer does not necessarily identify the source of the carbon as being anthropogenic but instead suggests a coupling between the anthropogenic and biogenic components in the air mass that might be related to the source of the oxidant and/or the aerosol sulfate. Observations of organosulfates of isoprene and -pinene provided evidence for the likely importance of aerosol sulfate in spite of neutralized aerosol although acidic plumes might have played a role upwind of the site. This is in contrast to laboratory studies where strongly acidic seed aerosols were needed in order to form these compounds. These compounds together represented only a minor fraction (1%) of the total OA mass, which may be the result of the neutralized aerosol at the site or because only a small number of organosulfates were quantified. The low contribution of organosulfates to total OA suggests that other mechanisms, e.g. NOx enhancement of oxidant levels, are likely responsible for the majority of the anthropogenic enhancement of biogenic secondary organic aerosol observed at this site.
机译:在本文中,我们在加利福尼亚州于2007年8月15日至10日 - 加利福尼亚州的Blodgett Forest Research Station(Bearpex)的生物圈效果中报告了有机气溶胶(OA)和相关示踪剂的化学解决的有机气溶胶(OA)和相关示踪剂。OA贡献了大多数质量为细常压颗粒,主要是含氧(OOA)。当老化的羽毛撞击该部位时,最高浓度的OA在散发性野火影响中。在原位测量粒子相分子标记的测量由二次化合物固定,并且随着气相化合物可以分为六个因素或来源:(1)老年生物质燃烧排放和氧化的城市排放,(2)氧化城市排放(3)氧化单萜排放产品,(4)单萜排放,(5)人为排放量和(6)局部甲基凝血剂排放和氧化产品。有多种生物成分,这些组分有助于在本网站上的OA,其贡献在季节性变化,季节性和响应于变化的气象条件,例如。温度和降水事件。由于异戊二烯的更大量排放和增强的光化学,当竞选活动的上半年(8月12日至9月12日)在竞选中的上半场(8月12日)时,异戊二烯氧化产品的浓度较大。甲基凝血醇的氧化,由Ponderosa松树发射的含氧萜烯,在整个活动中与OA类似地贡献。相反,在竞选中的一半(10月13日至10月13日)中,粒子阶段中的单萜氧化产物的丰富是更大的,尽管前体的排放较低,但是该机制尚不清楚。 OA与与先前观察结果一致的人为硝酸丙酯2-硝酸丙酯和一氧化碳(CO)相关,同时由大多数非化石碳(> 75%)组成。 OA和人为示踪剂之间的相关性不一定将碳的源识别为人为的碳源,而是表明在空气质量中的人为和生物成分之间的偶联可能与氧化剂和/或气溶胶的来源有关硫酸盐。异戊二烯和 - 丁烯有机硫酸盐的观察提供了气溶胶硫酸盐的可能重要性,尽管酸性羽毛可能发挥了该部位的作用逆风。这与实验室研究形成鲜明地,以便形成这些化合物需要强烈酸性的种子气溶胶。这些化合物在一起仅代表了总OA质量的小部分(1%),这可能是现场中和中和气溶胶的结果,或者由于仅量化少量有机硫酸盐。有机硫酸盐对整体OA的低贡献表明,其他机制,例如, NOx增强氧化剂水平,可能负责在该网站观察到的生物学中学有机气溶胶的大多数人为增强。
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