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Volume 13, issue 19 | Copyright

Special issue: Atmospheric impacts of Eastern Asia megacities

Atmos. Chem. Phys., 13, 10095-10112, 2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 15 Oct 2013

Research article | 15 Oct 2013

Insights on organic aerosol aging and the influence of coal combustion at a regional receptor site of central eastern China

W. W. Hu*,1, M. Hu1, B. Yuan**,1, J. L. Jimenez3, Q. Tang1, J. F. Peng1, W. Hu1, M. Shao1, M. Wang1, L. M. Zeng1, Y. S. Wu1, Z. H. Gong2,1, X. F. Huang2,1, and L. Y. He2,1 W. W. Hu et al.
  • 1State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
  • 2Key Laboratory for Urban Habitat Environmental Science and Technology, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen 518055, China
  • 3Cooperative Institute for Research in the Environmental Sciences (CIRES) and Department of Chemistry and Biochemistry, Univ. of Colorado, Boulder, CO, USA
  • *now at: Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO 80309, USA
  • **now at: Earth System Research Laboratory, Chemical Sciences Division, NOAA, 325 Broadway, Boulder, Colorado 80305, USA

Abstract. In order to understand the aging and processing of organic aerosols (OA), an intensive field campaign (Campaign of Air Pollution at Typical Coastal Areas IN Eastern China, CAPTAIN) was conducted March–April at a receptor site (a Changdao island) in central eastern China. Multiple fast aerosol and gas measurement instruments were used during the campaign, including a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) that was applied to measure mass concentrations and non-refractory chemical components of submicron particles (PM1nr). The average mass concentration of PM1(PM1nr+black carbon) was 47 ± 36 μg m−3 during the campaign and showed distinct variation, depending on back trajectories and their overlap with source regions. Organic aerosol (OA) is the largest component of PM1 (30%), followed by nitrate (28%), sulfate (19%), ammonium (15%), black carbon (6%), and chloride (3%). Four OA components were resolved by positive matrix factorization (PMF) of the high-resolution spectra, including low-volatility oxygenated organic aerosol (LV-OOA), semi-volatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA) and a coal combustion OA (CCOA). The mass spectrum of CCOA had high abundance of fragments from polycyclic aromatic hydrocarbons (PAHs) (m/z 128, 152, 178, etc.). The average atomic ratio of oxygen to carbon in OA (O / C) at Changdao was 0.59, which is comparable to other field studies reported at locations downwind of large pollution sources, indicating the oxidized nature of most OA during the campaign. The evolution of OA elemental composition in the van Krevelen diagram (H / C vs. O / C) showed a slope of −0.63; however, the OA influenced by coal combustion exhibits a completely different evolution that appears dominated by physical mixing. The aging of organic aerosols vs. photochemical age was investigated. It was shown that OA / ΔCO, as well as LV-OOA / ΔCO and SV-OOA / ΔCO, positively correlated with photochemical age. LV-OOA accounted for 73% of the OA secondary formation (SOA) in the oldest plumes (photochemical age of 25 h). The kOH at Changdao, by assuming SOA formation and aging as a first-order process proportional to OH, was calculated to be 5.2 × 10−12 cm3 molec.−1 s−1, which is similar to those determined in recent studies of polluted air in other continents.

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