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

D. J. Bryant; W. J. Dixon; J. R. Hopkins; J. R. Hopkins; R. E. Dunmore; K. L. Pereira; M. Shaw; M. Shaw; F. A. Squires; T. J. Bannan; A. Mehra; S. D. Worrall; S. D. Worrall; A. Bacak; A. Bacak; H. Coe; C. J. Percival; C. J. Percival; L. K. Whalley; L. K. Whalley; D. E. Heard; E. J. Slater; B. Ouyang; B. Ouyang; T. Cui; T. Cui; J. D. Surratt; D. Liu; D. Liu; Z. Shi; Z. Shi; R. Harrison; Y. Sun; W. Xu; A. C. Lewis; A. C. Lewis; J. D. Lee; J. D. Lee; A. R. Rickard; A. R. Rickard; J. F. Hamilton

doi:10.5194/acp-20-7531-2020

Atmospheric Chemistry and Physics (Jun 2020)

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

D. J. Bryant,
W. J. Dixon,
J. R. Hopkins,
J. R. Hopkins,
R. E. Dunmore,
K. L. Pereira,
M. Shaw,
M. Shaw,
F. A. Squires,
T. J. Bannan,
A. Mehra,
S. D. Worrall,
S. D. Worrall,
A. Bacak,
A. Bacak,
H. Coe,
C. J. Percival,
C. J. Percival,
L. K. Whalley,
L. K. Whalley,
D. E. Heard,
E. J. Slater,
B. Ouyang,
B. Ouyang,
T. Cui,
T. Cui,
J. D. Surratt,
D. Liu,
D. Liu,
Z. Shi,
Z. Shi,
R. Harrison,
Y. Sun,
W. Xu,
A. C. Lewis,
A. C. Lewis,
J. D. Lee,
J. D. Lee,
A. R. Rickard,
A. R. Rickard,
J. F. Hamilton

Affiliations

D. J. Bryant: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
W. J. Dixon: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
J. R. Hopkins: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
J. R. Hopkins: National Centre for Atmospheric Science, University of York, York, UK
R. E. Dunmore: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
K. L. Pereira: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
M. Shaw: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
M. Shaw: National Centre for Atmospheric Science, University of York, York, UK
F. A. Squires: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
T. J. Bannan: School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
A. Mehra: School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
S. D. Worrall: School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
S. D. Worrall: now at: Chemical Engineering and Applied Chemistry, School of Engineering and Applied Science, Aston University, Birmingham, UK
A. Bacak: School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
A. Bacak: now at: Turkish Accelerator and Radiation Laboratory, Ankara University Institute of Accelerator Technologies, Ankara, Turkey
H. Coe: School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
C. J. Percival: School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
C. J. Percival: now at: Jet Propulsion Laboratory, California Institute of Technology, 4800 Oak Grove Drive, Pasadena, CA, USA
L. K. Whalley: School of Chemistry, University of Leeds, Leeds, UK
L. K. Whalley: National Centre for Atmospheric Science, University of Leeds, Leeds, UK
D. E. Heard: School of Chemistry, University of Leeds, Leeds, UK
E. J. Slater: School of Chemistry, University of Leeds, Leeds, UK
B. Ouyang: Lancaster Environment Centre, Lancaster University, Lancaster, UK
B. Ouyang: Department of Chemistry, University of Cambridge, Cambridge, UK
T. Cui: Department of Environmental Sciences and Engineering, Gillings School of Global Health, University of North Carolina, Chapel Hill, USA
T. Cui: now at: Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen, Switzerland
J. D. Surratt: Department of Environmental Sciences and Engineering, Gillings School of Global Health, University of North Carolina, Chapel Hill, USA
D. Liu: School of Geography, Earth and Environmental Sciences, the University of Birmingham, Birmingham, UK
D. Liu: now at: State Key Laboratory of Organic Geochemistry and Guangdong Provincial Key Laboratory of Environmental Protection and Resources Utilization, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, PR China
Z. Shi: School of Geography, Earth and Environmental Sciences, the University of Birmingham, Birmingham, UK
Z. Shi: Institute of Surface-Earth System Science, Tianjin University, Tianjin, China
R. Harrison: School of Geography, Earth and Environmental Sciences, the University of Birmingham, Birmingham, UK
Y. Sun: Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, PR China
W. Xu: Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, PR China
A. C. Lewis: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
A. C. Lewis: National Centre for Atmospheric Science, University of York, York, UK
J. D. Lee: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
J. D. Lee: National Centre for Atmospheric Science, University of York, York, UK
A. R. Rickard: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK
A. R. Rickard: National Centre for Atmospheric Science, University of York, York, UK
J. F. Hamilton: Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, UK

DOI: https://doi.org/10.5194/acp-20-7531-2020
Journal volume & issue: Vol. 20
pp. 7531 – 7552

Abstract

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Isoprene-derived secondary organic aerosol (iSOA) is a significant contributor to organic carbon (OC) in some forested regions, such as tropical rainforests and the Southeastern US. However, its contribution to organic aerosol in urban areas that have high levels of anthropogenic pollutants is poorly understood. In this study, we examined the formation of anthropogenically 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-high-performance 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, which was around 3 times higher than the observed concentrations of their oxygenated precursors (2-methyltetrols and 2-methylglyceric acid). OS formation was dependant on both photochemistry and the 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 with previous studies in less polluted environments. The iSOA-derived OSs and NOSs represented 0.62 % of the oxidized organic aerosol measured by aerosol mass spectrometry on average, 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 OS products from heterogenous reactions.

Published in Atmospheric Chemistry and Physics

ISSN: 1680-7316 (Print); 1680-7324 (Online)
Publisher: Copernicus Publications
Country of publisher: Germany
LCC subjects: Science: Physics; Science: Chemistry
Website: http://www.atmospheric-chemistry-and-physics.net/

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