A1 Journal article (refereed)
Towards automated inclusion of autoxidation chemistry in models : from precursors to atmospheric implications (2024)
Pichelstorfer, L., Roldin, P., Rissanen, M., Hyttinen, N., Garmash, O., Xavier, C., Zhou, P., Clusius, P., Foreback, B., Golin, A. T., Deng, C., Baykara, M., Kurten, T., & Boy, M. (2024). Towards automated inclusion of autoxidation chemistry in models : from precursors to atmospheric implications. Environmental Science : Atmospheres, 4(8), 879-896. https://doi.org/10.1039/d4ea00054d
JYU authors or editors
Publication details
All authors or editors: Pichelstorfer, Lukas; Roldin, Pontus; Rissanen, Matti; Hyttinen, Noora; Garmash, Olga; Xavier, Carlton; Zhou, Putian; Clusius, Petri; Foreback, Benjamin; Golin, Almeida Thomas; et al.
Journal or series: Environmental Science : Atmospheres
eISSN: 2634-3606
Publication year: 2024
Publication date: 09/07/2024
Volume: 4
Issue number: 8
Pages range: 879-896
Publisher: Royal Society of Chemistry
Publication country: United Kingdom
Publication language: English
DOI: https://doi.org/10.1039/d4ea00054d
Research data link: https://doi.org/10.5281/zenodo.8087267
Publication open access: Openly available
Publication channel open access: Open Access channel
Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/96637
Publication is parallel published: https://trepo.tuni.fi/handle/10024/159670
Abstract
In the last few decades, atmospheric formation of secondary organic aerosols (SOA) has gained increasing attention due to their impact on air quality and climate. However, methods to predict their abundance are mainly empirical and may fail under real atmospheric conditions. In this work, a close-to-mechanistic approach allowing SOA quantification is presented, with a focus on a chain-like chemical reaction called "autoxidation". A novel framework is employed to (a) describe the gas-phase chemistry, (b) predict the products' molecular structures and (c) explore the contribution of autoxidation chemistry on SOA formation under various conditions. As a proof of concept, the method is applied to benzene, an important anthropogenic SOA precursor. Our results suggest autoxidation to explain up to 100% of the benzene-SOA formed under low-NOx laboratory conditions. Under atmospheric-like day-time conditions, the calculated benzene-aerosol mass continuously forms, as expected based on prior work. Additionally, a prompt increase, driven by the NO3 radical, is predicted by the model at dawn. This increase has not yet been explored experimentally and stresses the potential for atmospheric SOA formation via secondary oxidation of benzene by O3 and NO3.
Keywords: atmosphere (earth); atmospheric sciences; aerosols; aerosol physics; air quality; climate; atmospheric chemistry; molecules; oxidation (passive); benzene; modelling (representation)
Contributing organizations
Ministry reporting: Yes
VIRTA submission year: 2024
Preliminary JUFO rating: 1