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Volume 17, issue 16 | Copyright
Atmos. Chem. Phys., 17, 9979-10000, 2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 25 Aug 2017

Research article | 25 Aug 2017

Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

Wei Hu1,a, Min Hu1,2, Wei-Wei Hu1,b, Jing Zheng1, Chen Chen1, Yusheng Wu1, and Song Guo1 Wei Hu et al.
  • 1State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
  • 2Beijing Innovation Center for Engineering Science and Advanced Technology, Peking University, Beijing 100871, China
  • anow at: Graduate School of Environmental and Symbiotic Sciences, Prefectural University of Kumamoto, Kumamoto 862-8502, Japan
  • bnow at: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA

Abstract. A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31°E, 37.99°N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1±45.8, 37.5±31.0, 41.3±42.7, and 81.7±72.4µgm−3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36% seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55% of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50% in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60–80% to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations (r = 0.53–0.75, p < 0.01) between LO-OOA and odd oxygen (Ox = O3 +NO2), and between MO-OOA and liquid water content in aerosols. BBOA was resolved in spring and autumn, influenced by agricultural biomass burning (e.g., field preparation burnings, straw burning after the harvest). CCOA was only identified in winter due to domestic heating. These results signified that the comprehensive management for biomass burning and coal combustion emissions is needed. High concentrations of chemical components in PM1 in Beijing, especially in winter or in adverse meteorological conditions, suggest that further strengthening the regional emission control of primary particulate and precursors of secondary species is expected.

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Short summary
Seasonal changes in chemical compositions, sources, and evolution for submicron aerosols in the megacity Beijing were investigated based on high-resolution AMS measurements. Carbonaceous fraction (OA+BC) constituted over 50 % of PM1 in autumn due to primary emissions, while SNA contributed 60 % to PM1 in other seasons. Secondary components (OOA+SNA) contributed ~ 60–80 % to PM1, suggesting that secondary formation played an important role in PM pollution. OA was in a relatively high oxidation state.
Seasonal changes in chemical compositions, sources, and evolution for submicron aerosols in the...