12 Aug 2021

12 Aug 2021

Review status: this preprint is currently under review for the journal ACP.

Are reactive oxygen species (ROS) a suitable metric to predict toxicity of carbonaceous aerosol particles?

Zhi-Hui Zhang1,2, Elena Hartner3,4, Battist Utinger1, Benjamin Gfeller1, Andreas Paul5, Martin Sklorz3, Hendryk Czech3,4, Bin Xia Yang6, Xin Yi Su6, Gert Jakobi3, Jürgen Orasche3, Jürgen Schnelle-Kreis3, Seongho Jeong3,4, Thomas Gröger3, Michal Pardo7, Thorsten Hohaus5, Thomas Adam8, Astrid Kiendler-Scharr5, Yinon Rudich7, Ralf Zimmermann3,4, and Markus Kalberer1,2 Zhi-Hui Zhang et al.
  • 1Department of Environmental Sciences, University of Basel, 4056 Basel, Switzerland
  • 2Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, UK
  • 3Joint Mass Spectrometry, Cooperation Group “Comprehensive Molecular Analytics” (CMA), Zentrum München, 81379 München, Germany
  • 4Joint Mass Spectrometry Centre, Chair of Analytical Chemistry , University of Rostock, 18059 Rostock, Germany
  • 5Forschungzentrum Jülich, IEK-8: Troposphere, Jülich, Germany
  • 6Institute of Molecular and Cell Biology (IMCB), Agency for Science, Technology and Research (A*STAR), Singapore
  • 7Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot 76100, Israel
  • 8Universität der Bundeswehr München, 85577 Neubiberg, Germany

Abstract. It is being suggested that particle-bound or particle-induced reactive oxygen species (ROS), which significantly contribute to the oxidative potential (OP) of aerosol particles, are a promising metric linking aerosol compositions to toxicity and adverse health effects. However, accurate ROS quantification remains challenging due to the reactive and short-lived nature of many ROS components and the lack of appropriate analytical methods for a reliable quantification. Consequently, it remains difficult to gauge their impact on human health, especially to identify how aerosol particle sources and atmospheric processes drive particle-bound ROS formation in a real-world urban environment.

In this study, using a novel online particle-bound ROS instrument (OPROSI), we comprehensively characterized and compared the formation of ROS in secondary organic aerosols (SOA) generated from organic compounds that represent anthropogenic (naphthalene, SOANAP) and biogenic (β-pinene, SOAβPIN) precursors. The SOA mass was condensed onto soot particles (SP) under varied atmospherically relevant conditions (photochemical aging and humidity). We systematically analysed the ability of the aqueous extracts of the two aerosol types (SOANAP-SP and SOAβPIN-SP) to induce ROS production and OP. We further investigated cytotoxicity and cellular ROS production after exposing human lung epithelial cell cultures (A549) to extracts of the two aerosols. A significant finding of this study is that more than 90 % of all ROS components in both SOA types have a short lifetime, highlighting the need to develop online instruments for a meaningful quantification of ROS. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the OP of the aerosols. Compared to SOAβPIN-SP, SOANAP-SP elicited a higher acellular and cellular ROS production, a higher OP and a lower cell viability. These consistent results between chemical-based and biological-based analyses indicate that particle-bound ROS quantification could be a feasible metric to predict aerosol particle toxicity and adverse human effects. Moreover, the cellular ROS production caused by SOA exposure not only depends on aerosol type, but is also affected by exposure dose, highlighting a need to mimic the process of particle deposition onto lung cells and their interactions as realistically as possible to avoid unknown biases.

Zhi-Hui Zhang et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-666', Anonymous Referee #1, 16 Sep 2021
  • RC2: 'Comment on acp-2021-666', Anonymous Referee #2, 21 Sep 2021
  • RC3: 'Comment on acp-2021-666', Anonymous Referee #3, 21 Sep 2021

Zhi-Hui Zhang et al.

Zhi-Hui Zhang et al.


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Short summary
Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOA). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.