Articles | Volume 3, issue 1
https://doi.org/10.5194/ar-3-337-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/ar-3-337-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
16 Jun 2025
Research article |
| 16 Jun 2025
| 16 Jun 2025
Reactive oxygen species buildup in photochemically aged iron- and copper-doped secondary organic aerosol proxy
PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, 5232 Villigen, Switzerland
Department of Environmental System Science, Institute for Atmospheric and Climate Science, ETH Zurich, 8092 Zurich, Switzerland
now at: Physikalisch-Meteorologisches Observatorium Davos, World Radiation Center (PMOD/WRC), 7260 Davos, Switzerland
Alexandre Barth
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Battist Utinger
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Markus Kalberer
Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
Markus Ammann
PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, 5232 Villigen, Switzerland
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R. Anthony Cox, Markus Ammann, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Jürgen Troe, and Timothy J. Wallington
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Sarah S. Steimer, Daniel J. Patton, Tuan V. Vu, Marios Panagi, Paul S. Monks, Roy M. Harrison, Zoë L. Fleming, Zongbo Shi, and Markus Kalberer
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Jan-David Förster, Christian Gurk, Mark Lamneck, Haijie Tong, Florian Ditas, Sarah S. Steimer, Peter A. Alpert, Markus Ammann, Jörg Raabe, Markus Weigand, Benjamin Watts, Ulrich Pöschl, Meinrat O. Andreae, and Christopher Pöhlker
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Pablo Corral Arroyo, Raffael Aellig, Peter A. Alpert, Rainer Volkamer, and Markus Ammann
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Guo Li, Yafang Cheng, Uwe Kuhn, Rongjuan Xu, Yudong Yang, Hannah Meusel, Zhibin Wang, Nan Ma, Yusheng Wu, Meng Li, Jonathan Williams, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Hang Su
Atmos. Chem. Phys., 19, 2209–2232, https://doi.org/10.5194/acp-19-2209-2019, https://doi.org/10.5194/acp-19-2209-2019, 2019
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VOCs play a key role in atmospheric chemistry. Emission and deposition on soil have been suggested as important sources and sinks of atmospheric trace gases. The exchange characteristics and heterogeneous chemistry of VOCs on soil, however, are not well understood. We used a newly designed differential coated-wall flow tube system to investigate the long-term variability of bidirectional air–soil exchange of 13 VOCs at ambient air conditions of an urban background site in Beijing.
Sarah S. Steimer, Aurélie Delvaux, Steven J. Campbell, Peter J. Gallimore, Peter Grice, Duncan J. Howe, Dominik Pitton, Magda Claeys, Thorsten Hoffmann, and Markus Kalberer
Atmos. Chem. Phys., 18, 10973–10983, https://doi.org/10.5194/acp-18-10973-2018, https://doi.org/10.5194/acp-18-10973-2018, 2018
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Aerosol particles are a major public health concern, but particle properties contributing to their toxicity are not well known. Oxidising components such as peroxy acids might contribute significantly to particle toxicity. However, there is a lack of analytical methods for their characterisation. We synthesized three peroxy acids, developed an analysis method and showed that degradation affects peracid yield, likely leading to underestimation of their concentration in conventional analyses.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457, https://doi.org/10.5194/acp-18-10433-2018, https://doi.org/10.5194/acp-18-10433-2018, 2018
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This work helps to better understand the potential climate and health impacts of airborne aerosol particles. We applied a new technique to provide a diagnostic fingerprint of the organic compounds present in aerosols. We followed changes in this fingerprint over time in lab experiments which mimic the conversion of plant emissions into aerosols. Our results compare well with computer simulations of the reactions and we conclude that the technique merits continuing use and development in future.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Peter J. Gallimore, Brendan M. Mahon, Francis P. H. Wragg, Stephen J. Fuller, Chiara Giorio, Ivan Kourtchev, and Markus Kalberer
Atmos. Chem. Phys., 17, 9853–9868, https://doi.org/10.5194/acp-17-9853-2017, https://doi.org/10.5194/acp-17-9853-2017, 2017
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Limonene is emitted in substantial quantities by plants, and also has indoor sources from
air freshenersand cleaning products. We studied particle formation from the oxidation of limonene and found substantial quantities of oxidising components which are thought to be associated with the negative health effects of particulates. State-of-the-art measurements of the products of limonene–ozone chemistry were also presented.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Kinetic process models are efficient tools used to unravel the mechanisms governing chemical and physical transformation in multiphase atmospheric chemistry. However, determination of kinetic parameters such as reaction rate or diffusion coefficients from multiple data sets is often difficult or ambiguous. This study presents a novel optimization algorithm and framework to determine these parameters in an automated fashion and to gain information about parameter uncertainty and uniqueness.
