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Discussion papers
https://doi.org/10.5194/acp-2018-1004
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1004
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 27 Sep 2018

Research article | 27 Sep 2018

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

Carboxylic acids from limonene oxidation by ozone and OH radicals: Insights into mechanisms derived using a FIGAERO-CIMS

Julia Hammes1, Anna Lutz1, Thomas Mentel1,2, Cameron Faxon1, and Mattias Hallquist1 Julia Hammes et al.
  • 1Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden
  • 2Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany

Abstract. This work presents the results from flow reactor studies on the formation of carboxylic acids from limonene oxidation under various conditions. A High Resolution Time Of Flight acetate Chemical Ionisation Mass Spectrometer (HR – TOF – CIMS) was used in combination with the Filter Inlet for Gases and AEROsols (FIGAERO) to measure the carboxylic acid profile in the gas and particle phases. The results revealed that limonene oxidation produced large amounts of carboxylic acids which are important contributors to secondary organic aerosol (SOA) formation. The highest 10 acids contributed 56–91% to the total gas-phase signal and the dominant gas-phase species in most experiments were C8H12O4, C9H14O4, C7H10O4 and

C10H16O3. The particle-phase composition was generally more complex than the gas-phase composition and the highest 10 acids contributed 47–92% to the total signal. The dominant species in the particle phase were C8H12O5, C9H14O5, C9H12O5 and C10H16O4. The measured concentrations of dimers in the particle phase were very low, indicating that acidic dimers play a minor role in SOA formation via ozone/OH oxidation of limonene. Spearman correlation analysis of the produced carboxylic acid species and experimental parameters were helpful in interpreting the results. Based on the various experimental conditions, the acidic composition for all experiments were modelled using the Master Chemical Mechanisms (MCM). Significant concentrations of 11 acids, from a total of 16 acids, included in MCM were measured with the CIMS. However, the model predictions were, in some cases, inconsistent with the measurement results, especially in the case of the OH dependence. Reaction mechanisms are suggested to fill-in the knowledge gaps. Based on the mechanisms proposed in this work, nearly 75% of the qualitative gas-phase signal of the low concentration (ppb converted), humid, mixed oxidant experiment can be explained.

Julia Hammes et al.
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