Anthropogenic organic aerosol in Europe produced mainly through second-generation oxidation

Exposure to anthropogenic atmospheric aerosol is a major health issue, causing several million deaths per year worldwide. The oxidation of aromatic hydrocarbons from traffic and wood combustion is an important anthropogenic source of low-volatility species in secondary organic aerosol, especially in heavily polluted environments. It is not yet established whether the formation of anthropogenic secondary organic aerosol involves mainly rapid autoxidation, slower sequential oxidation steps or a combination of the two. Here we reproduced a typical urban haze in the 'Cosmics Leaving Outdoor Droplets' chamber at the European Organization for Nuclear Research and observed the dynamics of aromatic oxidation products during secondary organic aerosol growth on a molecular level to determine mechanisms underlying their production and removal. We demonstrate that sequential oxidation is required for substantial secondary organic aerosol formation. Second-generation oxidation decreases the products' saturation vapour pressure by several orders of magnitude and increases the aromatic secondary organic aerosol yields from a few percent to a few tens of percent at typical atmospheric concentrations. Through regional modelling, we show that more than 70% of the exposure to anthropogenic organic aerosol in Europe arises from second-generation oxidation.

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Publication Details

Journal
Nature Geoscience
Published
2025-03-01
DOI
https://doi.org/10.1038/s41561-025-01645-z
Citations
6
Primary Topic
Atmospheric chemistry and aerosols
Type
article
Field-Weighted Citation Impact
7.80

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article

Anthropogenic organic aerosol in Europe produced mainly through second-generation oxidation

Markku Kulmala, Roy L. Mauldin, Huajun Mai, J. Kirkby et al.
6 citations
Nature Geoscience
Atmospheric chemistry and aerosols
7.80
article

Anthropogenic organic aerosol in Europe produced mainly through second-generation oxidation

Markku Kulmala, Roy L. Mauldin, Huajun Mai, J. Kirkby, Qiaozhi Zha, Victoria Hofbauer, Serge Mathot, Houssni Lamkaddam, Rainer Volkamer, А. Н. Квашнин, Katrianne Lehtipalo, António Tomé, Douglas R. Worsnop, Lukas Fischer, Joachim Curtius, В. С. Махмутов, Martin Heinritzi, Robert Wagner, Josef Dommen, Christian Tauber, Neil M. Donahue, Paul M. Winkler, Xu‐Cheng He, Urs Baltensperger, Chao Yan, Mikko Sipilä, Lubna Dada, Lauri Reino Ahonen, Andreas Kürten, Paulus S. Bauer, Lauriane L. J. Quéléver, C. R. Hoyle, Jianhui Jiang, A. Amorim, Dominik Stolzenburg, Changhyuk Kim, Wei Nie, Tuukka Petäjä, Matti P. Rissanen, Dexian Chen, Imad El Haddad, Randall Chiu, Henning Finkenzeller, Andrea Baccarini, Ugo Molteni, Mario Simon, Penglin Ye, Jonathan Duplissy, Antti Onnela, Armin Hansel, Yuri Stozhkov, Olga Garmаsh, Bernhard Mentler, Yuliang Liu, Mingyi Wang, Boxing Yang, Mao Xiao, Simone Schuchmann
article en
6 citations

Abstract

Exposure to anthropogenic atmospheric aerosol is a major health issue, causing several million deaths per year worldwide. The oxidation of aromatic hydrocarbons from traffic and wood combustion is an important anthropogenic source of low-volatility species in secondary organic aerosol, especially in heavily polluted environments. It is not yet established whether the formation of anthropogenic secondary organic aerosol involves mainly rapid autoxidation, slower sequential oxidation steps or a combination of the two. Here we reproduced a typical urban haze in the 'Cosmics Leaving Outdoor Droplets' chamber at the European Organization for Nuclear Research and observed the dynamics of aromatic oxidation products during secondary organic aerosol growth on a molecular level to determine mechanisms underlying their production and removal. We demonstrate that sequential oxidation is required for substantial secondary organic aerosol formation. Second-generation oxidation decreases the products' saturation vapour pressure by several orders of magnitude and increases the aromatic secondary organic aerosol yields from a few percent to a few tens of percent at typical atmospheric concentrations. Through regional modelling, we show that more than 70% of the exposure to anthropogenic organic aerosol in Europe arises from second-generation oxidation.

Nature GeoscienceVol. 18(3)
Goethe University Frankfurt (DE), P.N. Lebedev Physical Institute of the Russian Academy of Sciences (RU), California Institute of Technology (US), University of Copenhagen (DK), Finnish Meteorological Institute (FI), University of Vienna (AT), University of Helsinki (FI), University of Lisbon (PT), TU Wien (AT), University of Beira Interior (PT), Cooperative Institute for Research in Environmental Sciences (US), Tampere University (FI), University of Colorado Boulder (US), Universität Innsbruck (AT), Johannes Gutenberg University Mainz (DE), Helsinki Institute of Physics (FI), Swiss Federal Institute for Forest, Snow and Landscape Research (CH), Paul Scherrer Institute (CH), NOAA Oceanic and Atmospheric Research (US), ETH Zurich (CH), Aerodyne Research (US), Pusan National University (KR), École Polytechnique Fédérale de Lausanne (CH), East China Normal University (CN), European Organization for Nuclear Research (CH), Carnegie Mellon University (US), Nanjing University (CN)
National Science Foundation, National Aeronautics and Space Administration, CERN, European Commission, Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, National Natural Science Foundation of China, Bundesministerium für Bildung und Forschung, Science and Technology Commission of Shanghai Municipality, Seventh Framework Programme, National Key Research and Development Program of China
Sustainable cities and communities
Openalex Percentile: Top 2%
Atmospheric chemistry and aerosols
7.80
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