Goran Gržinić, Thorsten Bartels-Rausch, Andreas Türler, and Markus Ammann
Atmos. Chem. Phys., 17, 6493–6502, https://doi.org/10.5194/acp-17-6493-2017, https://doi.org/10.5194/acp-17-6493-2017, 2017
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Nitrogen oxides (NOx) largely control the ozone budget in the troposphere globally. Dinitrogen pentoxide (N2O5) is an important species as a nighttime reservoir for nitrogen oxides. Loss of N2O5 to aerosol particles is therefore important for the budget of NOx and the oxidation capacity. Here we provide direct evidence for its efficient accommodation into aqueous aerosol particles and its fast dissociation, which has not been elucidated as directly in previous studies.
Mingjin Tang, James Keeble, Paul J. Telford, Francis D. Pope, Peter Braesicke, Paul T. Griffiths, N. Luke Abraham, James McGregor, I. Matt Watson, R. Anthony Cox, John A. Pyle, and Markus Kalberer
Atmos. Chem. Phys., 16, 15397–15412, https://doi.org/10.5194/acp-16-15397-2016, https://doi.org/10.5194/acp-16-15397-2016, 2016
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We have investigated for the first time the heterogeneous hydrolysis of ClONO2 on TiO2 and SiO2 aerosol particles at room temperature and at different relative humidities (RHs), using an aerosol flow tube. The kinetic data reported in our current and previous studies have been included in the UKCA chemistry–climate model to assess the impact of TiO2 injection on stratospheric chemistry and stratospheric ozone in particular.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Francis P. H. Wragg, Stephen J. Fuller, Ray Freshwater, David C. Green, Frank J. Kelly, and Markus Kalberer
Atmos. Meas. Tech., 9, 4891–4900, https://doi.org/10.5194/amt-9-4891-2016, https://doi.org/10.5194/amt-9-4891-2016, 2016
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A new portable, online instrument was designed, built and characterised to quantify reactive oxygen species (ROS) in atmospheric aerosols for laboratory and field deployment. ROS are potentially major contributors to the toxicity of particles. Our new instrument allows automated quantification of ROS over days with a detection limit of about 4 nmol [H2O2] equivalents per cubic metre of air, allowing for continuous atmospheric measurements of this important aerosol toxicity parameter.
Laura González Palacios, Pablo Corral Arroyo, Kifle Z. Aregahegn, Sarah S. Steimer, Thorsten Bartels-Rausch, Barbara Nozière, Christian George, Markus Ammann, and Rainer Volkamer
Atmos. Chem. Phys., 16, 11823–11836, https://doi.org/10.5194/acp-16-11823-2016, https://doi.org/10.5194/acp-16-11823-2016, 2016
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The sources of radicals at aerosol surfaces are highly uncertain. Here we investigate the HO2 radical production from the UV irradiation of imidazole-2-carboxaldehyde (IC) in bulk aqueous films containing IC and citric acid, as well as IC in ammonium sulfate aerosols. We find that IC is an efficient photosensitizer that forms HO2 radicals from H-donor chemistry. IC is a proxy species for brown carbon in atmospheric aerosols.
Ivan Kourtchev, Ricardo H. M. Godoi, Sarah Connors, James G. Levine, Alex T. Archibald, Ana F. L. Godoi, Sarah L. Paralovo, Cybelli G. G. Barbosa, Rodrigo A. F. Souza, Antonio O. Manzi, Roger Seco, Steve Sjostedt, Jeong-Hoo Park, Alex Guenther, Saewung Kim, James Smith, Scot T. Martin, and Markus Kalberer
Atmos. Chem. Phys., 16, 11899–11913, https://doi.org/10.5194/acp-16-11899-2016, https://doi.org/10.5194/acp-16-11899-2016, 2016
Guo Li, Hang Su, Xin Li, Uwe Kuhn, Hannah Meusel, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Yafang Cheng
Atmos. Chem. Phys., 16, 10299–10311, https://doi.org/10.5194/acp-16-10299-2016, https://doi.org/10.5194/acp-16-10299-2016, 2016
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Indoor and outdoor formaldehyde (HCHO) are both of considerable concern because of its health effects and its role in atmospheric chemistry. The heterogeneous reactions between gaseous HCHO with soils can pose important impact on both HCHO budget and soil ecosystem. Our results confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions. Soil and soil-derived airborne particles can either act as a source or a sink for HCHO.
D. F. Zhao, A. Buchholz, B. Kortner, P. Schlag, F. Rubach, H. Fuchs, A. Kiendler-Scharr, R. Tillmann, A. Wahner, Å. K. Watne, M. Hallquist, J. M. Flores, Y. Rudich, K. Kristensen, A. M. K. Hansen, M. Glasius, I. Kourtchev, M. Kalberer, and Th. F. Mentel
Atmos. Chem. Phys., 16, 1105–1121, https://doi.org/10.5194/acp-16-1105-2016, https://doi.org/10.5194/acp-16-1105-2016, 2016
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This study investigated the cloud droplet activation behavior and hygroscopic growth of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Cloud droplet activation behaviors of different types of SOA were similar. In contrast, the hygroscopicity of ASOA was higher than BSOA and ABSOA. ASOA components enhanced the hygroscopicity of the ABSOA. Yet this enhancement cannot be described by a linear mixing of pure SOA systems.
