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
, 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

Centre for Atmospheric Science,School of Earth and Environmental Sciences,The University of Manchester,Manchester,UK
Center for Aerosol and Cloud Chemistry,Aerodyne Research Inc,Billerica,USA
Turkish Accelerator & Radiation Laboratory,Ankara University Institute of Accelerator Technologies,06830 Golbasi,Turkey
Department of Chemistry and Molecular Biology,University of Gothenburg,Gothenburg,Sweden
Department of Atmospheric Sciences,School of Earth Sciences,Zhejiang University,Hangzhou,China
State Key Laboratory of Atmospheric Boundary Physics and Atmospheric Chemistry,Institute of Atmospheric Physics,Chinese Academy of Sciences,Beijing 100029,China
Wolfson Atmospheric Chemistry Laboratories,Department of Chemistry,University of York,UK
State Key Joint Laboratory of Environmental Simulation and Pollution Control,College of Environmental Science and Engineering,Peking University,Beijing,China
Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3),Department of Environmental Science & Engineering,Fudan University,Shanghai 200438,China
Center for Aerosol and Cloud Chemistry,Aerodyne Research Inc,Billerica,USA,Cooperative Institute for Research in Environmental Sciences (CIRES)
Division of Environmental Health and Risk Management,School of Geography, Earth and Environmental Sciences,University of Birmingham,Birmingham B15 2TT,UK
School of Chemistry, University of Leeds, Woodhouse Lane, Leeds, LS2 9JT, U.K.
School of Chemistry,University of Leeds,Leeds,UK,National Centre for Atmospheric Science
Lancaster Environment Centre,Lancaster University,Lancaster,UK
Guangzhou Institute of Geochemistry,Guangzhou,China
Institute of Surface-Earth System Science,Tianjin University,Tianjin,China

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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.

Original language	English
Pages (from-to)	382-408
Number of pages	27
Journal	Faraday Discussions
Volume	226
Early online date	21 Jan 2021
DOIs	https://doi.org/10.1039/d0fd00080a
Publication status	Published - 1 Mar 2021

Bibliographical note

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.

Funding: Archit Mehra is fully funded by the Natural Environment Research Council (NERC) and acknowledges his funding through the NERC EAO Doctoral Training Partnership (NE/L002469/1) and CASE partnership support from Aerodyne Research Inc. Funding for this work was provided by the UK Natural Environment Research Council as part of AIRPRO (NE/N00695X/1) and AIRPOLL (NE/N007123/1) alongside UK Natural Environment Research Council and UK Medical Research Council funding under the framework of the Newton Innovation Fund (grant NE/N006976/1).

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 3 Good Health and Well-being
SDG 11 Sustainable Cities and Communities

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10.1039/d0fd00080aLicence: CC BY 3.0

Using highly time-resolved online mass spectrometry
This article is licensed under a Creative Commons Attribution 3.0 Unported Licence.
Final published version, 1.9 MBLicence: CC BY 3.0

Cite this

Mehra, A., Canagaratna, M., Bannan, T. J., Worrall, S. D., Bacak, A., Priestley, M., Liu, D., Zhao, J., Xu, W., Sun, Y., Hamilton, J. F., Squires, F. A., Lee, J., Bryant, D. J., Hopkins, J. R., Elzein, A., Budisulistiorini, S. H., Cheng, X., Chen, Q., ... Coe, H. (2021). Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing. Faraday Discussions, 226, 382-408. https://doi.org/10.1039/d0fd00080a

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

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.",

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

note = "This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Funding: Archit Mehra is fully funded by the Natural Environment Research Council (NERC) and acknowledges his funding through the NERC EAO Doctoral Training Partnership (NE/L002469/1) and CASE partnership support from Aerodyne Research Inc. Funding for this work was provided by the UK Natural Environment Research Council as part of AIRPRO (NE/N00695X/1) and AIRPOLL (NE/N007123/1) alongside UK Natural Environment Research Council and UK Medical Research Council funding under the framework of the Newton Innovation Fund (grant NE/N006976/1).",

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month = mar,

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doi = "10.1039/d0fd00080a",

language = "English",

volume = "226",

pages = "382--408",

journal = "Faraday Discussions",

issn = "1359-6640",

publisher = "Royal Society of Chemistry",

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Mehra, A, Canagaratna, M, Bannan, TJ, Worrall, SD, Bacak, A, Priestley, M, Liu, D, Zhao, J, Xu, W, Sun, Y, Hamilton, JF, Squires, FA, Lee, J, Bryant, DJ, Hopkins, JR, Elzein, A, Budisulistiorini, SH, Cheng, X, Chen, Q, Wang, Y, Wang, L, Stark, H, Krechmer, JE, Brean, J, Slater, E, Whalley, L, Heard, D, Ouyang, B, Acton, WJF, Hewitt, CN, Wang, X, Fu, P, Jayne, J, Worsnop, D, Allan, J, Percival, C & Coe, H 2021, 'Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing', Faraday Discussions, vol. 226, pp. 382-408. https://doi.org/10.1039/d0fd00080a

TY - JOUR

T1 - Using highly time-resolved online mass spectrometry to examine biogenic and anthropogenic contributions to organic aerosol in Beijing

AU - Mehra, Archit

AU - Canagaratna, Manjula

AU - Bannan, Thomas J.

AU - Worrall, Stephen D.

AU - Bacak, Asan

AU - Priestley, Michael

AU - Liu, Dantong

AU - Zhao, Jian

AU - Xu, Weiqi

AU - Sun, Yele

AU - Hamilton, Jacqueline F.

AU - Squires, Freya A.

AU - Lee, James

AU - Bryant, Daniel J.

AU - Hopkins, James R.

AU - Elzein, Atallah

AU - Budisulistiorini, Sri Hapsari

AU - Cheng, Xi

AU - Chen, Qi

AU - Wang, Yuwei

AU - Wang, Lin

AU - Stark, Harald

AU - Krechmer, Jordan E.

AU - Brean, James

AU - Slater, Eloise

AU - Whalley, Lisa

AU - Heard, Dwayne

AU - Ouyang, Bin

AU - Acton, W. Joe F.

AU - Hewitt, C. Nicholas

AU - Wang, Xinming

AU - Fu, Pingqing

AU - Jayne, John

AU - Worsnop, Douglas

AU - Allan, James

AU - Percival, Carl

AU - Coe, Hugh

N1 - This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. Funding: Archit Mehra is fully funded by the Natural Environment Research Council (NERC) and acknowledges his funding through the NERC EAO Doctoral Training Partnership (NE/L002469/1) and CASE partnership support from Aerodyne Research Inc. Funding for this work was provided by the UK Natural Environment Research Council as part of AIRPRO (NE/N00695X/1) and AIRPOLL (NE/N007123/1) alongside UK Natural Environment Research Council and UK Medical Research Council funding under the framework of the Newton Innovation Fund (grant NE/N006976/1).

PY - 2021/3/1

Y1 - 2021/3/1

N2 - 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.

AB - 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.

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VL - 226

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JO - Faraday Discussions

JF - Faraday Discussions

ER -

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

Abstract

Bibliographical note

UN SDGs

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