Bhagawati Kunwar, Ambarish Pokhrel, Takeji Niwai and Kimitaka Kawamura*,
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Their averaged molecular distributions over the SO showed the predominance of acetic acid (C<sub>2</sub>) (5.2 ng m<sup>–3</sup>) followed by formic (C<sub>1</sub>) (4.1 ng m<sup>–3</sup>), nonanoic (C<sub>9</sub>), and decanoic acid (C<sub>10</sub>), whereas over the WP, the concentrations of C<sub>1</sub> (9.7 ng m<sup>–3</sup>) and C<sub>2</sub> (9.6) are in a similar level followed by C<sub>9</sub> and C<sub>10</sub>. The molecular distributions of branched-chain monoacids (iC<sub>5</sub> > iC<sub>4</sub>) are similar to those obtained by the laboratory oxidation of isoprene (C<sub>5</sub>), suggesting that isoprene oxidation is an important source for those acids. We found a different source of formic and acetic acid over the SO. Regression analysis (<i>R</i><sup>2</sup> = 0.67, <i>p</i> < 0.01) of formic acid with total sulfur suggests a link to biogenic dimethyl sulfide (DMS) via photochemical oxidation, whereas C<sub>2</sub> is suggested to form via the degradation of iC<sub>5</sub>, C<sub>7</sub>, and C<sub>8</sub> over the SO. 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This study provides new findings on spatial distributions and chemical compositions of monoacids in marine aerosols from the Western Pacific (WP) and Southern Ocean (SO). In addition, we disclose the formation mechanism of monoacids in the WP and SO. Marine aerosol samples (<i>n</i> = 27) were collected over the oceans and analyzed for LMW monoacids (C<sub>1</sub>–C<sub>10</sub>). Normal and branched chains (iC<sub>4</sub>, iC<sub>5</sub>, and iC<sub>6</sub>) and aromatic acids (benzoic and toluic) were detected over the WP and SO. Their averaged molecular distributions over the SO showed the predominance of acetic acid (C<sub>2</sub>) (5.2 ng m<sup>–3</sup>) followed by formic (C<sub>1</sub>) (4.1 ng m<sup>–3</sup>), nonanoic (C<sub>9</sub>), and decanoic acid (C<sub>10</sub>), whereas over the WP, the concentrations of C<sub>1</sub> (9.7 ng m<sup>–3</sup>) and C<sub>2</sub> (9.6) are in a similar level followed by C<sub>9</sub> and C<sub>10</sub>. 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引用次数: 0
摘要
低分子量(LMW)单羧酸具有吸湿性,因此对云的激活能力和全球气候系统有影响。本研究对西太平洋(WP)和南大洋(SO)海洋气溶胶中单酸的空间分布和化学组成有了新的发现。此外,我们还揭示了单酸在水杨浆和水杨浆中形成的机理。在海洋上收集了海洋气溶胶样品(n = 27),并分析了LMW单酸(C1-C10)。正常链和支链(iC4, iC5和iC6)和芳香酸(苯甲酸和甲苯)在WP和SO上被检测到。它们在SO上的平均分子分布显示乙酸(C2) (5.2 ng m-3)优势,其次是甲酸(C1) (4.1 ng m-3)、壬酸(C9)和癸酸(C10),而在WP上,C1 (9.7 ng m-3)和C2(9.6)的浓度相似,其次是C9和C10。支链单酸(iC5 >;iC4)与实验室氧化异戊二烯(C5)得到的酸相似,表明异戊二烯氧化是这些酸的重要来源。我们在SO上发现了不同来源的甲酸和乙酸。回归分析(R2 = 0.67, p <;甲酸与总硫的比值为0.01)表明生物二甲基硫(DMS)是通过光化学氧化形成的,而C2则是通过在SO上降解iC5、C7和C8形成的。相比之下,在WP上,生物源和人为活动的混合来源可能影响海洋气溶胶中甲酸和乙酸的分布。
Molecular Distributions and Sources of Water-Soluble Monocarboxylic Acids (C1–C10) in the Marine Aerosols Collected from the Western Pacific and Southern Ocean
Low molecular weight (LMW) monocarboxylic acids (monoacids) are hygroscopic in nature and thus have an impact on cloud activation ability and the global climate system. This study provides new findings on spatial distributions and chemical compositions of monoacids in marine aerosols from the Western Pacific (WP) and Southern Ocean (SO). In addition, we disclose the formation mechanism of monoacids in the WP and SO. Marine aerosol samples (n = 27) were collected over the oceans and analyzed for LMW monoacids (C1–C10). Normal and branched chains (iC4, iC5, and iC6) and aromatic acids (benzoic and toluic) were detected over the WP and SO. Their averaged molecular distributions over the SO showed the predominance of acetic acid (C2) (5.2 ng m–3) followed by formic (C1) (4.1 ng m–3), nonanoic (C9), and decanoic acid (C10), whereas over the WP, the concentrations of C1 (9.7 ng m–3) and C2 (9.6) are in a similar level followed by C9 and C10. The molecular distributions of branched-chain monoacids (iC5 > iC4) are similar to those obtained by the laboratory oxidation of isoprene (C5), suggesting that isoprene oxidation is an important source for those acids. We found a different source of formic and acetic acid over the SO. Regression analysis (R2 = 0.67, p < 0.01) of formic acid with total sulfur suggests a link to biogenic dimethyl sulfide (DMS) via photochemical oxidation, whereas C2 is suggested to form via the degradation of iC5, C7, and C8 over the SO. In contrast, over the WP, it is likely that mixed sources of biogenic and anthropogenic activities influenced the distributions of formic and acetic acids in marine aerosols.
期刊介绍:
The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.