G. Gržinić, T. Bartels-Rausch, T. Berkemeier, A. Türler, and M. Ammann
Atmos. Chem. Phys., 15, 13615–13625, https://doi.org/10.5194/acp-15-13615-2015, https://doi.org/10.5194/acp-15-13615-2015, 2015
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The heterogeneous loss of dinitrogen pentoxide (N2O5) to citric acid aerosol, a proxy for highly oxygenated secondary organic aerosol, is shown to be substantially lower than to other aqueous organic aerosol proxies investigated previously. This is attributed to the widely changing viscosity within the atmospherically relevant humidity range. It may explain some of the unexpectedly low loss rates of N2O5 to aerosol particles derived from field studies.
S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, https://doi.org/10.5194/amt-8-2397-2015, 2015
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Atmospheric aerosol is often subject to supersaturated or supercooled conditions where bulk measurements are not possible. Here we demonstrate how measurements using single particle electrodynamic levitation combined with light scattering spectroscopy allow the retrieval of thermodynamic data, optical properties and water diffusivity of such metastable particles even when auxiliary bulk data are not available due to lack of sufficient amounts of sample.
M. J. Tang, M. Shiraiwa, U. Pöschl, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 15, 5585–5598, https://doi.org/10.5194/acp-15-5585-2015, https://doi.org/10.5194/acp-15-5585-2015, 2015
S. S. Steimer, M. Lampimäki, E. Coz, G. Grzinic, and M. Ammann
Atmos. Chem. Phys., 14, 10761–10772, https://doi.org/10.5194/acp-14-10761-2014, https://doi.org/10.5194/acp-14-10761-2014, 2014
M. J. Tang, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 14, 9233–9247, https://doi.org/10.5194/acp-14-9233-2014, https://doi.org/10.5194/acp-14-9233-2014, 2014
M. J. Tang, P. J. Telford, F. D. Pope, L. Rkiouak, N. L. Abraham, A. T. Archibald, P. Braesicke, J. A. Pyle, J. McGregor, I. M. Watson, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 14, 6035–6048, https://doi.org/10.5194/acp-14-6035-2014, https://doi.org/10.5194/acp-14-6035-2014, 2014
M. Ammann, R. A. Cox, J. N. Crowley, M. E. Jenkin, A. Mellouki, M. J. Rossi, J. Troe, and T. J. Wallington
Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, https://doi.org/10.5194/acp-13-8045-2013, 2013
T. Bartels-Rausch, S. N. Wren, S. Schreiber, F. Riche, M. Schneebeli, and M. Ammann
Atmos. Chem. Phys., 13, 6727–6739, https://doi.org/10.5194/acp-13-6727-2013, https://doi.org/10.5194/acp-13-6727-2013, 2013
T. Berkemeier, A. J. Huisman, M. Ammann, M. Shiraiwa, T. Koop, and U. Pöschl
Atmos. Chem. Phys., 13, 6663–6686, https://doi.org/10.5194/acp-13-6663-2013, https://doi.org/10.5194/acp-13-6663-2013, 2013
Related subject area
Aerosols and Health (AH)
Emission dynamics of reactive oxygen species and oxidative potential in particles from a petrol car and wood stove
A rapid semi-quantitative screening method to assess chemicals present in heated e-liquids and e-cigarette aerosols
Battist Utinger, Alexandre Barth, Andreas Paul, Arya Mukherjee, Steven John Campbell, Christa-Maria Müller, Mika Ihalainen, Pasi Yli-Pirilä, Miika Kortelainen, Zheng Fang, Patrick Martens, Markus Somero, Juho Louhisalmi, Thorsten Hohaus, Hendryk Czech, Olli Sippula, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Aerosol Research, 3, 205–218, https://doi.org/10.5194/ar-3-205-2025, https://doi.org/10.5194/ar-3-205-2025, 2025
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The oxidative potential (OP) of air pollution particles might be a metric explaining particle toxicity. This study quantifies the OP of fresh and aged car and wood burning emission particles and explores how the OP changes over time, using novel high-temporal-resolution instruments. We show that emissions from wood burning are more toxic than car exhaust per unit particle mass, especially as they age in the atmosphere. We also calculate emission factors for the OP, which could help to improve air pollution policies.
Natalie Anderson, Paul Pringle, Ryan Mead-Hunter, Benjamin Mullins, Alexander Larcombe, and Sebastien Allard
Aerosol Research, 1, 17–27, https://doi.org/10.5194/ar-1-17-2023, https://doi.org/10.5194/ar-1-17-2023, 2023
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The accelerated vaping (aerosol generation) method described here mimicked typical vaping on an accelerated time frame and could form the basis of a standardized screening tool to test heated e-liquids and their aerosols for harmful or banned substances. This method could help protect consumers in jurisdictions that have banned certain e-liquid chemicals such as Australia, Europe, and the United Kingdom.
