Supplementary material to "Vertical distribution of particle-phase dicarboxylic acids, oxoacids and α-dicarbonyls in the urban boundary layer based on the 325-meter tower in Beijing"

semanticscholar(2020)

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摘要
Abstract. Vertical distribution of dicarboxylic acids, oxoacids, α-dicarbonyls, and other organic tracer compounds in fine aerosols (PM2.5) was investigated from the ground surface (8 m) to 260 m at a 325-meter meteorological tower in Beijing in the summer of 2015. Results showed that the concentrations of oxalic acid (C2), the predominant diacid, were more abundant at 120 m (210 ± 154 ng m−3) and 260 m (220 ± 140 ng m−3) than those at the ground level (160 ± 90 ng m−3). Concentrations of phthalic acid (Ph) decreased with the increase of heights, demonstrating that the vehicular exhausts at the ground surface was the main contributor. Positive correlations were noteworthy for C2/total diacids with mass ratios of C2 to main oxoacids (Pyr, ωC2) and α-dicarbonyls (Gly, MeGly) in polluted days (0.42 ≤ r2 ≤ 0.65), especially at the ground level. In clean days, the ratios of carbon content in oxalic acid to water soluble organic carbon (C2-C/WSOC) showed larger values at 120 m and 260 m than those at the ground surface. However, in polluted days, the C2-C/WSOC ratio mainly reached its maximum at the ground level. These phenomena may indicate the enhanced contribution of aqueous-phase oxidation to oxalic acid in polluted days. Combined with the influence of wind field, total diacids, oxoacids and α-dicarbonyls decreased by 22 %–58 % under the control on anthropogenic activities during the 2015 Victory Parade period. Furthermore, the PMF results showed that the secondary formation routes (secondary sulfate formation and secondary nitrate formation) were the dominant contributors (37–44 %) to organic acids, followed by biomass burning (25–30 %) and motor vehicles (18–24 %). In this study, the organic acids at the ground level were largely associated with local traffic emissions, while the long-range atmospheric transport followed by photochemical aging contributed more to diacids and related compounds in the boundary layer over Beijing than the ground surface.
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