Characterization and Quantification of Particle-Bound Criegee Intermediates in Secondary Organic Aerosol

Campbell, Steven J. and Wolfer, Kate and Gallimore, Peter J. and Giorio, Chiara and Häussinger, Daniel and Boillat, Marc-Aurèle and Kalberer, Markus. (2022) Characterization and Quantification of Particle-Bound Criegee Intermediates in Secondary Organic Aerosol. Environmental Science and Technology, 56 (18). pp. 12945-12954.

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Official URL: https://edoc.unibas.ch/92612/

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The ozonolysis of alkenes contributes substantially to the formation of secondary organic aerosol (SOA), which are important modulators of air quality and the Earth's climate. Criegee intermediates (CIs) are abundantly formed through this reaction. However, their contributions to aerosol particle chemistry remain highly uncertain. In this work, we present the first application of a novel methodology, using spin traps, which simultaneously quantifies CIs produced from the ozonolysis of volatile organic compounds in the gas and particle phases. Only the smallest CI with one carbon atom was detected in the gas phase of a β-caryophyllene ozonolysis reaction system. However, multiple particle-bound CIs were observed in β-caryophyllene SOA. The concentration of the most abundant CI isomer in the particle phase was estimated to constitute ∼0.013% of the SOA mass under atmospherically relevant conditions. We also demonstrate that the lifetime of CIs in highly viscous SOA particles is at least on the order of minutes, substantially greater than their gas-phase lifetime. The confirmation of substantial concentrations of large CIs with elongated lifetimes in SOA raises new questions regarding their influence on the chemical evolution of viscous SOA particles, where CIs may be a previously underestimated source of reactive species.
Faculties and Departments:05 Faculty of Science > Departement Chemie > Chemie > Nuclear Magnetic Resonance (Häussinger)
05 Faculty of Science > Departement Umweltwissenschaften > Geowissenschaften > Atmospheric Sciences (Kalberer)
UniBasel Contributors:Kalberer, Markus and Häussinger, Daniel
Item Type:Article, refereed
Article Subtype:Research Article
Publisher:American Chemical Society
Note:Publication type according to Uni Basel Research Database: Journal article
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Last Modified:16 Jan 2023 14:36
Deposited On:16 Jan 2023 14:36

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