Cited articles
Al-Abadleh, H. A.: Iron content in aerosol particles and its impact on atmospheric chemistry, Chem. Commun., 60, 1840–1855, https://doi.org/10.1039/d3cc04614a, 2024. a
Alpert, P. A., Dou, J., Arroyo, P. C., Schneider, F., Xto, J., Luo, B., Peter, T., Huthwelker, T., Borca, C. N., Henzler, K. D., Schaefer, T., Herrmann, H., Raabe, J., Watts, B., Krieger, U. K., and Ammann, M.: Photolytic radical persistence due to anoxia in viscous aerosol particles, Nat. Commun., 12, 12, 1–8, https://doi.org/10.1038/s41467-021-21913-x, 2021. a, b, c, d, e, f, g, h, i
Arangio, A. M., Tong, H., Socorro, J., Pöschl, U., and Shiraiwa, M.: Quantification of environmentally persistent free radicals and reactive oxygen species in atmospheric aerosol particles, Atmos. Chem. Phys., 16, 13105–13119, https://doi.org/10.5194/acp-16-13105-2016, 2016. a
Bates, J. T., Fang, T., Verma, V., Zeng, L., Weber, R. J., Tolbert, P. E., Abrams, J. Y., Sarnat, S. E., Klein, M., Mulholland, J. A., and Russell, A. G.: Review of Acellular Assays of Ambient Particulate Matter Oxidative Potential: Methods and Relationships with Composition, Sources, and Health Effects, Environ. Sci. Technol., 53, 4003–4019, https://doi.org/10.1021/acs.est.8b03430, 2019. a, b
Berglund, G. I., Carlsson, G. H., Smith, A. T., Szöke, H., Henriksen, A., and Hajdu, J.: The catalytic pathway of horseradish peroxidase at high resolution, Nature, 417, 463–468, https://doi.org/10.1038/417463a, 2002. a
Bielski, B. H. J., Cabelli, D. E., Arudi, R. L., and Ross, A. B.: Reactivity of HO2/O2 Radicals in Aqueous Solution, J. Phys. Chem. Ref. Data, 14, 1041–1100, https://doi.org/10.1063/1.555739, 1985. a, b
Boreddy, S. K., Hegde, P., and Aswini, A. R.: Summertime High Abundances of Succinic, Citric, and Glyoxylic Acids in Antarctic Aerosols: Implications to Secondary Organic Aerosol Formation, J. Geophys. Res.-Atmos., 127, 1–17, https://doi.org/10.1029/2021JD036172, 2022. a
Calas, A., Uzu, G., Kelly, F. J., Houdier, S., Martins, J. M. F., Thomas, F., Molton, F., Charron, A., Dunster, C., Oliete, A., Jacob, V., Besombes, J.-L., Chevrier, F., and Jaffrezo, J.-L.: Comparison between five acellular oxidative potential measurement assays performed with detailed chemistry on PM10 samples from the city of Chamonix (France), Atmos. Chem. Phys., 18, 7863–7875, https://doi.org/10.5194/acp-18-7863-2018, 2018. a
Campbell, S. J., Utinger, B., Barth, A., Paulson, S. E., and Kalberer, M.: Iron and Copper Alter the Oxidative Potential of Secondary Organic Aerosol: Insights from Online Measurements and Model Development, Environ. Sci. Technol., 57, 13546–13558, https://doi.org/10.1021/acs.est.3c01975, 2023. a, b, c, d, e
Campbell, S. J., Utinger, B., Barth, A., Leni, Z., Zhang, Z. H., Resch, J., Li, K., Steimer, S. S., Banach, C., Gfeller, B., Wragg, F. P., Westwood, J., Wolfer, K., Bukowiecki, N., Ihalainen, M., Yli-Pirilä, P., Somero, M., Kortelainen, M., Louhisalmi, J., Sklorz, M., Czech, H., di Bucchianico, S., Streibel, T., Delaval, M. N., Ruger, C., Baumlin, N., Salathe, M., Fang, Z., Pardo, M., D’Aronco, S., Giorio, C., Shi, Z., Harrison, R. M., Green, D. C., Kelly, F. J., Rudich, Y., Paulson, S. E., Sippula, O., Zimmermann, R., Geiser, M., and Kalberer, M.: Short-lived reactive components substantially contribute to particulate matter oxidative potential, Sci. Adv., 11, eadp8100, https://doi.org/10.1126/sciadv.adp8100, 2025. a
Cathcart, R., Schwiers, E., and Ames, B. N.: Detection of Picomole Levels of Lipid Hydroperoxides Using a Dichlorofluorescein Fluorescent Assay, Method. Enzymol., 105, 352–358, https://doi.org/10.1016/S0076-6879(84)05047-3, 1983. a
Charrier, J. G., McFall, A. S., Richards-Henderson, N. K., and Anastasio, C.: Hydrogen peroxide formation in a surrogate lung fluid by transition metals and quinones present in particulate matter, Environ. Sci. Technol., 48, 7010–7017, https://doi.org/10.1021/es501011w, 2014. a
