Urban organic aerosol composition in eastern China differs from north to south: molecular insight from a liquid chromatography–mass spectrometry (Orbitrap) study

Wang, Kai; Huang, Ru-Jin; Brüggemann, Martin; Zhang, Yun; Yang, Lu; Ni, Haiyan; Guo, Jie; Wang, Meng; Han, Jiajun; Bilde, Merete; Glasius, Marianne; Hoffmann, Thorsten

Air pollution by particulate matter in China affects human health, the ecosystem and the climate. However, the chemical composition of particulate aerosol, especially of the organic fraction, is still not well understood. In this study, particulate aerosol samples with a diameter of inline-formula≤2.5inline-formulaµm (inline-formulaPM2.5) were collected in January 2014 in three cities located in northeast, east and southeast China, namely Changchun, Shanghai and Guangzhou. Organic aerosol (OA) in the inline-formulaPM2.5 samples was analyzed by an ultrahigh-performance liquid chromatograph (UHPLC) coupled to a high-resolution Orbitrap mass spectrometer in both negative mode (ESI-) and positive mode electrospray ionization (ESI+). After non-target screening including the assignment of molecular formulas, the compounds were classified into five groups based on their elemental composition, i.e., CHO, CHON, CHN, CHOS and CHONS. The CHO, CHON and CHN groups present the dominant signal abundances of 81 %–99.7 % in the mass spectra and the majority of these compounds were assigned to mono- and polyaromatics, suggesting that anthropogenic emissions are a major source of urban OA in all three cities. However, the chemical characteristics of these compounds varied between the different cities. The degree of aromaticity and the number of polyaromatic compounds were substantially higher in samples from Changchun, which could be attributed to the large emissions from residential heating (i.e., coal combustion) during wintertime in northeast China. Moreover, the ESI- analysis showed higher inline-formula M5inlinescrollmathml chem normal H / normal C 24pt14ptsvg-formulamathimg83ae2b3ee9ce962b1864509e19943551 acp-21-9089-2021-ie00001.svg24pt14ptacp-21-9089-2021-ie00001.png and inline-formula M6inlinescrollmathml chem normal O / normal C 25pt14ptsvg-formulamathimgfb9e1248ce2bf802c7c3ce2f343b712f acp-21-9089-2021-ie00002.svg25pt14ptacp-21-9089-2021-ie00002.png ratios for organic compounds in Shanghai and Guangzhou compared to samples from Changchun, indicating that OA undergoes more intense photochemical oxidation processes in lower-latitude regions of China and/or is affected to a larger degree by biogenic sources. The majority of sulfur-containing compounds (CHOS and CHONS) in all cities were assigned to aliphatic compounds with low degrees of unsaturation and aromaticity. Here again, samples from Shanghai and Guangzhou show a greater chemical similarity but differ largely from those from Changchun. It should be noted that the conclusions drawn in this study are mainly based on comparison of molecular formulas weighted by peak abundance and thus are associated with inherentpage9090 uncertainties due to different ionization efficiencies for different organic species.



Wang, Kai / Huang, Ru-Jin / Brüggemann, Martin / et al: Urban organic aerosol composition in eastern China differs from north to south: molecular insight from a liquid chromatography–mass spectrometry (Orbitrap) study. 2021. Copernicus Publications.


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