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Volume 18, issue 6 | Copyright

Special issue: Multiphase chemistry of secondary aerosol formation under...

Atmos. Chem. Phys., 18, 4005-4017, 2018
https://doi.org/10.5194/acp-18-4005-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 22 Mar 2018

Research article | 22 Mar 2018

Large contribution of fossil fuel derived secondary organic carbon to water soluble organic aerosols in winter haze in China

Yan-Lin Zhang1,2,3,6, Imad El-Haddad3, Ru-Jin Huang3,4, Kin-Fai Ho4,5, Jun-Ji Cao4, Yongming Han4, Peter Zotter3, Carlo Bozzetti3, Kaspar R. Daellenbach3, Jay G. Slowik3, Gary Salazar2, André S. H. Prévôt3, and Sönke Szidat2 Yan-Lin Zhang et al.
  • 1Yale-NUIST Center on Atmospheric Environment, Nanjing University of Information Science and Technology, 210044 Nanjing, China
  • 2Department of Chemistry and Biochemistry & Oeschger Centre for Climate Change Research, University of Bern, 3012 Bern, Switzerland
  • 3Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland
  • 4Key Laboratory of Aerosol Chemistry and Physics, Institute of Earth Environment, Chinese Academy of Sciences, 710061 Xi'an  China
  • 5School of Public Health and Primary Care, The Chinese University of Hong Kong, Hong Kong, China
  • 6Key Laboratory of Meteorological Disaster, Ministry of Education (KLME)/Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters (CIC-FEMD), Nanjing University of Information Science & Technology, Nanjing 210044, China

Abstract. Water-soluble organic carbon (WSOC) is a large fraction of organic aerosols (OA) globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32–47% of WSOC. Secondary organic carbon (SOC) dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61±4 and 50±9% in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36±9%) and Xi'an (26±9%). The most important primary sources were biomass burning emissions, contributing 17–26% of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10%. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban and background regions in Asia, Europe and the USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75±11%) to WSOC aerosols in the Northern Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the eastern Asian pollution outflow, especially during winter, due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.

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Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time of flight aerosol mass spectrometer measurements. We demonstrate a dominant contribution of non-fossil emissions to WSOC aerosols in the Northern Hemisphere. However, the fossil fraction is substantially larger in aerosols from East Asia and the east Asian pollution outflow, especially during winter, due to increasing coal combustion.
Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China...
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