Christensen, H. and Sehested, K.: Pulse radiolysis at high temperatures and high pressures, Radiat. Phys. Chem., 18, 723–731, https://doi.org/10.1016/0146-5724(81)90195-3, 1981. a
Christensen, H., Sehested, K., and Corfitzen, H.: Reactions of hydroxyl radicals with hydrogen peroxide at ambient and elevated temperatures, J. Phys. Chem., 86, 1588–1590, https://doi.org/10.1021/j100206a023, 1982. a
Corral Arroyo, P., Bartels-Rausch, T., Alpert, P. A., Dumas, S., Perrier, S., George, C., and Ammann, M.: Particle-Phase Photosensitized Radical Production and Aerosol Aging, Environ. Sci. Technol., 52, 7680–7688, https://doi.org/10.1021/acs.est.8b00329, 2018. a
Daellenbach, K. R., Uzu, G., Jiang, J., Cassagnes, L. E., Leni, Z., Vlachou, A., Stefenelli, G., Canonaco, F., Weber, S., Segers, A., Kuenen, J. J., Schaap, M., Favez, O., Albinet, A., Aksoyoglu, S., Dommen, J., Baltensperger, U., Geiser, M., El Haddad, I., Jaffrezo, J. L., and Prévôt, A. S.: Sources of particulate-matter air pollution and its oxidative potential in Europe, Nature, 587, 414–419, https://doi.org/10.1038/s41586-020-2902-8, 2020. a
Decesari, S., Facchini, M. C., Matta, E., Mircea, M., Fuzzi, S., Chughtai, A. R., and Smith, D. M.: Water soluble organic compounds formed by oxidation of soot, Atmos. Environ., 36, 1827–1832, https://doi.org/10.1016/S1352-2310(02)00141-3, 2002. a
Dellinger, B., Pryor, W. A., Cueto, R., Squadrito, G. L., Hegde, V., and Deutsch, W. A.: Role of free radicals in the toxicity of airborne fine particulate matter, Chem. Res. Toxicol., 14, 1371–1377, https://doi.org/10.1021/tx010050x, 2001. a
Dockery, D. W. and Pope, C. A.: Acute respiratory effects of particulate air pollution, Annu. Rev. Publ. Health, 15, 107–132, https://doi.org/10.1146/annurev.pu.15.050194.000543, 1994. a
Donaldson, K., Stone, V., Seaton, A., and MacNee, W.: Ambient particle inhalation and the cardiovascular system: Potential mechanisms, Environ. Health Persp., 109, 523–527, https://doi.org/10.1289/ehp.01109s4523, 2001. a
Dou, J., Alpert, P. A., Corral Arroyo, P., Luo, B., Schneider, F., Xto, J., Huthwelker, T., Borca, C. N., Henzler, K. D., Raabe, J., Watts, B., Herrmann, H., Peter, T., Ammann, M., and Krieger, U. K.: Photochemical degradation of iron(III) citrate/citric acid aerosol quantified with the combination of three complementary experimental techniques and a kinetic process model, Atmos. Chem. Phys., 21, 315–338, https://doi.org/10.5194/acp-21-315-2021, 2021. a, b, c
Ervens, B., George, C., Williams, J. E., Buxton, G. V., Salmon, G. A., Bydder, M., Wilkinson, F., Dentener, F., Mirabel, P., Wolke, R., and Herrmann, H.: CAPRAM 2.4 (MODAC mechanism): An extended and condensed tropospheric aqueous phase mechanism and its application, J. Geophys. Res.-Atmos., 108, 4426–4447, https://doi.org/10.1029/2002jd002202, 2003. a
Fang, T., Guo, H., Zeng, L., Verma, V., Nenes, A., and Weber, R. J.: Highly Acidic Ambient Particles, Soluble Metals, and Oxidative Potential: A Link between Sulfate and Aerosol Toxicity, Environ. Sci. Technol., 51, 2611–2620, https://doi.org/10.1021/acs.est.6b06151, 2017. a
Fuller, S. J., Wragg, F., Nutter, J., and Kalberer, M.: Comparison of on-line and off-line methods to quantify reactive oxygen species (ROS) in atmospheric aerosols, Atmos. Environ., 92, 97–103, https://doi.org/10.1016/j.atmosenv.2014.04.006, 2014. a, b
Gonzalez, D. H., Cala, C. K., Peng, Q., and Paulson, S. E.: HULIS Enhancement of Hydroxyl Radical Formation from Fe(II): Kinetics of Fulvic Acid-Fe(II) Complexes in the Presence of Lung Antioxidants, Environ. Sci. Technol., 51, 7676–7685, https://doi.org/10.1021/acs.est.7b01299, 2017. a
Graham, B., Mayol-Bracero, O. L., Guyon, P., Roberts, G. C., Decesari, S., Facchini, M. C., Artaxo, P., Maenhaut, W., Köll, P., and Andreae, M. O.: Water-soluble organic compounds in biomass burning aerosols over Amazonia 1. Characterization by NMR and GC-MS, J. Geophys. Res.-Atmos., 107, LBA 14-1–LBA 14-16,https://doi.org/10.1029/2001JD000336, 2002. a
