Preprints
https://doi.org/10.5194/acp-2021-881
https://doi.org/10.5194/acp-2021-881

  27 Oct 2021

27 Oct 2021

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

Oxidation product characterization from ozonolysis of the diterpene ent-kaurene

Yuanyuan Luo1, Olga Garmash1,2, Haiyan Li1,3, Frans Graeffe1, Arnaud P. Praplan4, Anssi Liikanen4, Yanjun Zhang1,5, Melissa Meder1, Otso Peräkylä1, Josep Peñuelas6,7, Ana María Yáñez-Serrano6,7,8, and Mikael Ehn1 Yuanyuan Luo et al.
  • 1Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, 00014, Finland
  • 2Aerosol Physics Laboratory, Physics Unit, Tampere University, Tampere, 33014, Finland
  • 3School of Civil and Environmental Engineering, Harbin Institute of Technology, Shenzhen, 518055, China
  • 4Atmospheric Composition Research, Finnish Meteorological Institute, Helsinki, 00101, Finland
  • 5Univ Lyon, Université Claude Bernard Lyon 1, CNRS, IRCELYON, Villeurbanne, 69626, France
  • 6CREAF, Bellaterra (Cerdanyola del Vallès), Catalonia, E08193, Spain
  • 7CSIC, Global Ecology Unit, CREAF‐CSIC‐UAB, Bellaterra (Cerdanyola del Vallès), Catalonia, E08193, Spain
  • 8IDAEA-CSIC, Barcelona, 08034, Spain

Abstract. Diterpenes (C20H32) are biogenically emitted volatile compounds that only recently have been observed in ambient air. They are expected to be highly reactive, and their oxidation is likely to form condensable vapors. However, until now, no studies have investigated gas-phase diterpene oxidation. In this paper, we explored the ozonolysis of a diterpene, ent-kaurene, in a simulation chamber. Using state-of-the-art mass spectrometry, we characterized diterpene oxidation products for the first time, and we identified several products with varying oxidation levels, including highly oxygenated organic molecules (HOM) monomers and dimers. The most abundant monomers measured using a nitrate chemical ionization mass spectrometer were C19H28O8 and C20H30O5, and dimers were C38H60O6 and C39H62O6. The exact molar yield of HOM from kaurene ozonolysis was hard to quantify due to uncertainties in both the kaurene and HOM concentrations, but our best estimate was a few percent, which is similar to values reported earlier for many monoterpenes. We also monitored the decrease of the gas-phase oxidation products in response to an increased condensation sink in the chamber to deduce their affinity to condense. The oxygen content was a critical parameter affecting the volatility of products, with 4–5 O-atoms needed for the main monomeric species to condense. Finally, we report on the observed fragmentation and clustering patterns of kaurene in a Vocus proton transfer reaction time-of-flight mass spectrometer. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation, but more studies on different diterpenes are needed for a broader view of their role in atmospheric chemistry.

Yuanyuan Luo et al.

Status: open (until 24 Dec 2021)

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Yuanyuan Luo et al.

Yuanyuan Luo et al.

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Short summary
Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
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