Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing

Archit Mehra; Manjula Canagaratna; Thomas J. Bannan; Stephen D. Worrall; Asan Bacak; Michael Priestley; Dantong Liu; Jian Zhao; Weiqi Xu; Yele Sun; Jacqueline F. Hamilton; Freya A. Squires; James Lee; Daniel J. Bryant; James R. Hopkins; Atallah Elzein; Sri Hapsari Budisulistiorini; Xi Cheng; Qi Chen; Yuwei Wang; Lin Wang; Harald Stark; Jordan E. Krechmer; James Brean; Eloise Slater; Lisa Whalley; Dwayne Heard; Bin Ouyang; W. Joe F. Acton; C. Nicholas Hewitt; Xinming Wang; Pingqing Fu; John Jayne; Douglas Worsnop; James Allan; Carl Percival; Hugh Coe

doi:10.1039/D0FD00080A

Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing†

Archit Mehra,

^a Manjula Canagaratna,^b Thomas J. Bannan,

^a Stephen D. Worrall,

^c Asan Bacak,^d Michael Priestley,^e Dantong Liu,^f Jian Zhao,^g Weiqi Xu,^g Yele Sun,

^g Jacqueline F. Hamilton,^h Freya A. Squires,

^h James Lee,

^h Daniel J. Bryant,^h James R. Hopkins,^h Atallah Elzein,^h Sri Hapsari Budisulistiorini,

^h Xi Cheng,ⁱ Qi Chen,ⁱ Yuwei Wang,^j Lin Wang,

^j Harald Stark,^bkl Jordan E. Krechmer,

^b James Brean,^m Eloise Slater,ⁿ Lisa Whalley,^no Dwayne Heard,

ⁿ Bin Ouyang,^p W. Joe F. Acton,^p C. Nicholas Hewitt,

^p Xinming Wang,

^q Pingqing Fu,

^r John Jayne,^b Douglas Worsnop,^b James Allan,^as Carl Percival

‡^a and Hugh Coe*^aj

Author affiliations

* Corresponding authors

^a Centre for Atmospheric Science, School of Earth and Environmental Sciences, The University of Manchester, Manchester, UK
E-mail: hugh.coe@manchester.ac.uk

^b Center for Aerosol and Cloud Chemistry, Aerodyne Research Inc, Billerica, Massachusetts, USA

^c Aston Institute of Materials Research, School of Engineering and Applied Science, Aston University, Birmingham, UK

^d Turkish Accelerator & Radiation Laboratory, Ankara University Institute of Accelerator Technologies, Gölbaşı Campus, 06830 Golbasi, Ankara, Turkey

^e Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden

^f Department of Atmospheric Sciences, School of Earth Sciences, Zhejiang University, Hangzhou, Zhejiang, China

^g State Key Laboratory of Atmospheric Boundary Physics and Atmospheric Chemistry, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China

^h Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, UK

ⁱ State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Science and Engineering, Peking University, Beijing, China

^j Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science & Engineering, Fudan University, Jiangwan Campus, Shanghai 200438, China

^k Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO 80309, USA

^l Department of Chemistry, University of Colorado, Boulder, CO 80309, USA

^m Division of Environmental Health and Risk Management, School of Geography, Earth and Environmental Sciences, University of Birmingham, Edgbaston, Birmingham B15 2TT, UK

ⁿ School of Chemistry, University of Leeds, Leeds, UK

^o National Centre for Atmospheric Science, University of Leeds, Leeds, UK

^p Lancaster Environment Centre, Lancaster University, Lancaster, UK

^q Guangzhou Institute of Geochemistry, Guangzhou, China

^r Institute of Surface-Earth System Science, Tianjin University, Tianjin, China

^s National Centre for Atmospheric Science, University of Manchester, Manchester, UK

Abstract

Organic aerosols, a major constituent of fine particulate mass in megacities, can be directly emitted or formed from secondary processing of biogenic and anthropogenic volatile organic compound emissions. The complexity of volatile organic compound emission sources, speciation and oxidation pathways leads to uncertainties in the key sources and chemistry leading to formation of organic aerosol in urban areas. Historically, online measurements of organic aerosol composition have been unable to resolve specific markers of volatile organic compound oxidation, while offline analysis of markers focus on a small proportion of organic aerosol and lack the time resolution to carry out detailed statistical analysis required to study the dynamic changes in aerosol sources and chemistry. Here we use data collected as part of the joint UK–China Air Pollution and Human Health (APHH-Beijing) collaboration during a field campaign in urban Beijing in the summer of 2017 alongside laboratory measurements of secondary organic aerosol from oxidation of key aromatic precursors (1,3,5-trimethyl benzene, 1,2,4-trimethyl benzene, propyl benzene, isopropyl benzene and 1-methyl naphthalene) to study the anthropogenic and biogenic contributions to organic aerosol. For the first time in Beijing, this study applies positive matrix factorisation to online measurements of organic aerosol composition from a time-of-flight iodide chemical ionisation mass spectrometer fitted with a filter inlet for gases and aerosols (FIGAERO-ToF-I-CIMS). This approach identifies the real-time variations in sources and oxidation processes influencing aerosol composition at a near-molecular level. We identify eight factors with distinct temporal variability, highlighting episodic differences in OA composition attributed to regional influences and in situ formation. These have average carbon numbers ranging from C₅–C₉ and can be associated with oxidation of anthropogenic aromatic hydrocarbons alongside biogenic emissions of isoprene, α-pinene and sesquiterpenes.

This article is part of the themed collection: Air quality in megacities

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Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing†

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Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing

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