Hong, S., Candelone, J. P., Soutif, M., and Boutron, C. F.: A reconstruction of changes in copper production and copper emissions to the atmosphere during the past 7000 years, Sci. Total Environ., 188, 183–193, https://doi.org/10.1016/0048-9697(96)05171-6, 1996. a
Hug, S. J., Canonica, L., Wegelin, M., Gechter, D., and von Gunten, U.: Solar Oxidation and Removal of Arsenic at Circumneutral pH in Iron Containing Waters, Environ. Sci. Technol., 35, 2114–2121, https://doi.org/10.1021/es001551s, 2001. a
Ito, A. and Miyakawa, T.: Aerosol Iron from Metal Production as a Secondary Source of Bioaccessible Iron, Environ. Sci. Technol., 57, 4091–4100, https://doi.org/10.1021/acs.est.2c06472, 2023. a
Jayson, G. G., Parsons, B. J., and Swallow, A. J.: Oxidation of ferrous ions by hydroxyl radicals, Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, 68, 2053–2058, https://doi.org/10.1039/F19726802053, 1973. a
Kasparoglu, S., Perkins, R., Ziemann, P. J., DeMott, P. J., Kreidenweis, S. M., Finewax, Z., Deming, B. L., DeVault, M. P., and Petters, M. D.: Experimental Determination of the Relationship Between Organic Aerosol Viscosity and Ice Nucleation at Upper Free Tropospheric Conditions, J. Geophys. Res.-Atmos., 127, 1–20, https://doi.org/10.1029/2021JD036296, 2022. a
Kilchhofer, K.: Data availability for the paper 'Reactive Oxygen Species Build-up in Photochemically Aged Iron-and Copper-doped Secondary Organic Aerosol Proxy', Zenodo [data set], https://doi.org/10.5281/zenodo.14505557, 2024. a
Knaapen, A. M., Borm, P. J., Albrecht, C., and Schins, R. P.: Inhaled particles and lung cancer. Part A: Mechanisms, Int. J. Cancer, 109, 799–809, https://doi.org/10.1002/ijc.11708, 2004. a
Laden, F., Schwartz, J., Speizer, F. E., and Dockery, D. W.: Reduction in fine particulate air pollution and mortality: Extended follow-up of the Harvard Six Cities Study, Am. J. Resp. Crit. Care, 173, 667–672, https://doi.org/10.1164/rccm.200503-443OC, 2006. a
Lelieveld, J., Pozzer, A., Pöschl, U., Fnais, M., Haines, A., and Münzel, T.: Loss of life expectancy from air pollution compared to other risk factors: A worldwide perspective, Cardiovasc. Res., 116, 1910–1917, https://doi.org/10.1093/cvr/cvaa025, 2020. a
Lelieveld, S., Wilson, J., Dovrou, E., Mishra, A., Lakey, P. S., Shiraiwa, M., Pöschl, U., and Berkemeier, T.: Hydroxyl Radical Production by Air Pollutants in Epithelial Lining Fluid Governed by Interconversion and Scavenging of Reactive Oxygen Species, Environ. Sci. Technol., 55, 14069–14079, https://doi.org/10.1021/acs.est.1c03875, 2021. a
Lepeule, J., Laden, F., Dockery, D., and Schwartz, J.: Chronic exposure to fine particles and mortality: An extended follow-up of the Harvard six cities study from 1974 to 2009, Environ. Health Persp., 120, 965–970, https://doi.org/10.1289/ehp.1104660, 2012. a
Li, N., Sioutas, C., Cho, A., Schmitz, D., Misra, C., Sempf, J., Wang, M., Oberley, T., Froines, J., and Nel, A.: Ultrafine particulate pollutants induce oxidative stress and mitochondrial damage, Environ. Health Persp., 111, 455–460, https://doi.org/10.1289/ehp.6000, 2003. a
Mao, J., Fan, S., Jacob, D. J., and Travis, K. R.: Radical loss in the atmosphere from Cu-Fe redox coupling in aerosols, Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, 2013. a, b
Murray, B. J., Wilson, T. W., Dobbie, S., Cui, Z., Al-Jumur, S. M. R. K., Möhler, O., Schnaiter, M., Wagner, R., Benz, S., Niemand, M., Saathoff, H., Ebert, V., Wagner, S., and Kärcher, B.: Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions, Nat. Geosci., 3, 233–237, https://doi.org/10.1038/ngeo817, 2010. a
Oettinger, R., Drumm, K., Knorst, M., Krinyak, P., Smolarski, R., and Kienast, K.: Production of reactive oxygen intermediates by human macrophages exposed to soot particles and asbestos fibers and increase in NF-kappa B p50/p105 mRNA, Lung, 177, 343–354, https://doi.org/10.1007/PL00007652, 1999. a
