Molecular Distributions and 13C Isotopic Composition of Dicarboxylic Acids, Oxocarboxylic Acids, and α‐dicarbonyls in Wintertime PM2.5 at Three Sites Over Northeast Asia: Implications for Origins and Long‐Range Atmospheric Transport

摘要

Abstract To investigate the spatial changes in origins and impact of long‐range transported air masses on organic aerosols (OA) loading and composition over Northeast Asia, fine aerosols (PM2.5) were collected at three sites: Tianjin (TJ), North China and in Padori (PD), and Daejeon (DJ), South Korea, during winter 2019. We studied molecular distributions and compound‐specific stable carbon isotopic composition (δ13C) of dicarboxylic acids, oxocarboxylic acids and α‐dicarbonyls, and carbonaceous and inorganic ionic components in PM2.5. Concentrations of organic carbon was drastically enhanced in haze period compared to that in clean period, but elemental carbon was almost comparable between the two periods. Concentrations of total diacids, oxoacids, and α‐dicarbonyls were higher at TJ followed by DJ and PD during haze period and at DJ followed by TJ and PD during clean period. On average, oxalic acid (C2) was the most abundant among measured species at all three sites, followed by methyl glyoxal (MeGly) and glyoxylic acid (ωC2) at TJ and DJ, and succinic acid (C4) and ωC2 were almost equal and second most abundant followed by MeGly at PD. Based on the mass ratios and linear relations of selected species together with δ13C of diacids and related compounds, we found that contributions of OA from biomass burning/biogenic emissions and their aging were higher at TJ and PD, whereas at DJ, emissions from anthropogenic sources and in situ secondary formation were also important. Furthermore, this study implies that long‐range atmospheric transport of aerosols from source regions to downwind regions are substantial over Northeast Asia.