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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 04 Jun 2019

Research article | 04 Jun 2019

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Investigation of the α-pinene photooxidation by OH in the atmospheric simulation chamber SAPHIR

Michael Rolletter1, Martin Kaminski1,a, Ismail-Hakki Acir1,b, Birger Bohn1, Hans-Peter Dorn1, Xin Li1,c, Anna Lutz2, Sascha Nehr1,d, Franz Rohrer1, Ralf Tillmann1, Robert Wegener1, Andreas Hofzumahaus1, Astrid Kiendler-Scharr1, Andreas Wahner1, and Hendrik Fuchs1 Michael Rolletter et al.
  • 1Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
  • 2Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden
  • anow at: Federal Office of Consumer Protection and Food Safety, Department 5: Method Standardisation, Reference Laboratories, Resistance to Antibiotics, Berlin, Germany
  • bnow at: Institute of Nutrition and Food Sciences, Food Chemistry, University of Bonn, Bonn, Germany
  • cnow at: State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China
  • dnow at: INBUREX Consulting GmbH, Process Safety, Hamm, Germany

Abstract. The photooxidation of the most abundant monoterpene α-pinene, by the hydroxyl radical (OH) was investigated at atmospheric concentrations in the atmospheric simulation chamber SAPHIR. Concentrations of nitric oxide (NO) were below 120 pptv. Yields of organic oxidation products are determined from measured time series giving values of 0.11 ± 0.05, 0.19 ± 0.06, and 0.05 ± 0.03 for formaldehyde, acetone, and pinonaldehyde, respectively. The pinonaldehyde yield is at the low side of yields measured in previous laboratory studies, ranging from 0.06 to 0.87. These studies were mostly performed at reactant concentrations much higher than observed in the atmosphere. Time series of measured radical and trace gas concentrations are compared to results from model calculations applying the Master Chemical Mechanism (MCM) 3.3.1. The model predicts pinonaldehyde mixing ratios that are at least a factor of 4 higher than measured values. At the same time, modelled hydroxyl and hydroperoxy (HO2) radical concentrations are approximately 25 % lower than measured values. Vereecken et al. (2007) suggested a shift of the initial organic peroxy radical (RO2) distribution towards RO2 species that do not yield pinonaldehyde, but produce other organic products. Implementing these modifications reduces the model-measurement gap of pinonaldehyde by 20 % and also improves the agreement in modelled and measured radical concentrations by 10 %. However, the chemical oxidation mechanism needs further adjustment to explain observed radical and pinonaldehyde concentrations. This could be achieved by adjusting the initial RO2 distribution, but could also be done by implementing alternative reaction channels of RO2 species that currently lead to the formation of pinonaldehyde in the model.

Michael Rolletter et al.
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Michael Rolletter et al.
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Short summary
Here we present a study of the photooxidation of α-pinene, the most abundant monoterpene, by hydroxyl radicals (OH) conducted in the simulation chamber SAPHIR. We determine yields of the main degradation products acetone, formaldehyde, and pinonaldehyde and investigate the HOx (OH + HO2) radical budget. Measurements were used to test current atmospheric models and a theory base proposed mechanism.
Here we present a study of the photooxidation of α-pinene, the most abundant monoterpene, by...