Pai, S. J., Carter, T. S., Heald, C. L., and Kroll, J. H.: Updated World Health Organization Air Quality Guidelines Highlight the Importance of Non-anthropogenic PM2.5, Environmental Science and Technology Letters, 9, 501–506, https://doi.org/10.1021/acs.estlett.2c00203, 2022. a
Prahalad, A. K., Soukup, J. M., Inmon, J., Willis, R., Ghio, A. J., Becker, S., and Gallagher, J. E.: Ambient air particles: Effects on cellular oxidant radical generation in relation to particulate elemental chemistry, Toxicol. Appl. Pharm., 158, 81–91, https://doi.org/10.1006/taap.1999.8701, 1999. a
Preiser, J. C.: Oxidative stress, JPEN-Parenter. Enter., 36, 147–154, https://doi.org/10.1177/0148607111434963, 2012. a
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters, M. D., Pope, F. D., and Rovelli, G.: The viscosity of atmospherically relevant organic particles, Nat. Commun., 9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018. a
Rush, J. D. and Bielski, B. H.: Pulse radiolytic studies of the reactions of HO2/O
Salana, S., Yu, H., Dai, Z., Subramanian, P. S., Puthussery, J. V., Wang, Y., Singh, A., Pope, F. D., Leiva G, M. A., Rastogi, N., Tripathi, S. N., Weber, R. J., and Verma, V.: Inter-continental variability in the relationship of oxidative potential and cytotoxicity with PM2.5 mass, Nat. Commun., 15, 5263, https://doi.org/10.1038/s41467-024-49649-4, 2024. a
Schroeder, W. H., Dobson, M., Kane, D. M., and Johnson, N. D.: Toxic Trace Elements Associated With Airborne Pariacnlaie Matter: A Review, JAPCA J. Air Waste Ma., 37, 1267–1285, https://doi.org/10.1080/08940630.1987.10466321, 1987. a, b
Sehested, K., Rasmussen, O. L., and Fricke, H.: Rate constants of OH with HO2, O
Seraghni, N., Belattar, S., Mameri, Y., Debbache, N., and Sehili, T.: Fe(III)-citrate-complex-induced photooxidation of 3-methylphenol in aqueous solution, Int. J. Photoenergy, 2012, 630425, https://doi.org/10.1155/2012/630425, 2012. a, b
Seraghni, N., Dekkiche, B. A., Debbache, N., Belattar, S., Mameri, Y., Belaidi, S., and Sehili, T.: Photodegradation of cresol red by a non-iron Fenton process under UV and sunlight irradiation: Effect of the copper(II)-organic acid complex activated by H2O2, J. Photoch. Photobio. A, 420, 113485, https://doi.org/10.1016/j.jphotochem.2021.113485, 2021. a
Shen, J., Griffiths, P. T., Campbell, S. J., Utinger, B., Kalberer, M., and Paulson, S. E.: Ascorbate oxidation by iron, copper and reactive oxygen species: review, model development, and derivation of key rate constants, Sci. Rep., 11, 1–14, https://doi.org/10.1038/s41598-021-86477-8, 2021. a
Shiraiwa, M., Ueda, K., Pozzer, A., Lammel, G., Kampf, C. J., Fushimi, A., Enami, S., Arangio, A. M., Fröhlich-Nowoisky, J., Fujitani, Y., Furuyama, A., Lakey, P. S., Lelieveld, J., Lucas, K., Morino, Y., Pöschl, U., Takahama, S., Takami, A., Tong, H., Weber, B., Yoshino, A., and Sato, K.: Aerosol Health Effects from Molecular to Global Scales, Environ. Sci. Technol., 51, 13545–13567, https://doi.org/10.1021/acs.est.7b04417, 2017. a
Tacu, I., Kokalari, I., Abollino, O., Albrecht, C., Malandrino, M., Ferretti, A. M., Schins, R. P., and Fenoglio, I.: Mechanistic Insights into the Role of Iron, Copper, and Carbonaceous Component on the Oxidative Potential of Ultrafine Particulate Matter, Chem. Res. Toxicol., 34, 767–779, https://doi.org/10.1021/acs.chemrestox.0c00399, 2021. a
Tong, H., Liu, F., Filippi, A., Wilson, J., Arangio, A. M., Zhang, Y., Yue, S., Lelieveld, S., Shen, F., Keskinen, H.-M. K., Li, J., Chen, H., Zhang, T., Hoffmann, T., Fu, P., Brune, W. H., Petäjä, T., Kulmala, M., Yao, M., Berkemeier, T., Shiraiwa, M., and Pöschl, U.: Aqueous-phase reactive species formed by fine particulate matter from remote forests and polluted urban air, Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, 2021. a
