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Discussion papers
https://doi.org/10.5194/acp-2019-929
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2019-929
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 23 Oct 2019

Submitted as: research article | 23 Oct 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Strong anthropogenic control of secondary organic aerosol formation from isoprene in Beijing

Daniel J. Bryant1, William J. Dixon1, James R. Hopkins1,2, Rachel E. Dunmore1, Kelly L. Pereira1, Marvin Shaw1,2, Freya A. Squires1, Thomas J. Bannan3, Archit Mehra3, Stephen D. Worrall3,a, Asan Bacak3, Hugh Coe3, Carl J. Percival3,b, Lisa K. Whalley2,4, Dwayne E. Heard2,4, Eloise J. Slater4, Bin Ouyang5,6, Tianqu Cui7, Jason D. Surratt7, Di Liu8, Zongbo Shi8,9, Roy Harrison8, Yele Sun10, Weiqi Xu10, Alastair C. Lewis1,2, James D. Lee1,2, Andrew R. Rickard1,2, and Jacqueline F. Hamilton1 Daniel J. Bryant et al.
  • 1Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
  • 2National Centre for Atmospheric Science, University of York, York, UK
  • 3School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
  • 4Schoolof Chemistry, University of Leeds, Leeds, UK
  • 5Lancaster Environment Centre, Lancaster University, Lancaster, UK
  • 6Department of Chemistry, University of Cambridge, Cambridge, UK
  • 7Department of Environmental Sciences and Engineering, Gillings School of Global Health, University of North Carolina, Chapel Hill, USA
  • 8School of Geography Earth and Environmental Sciences, the University of Birmingham, Birmingham, UK
  • 9Institute of Surface-Earth System Science, Tianjin University, Tianjin, China
  • 10Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, People's Republic of China
  • anow at: Chemical Engineering and Applied Chemistry, School of Engineering and Applied Science, Aston University, Birmingham, UK
  • bnow at: Jet Propulsion Laboratory, California Institute of Technology, 4800 Oak Grove Drive, Pasadena, CA, USA

Abstract. Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeast US. However, its contribution to organic aerosol in urban areas, with high levels of anthropogenic pollutants, is poorly understood. In this study we examined the formation of anthropogenic-influenced iSOA during summer in Beijing, China. Local isoprene emissions and high levels of anthropogenic pollutants, in particular NOx and particulate SO42−, led to the formation of iSOA under both high- and low-NO oxidation conditions, with significant heterogeneous transformations of isoprene-derived oxidation products to particulate organosulfates (OSs) and nitrooxy-organosulfates (NOSs). Ultra-pressure liquid chromatography coupled to high-resolution mass spectrometry was combined with a rapid automated data processing technique to quantify 31 proposed iSOA tracers in offline PM2.5 filter extracts. The co-elution of the inorganic ions in the extracts caused matrix effects that impacted two authentic standards differently. The average concentration of iSOA OSs and NOSs was 82.5 ng m−3, around three times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and sulfate available for reactive uptake as shown by a strong correlation with the product of ozone (O3) and particulate sulfate (SO42−). A greater proportion of high-NO OS products were observed in Beijing compared to previous studies in less polluted environments. The iSOA derived OSs and NOSs represented on average 0.62 % of the oxidised organic aerosol measured by aerosol mass spectrometry, but this increased to ~ 3 % on certain days. These results indicate for the first time that iSOA formation in urban Beijing is strongly controlled by anthropogenic emissions and results in extensive conversion to heterogeneous OS products.

Daniel J. Bryant et al.
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Short summary
By studying the chemical composition of offline filter samples, we report a large share of oxidised organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates (OSs) showed a strong correlation to the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate for heterogeneous reactions and further demonstrates iSOA formation is controlled by anthropogenic emissions.
By studying the chemical composition of offline filter samples, we report a large share of...
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