Seasonal Distributions and Stable Carbon Isotope Ratios of Water-Soluble Diacids, Oxoacids, and alpha-Dicarbonyls in Aerosols from Sapporo: Influence of Biogenic Volatile Organic Compounds and Photochemical Aging
Seasonal Distributions and Stable Carbon Isotope Ratios of Water-Soluble Diacids, Oxoacids, and alpha-Dicarbonyls in Aerosols from Sapporo: Influence of Biogenic Volatile Organic Compounds and Photochemical Aging
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札幌气溶胶中水溶性二酸、含氧酸和 α-二羰基的季节分布和稳定碳同位素比：生物挥发性有机化合物和光化学老化的影响
DOI：
10.1021/acsearthspacechem.8b00105
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发表时间：
2018
影响因子：
3.4
通讯作者：
Pingqing Fu
中科院分区：
文献类型：
--
作者：
Ch;ra Mouli Pavuluri;Kimitaka Kawamura;Pingqing Fu
为了更好地了解东北亚地区有机气溶胶的来源和光化学过程，我们研究了日本札幌市采集的大气气溶胶中的二元酸、含氧酸和α-二羰基及其稳定碳同位素比值(δ13C)。二元酸及其相关化合物的分子分布以草酸(C2)为主，其次是丙二酸(C3)、乙醛(ω)C2和琥珀酸(C4)。饱和正二酸(C2-C11，不含C6)和长链含氧酸(ωC7-ωC9)呈现季节性变化，从秋季到冬季逐渐减少，春季逐渐增加，初夏达到高峰。包括二元酸在内的所有物种的短链含氧酸、α-二羰基和δ~(13)C均不表现出季节性变化，~(13)C在饱和的正二酸中呈富集态，碳数减少。短链含氧酸和乙二醛对~(13)C的富集度高于C_2二酸。我们的结果与有机示踪剂一起表明，春季和夏季的季节分布是由增强的生物排放和光化学处理所驱动的。相比之下，生物质燃烧和化石燃料燃烧的贡献率在秋季和冬季较高。这项研究为通过纳入特定季节的生物排放来修正大气化学输送模型提供了启示。
To better understand the origins and photochemical processing of organic aerosols over Northeast Asia, we studied diacids, oxoacids, and α-dicarbonyls and their stable carbon isotope ratios (δ13C) in atmospheric aerosols collected at Sapporo, Japan. Molecular distributions of diacids and related compounds were characterized by a predominance of oxalic acid (C2) followed by malonic (C3), glyoxylic (ωC2), and succinic (C4) acids. Saturated normal diacids (C2–C11, excluding C6) and long-chain oxoacids (ωC7–ωC9) showed a seasonal pattern; gradually decreased from autumn to winter and then increased through spring with a peak in early summer. Short-chain oxoacids and α-dicarbonyls and δ13C of all species including diacids did not show a seasonal pattern.13C was enriched in saturated normal diacids with a decrease in carbon numbers. Short-chain oxoacids and glyoxal were more enriched with13C than C2diacid. Our results together with organic tracers demonstrate that seasonal distributions are driven by enhanced biogenic emissions and photochemical processing in spring/summer. In contrast, the contributions from biomass burning and fossil fuel combustion were higher in autumn and winter. This study provides the insights to modify the atmospheric chemical transport models by the inclusion of season specific biogenic emissions.