Tuet, W. Y., Liu, F., De Oliveira Alves, N., Fok, S., Artaxo, P., Vasconcellos, P., Champion, J. A., and Ng, N. L.: Chemical Oxidative Potential and Cellular Oxidative Stress from Open Biomass Burning Aerosol, Environmental Science and Technology Letters, 6, 126–132, https://doi.org/10.1021/acs.estlett.9b00060, 2019. a
Utinger, B., Campbell, S. J., Bukowiecki, N., Barth, A., Gfeller, B., Freshwater, R., Rüegg, H.-R., and Kalberer, M.: An automated online field instrument to quantify the oxidative potential of aerosol particles via ascorbic acid oxidation, Atmos. Meas. Tech., 16, 2641–2654, https://doi.org/10.5194/amt-16-2641-2023, 2023. a
Walling, C.: Fenton's Reagent Revisited, Accounts of Chem. Res., 8, 125–131, https://doi.org/10.1021/ar50088a003, 1975. a
Wang, S., Ye, J., Soong, R., Wu, B., Yu, L., Simpson, A. J., and Chan, A. W. H.: Relationship between chemical composition and oxidative potential of secondary organic aerosol from polycyclic aromatic hydrocarbons, Atmos. Chem. Phys., 18, 3987–4003, https://doi.org/10.5194/acp-18-3987-2018, 2018. a
Wei, J., Yu, H., Wang, Y., and Verma, V.: Complexation of Iron and Copper in Ambient Particulate Matter and Its Effect on the Oxidative Potential Measured in a Surrogate Lung Fluid, Environ. Sci. Technol., 53, 1661–1671, https://doi.org/10.1021/acs.est.8b05731, 2019. a, b
Wong, J. P., Tsagkaraki, M., Tsiodra, I., Mihalopoulos, N., Violaki, K., Kanakidou, M., Sciare, J., Nenes, A., and Weber, R. J.: Effects of Atmospheric Processing on the Oxidative Potential of Biomass Burning Organic Aerosols, Environ. Sci. Technol., 53, 6747–6756, https://doi.org/10.1021/acs.est.9b01034, 2019. a
Wragg, F. P. H., Fuller, S. J., Freshwater, R., Green, D. C., Kelly, F. J., and Kalberer, M.: An automated online instrument to quantify aerosol-bound reactive oxygen species (ROS) for ambient measurement and health-relevant aerosol studies, Atmos. Meas. Tech., 9, 4891–4900, https://doi.org/10.5194/amt-9-4891-2016, 2016. a, b, c, d
Yadav, S. and Phuleria, H. C.: Oxidative Potential of Particulate Matter: A Prospective Measure to Assess PM Toxicity, Springer, Singapore, https://doi.org/10.1007/978-981-15-0540-9_16, 2020. a
Yang, A., Wang, M., Eeftens, M., Beelen, R., Dons, E., Leseman, D. L., Brunekreef, B., Cassee, F. R., Janssen, N. A., and Hoek, G.: Spatial variation and land use regression modeling of the oxidative potential of fine particles, Environ. Health Persp., 123, 1187–1192, https://doi.org/10.1289/ehp.1408916, 2015. a
Yang, Y., Battaglia, M., Mohan, M. K., Robinson, E. S., Peter, F., Edwards, K. C., Fang, T., Kapur, S., Shiraiwa, M., Cesler, M., Simpson, W. R., Campbell, J. R., Mao, J., and Nenes, A.: Assessing the Oxidative Potential of Outdoor PM2.5 in Wintertime Fairbanks, Alaska, ACS ES&T Air, 1, 175–187, https://doi.org/10.1021/acsestair.3c00066, 2024. a
Zhang, Z.-H., Hartner, E., Utinger, B., Gfeller, B., Paul, A., Sklorz, M., Czech, H., Yang, B. X., Su, X. Y., Jakobi, G., Orasche, J., Schnelle-Kreis, J., Jeong, S., Gröger, T., Pardo, M., Hohaus, T., Adam, T., Kiendler-Scharr, A., Rudich, Y., Zimmermann, R., and Kalberer, M.: Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?, Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, 2022. a
Short summary
We report a substantial buildup of reactive molecules (due to sunlight) in organic particulate matter, causing adverse health effects. Metals, which occur naturally or are emitted by traffic, can complex with organic materials and initiate photochemical processes. At low humidity, organic particles may become highly viscous, which allows for the accumulation of reactive species. We found that copper acts as an reducing species to remove some of these harmful species from particles.
We report a substantial buildup of reactive molecules (due to sunlight) in organic particulate...
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