Preprints
https://doi.org/10.5194/acp-2021-672
https://doi.org/10.5194/acp-2021-672

  31 Aug 2021

31 Aug 2021

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

Field observational constraints on the controllers in glyoxal (CHOCHO) loss to aerosol

Dongwook Kim1,2,3, Changmin Cho2,a, Seokhan Jeong2,b, Soojin Lee2, Benjamin A. Nault3,c, Pedro Campuzano-Jost3, Douglas A. Day3, Jason C. Schroder3,d, Jose L. Jimenez3, Rainer Volkamer3, Donald R. Blake4, Armin Wisthaler5,6, Alan Fried7, Joshua P. DiGangi8, Glenn S. Diskin8, Sally E. Pusede9, Samuel R. Hall10, Kirk Ullmann10, L. Gregory Huey11, David J. Tanner11, Jack Dibb12, Christoph J. Knote13, and Kyung-Eun Min2 Dongwook Kim et al.
  • 1Department of Physics and Photon Science, Gwangju Institute of Science and Technology, Gwangju, South Korea
  • 2School of Environmental Sciences and Environmental Engineering, Gwangju Institute of Science and Technology, Gwangju, South Korea
  • 3Department of Chemistry and CIRES, University of Colorado Boulder, CO, USA
  • 4Department of Chemistry, University of California, Irvine, CA, USA
  • 5Institute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, Austria
  • 6Department of Chemistry, University of Oslo, Oslo, Norway
  • 7Institute of Arctic and Alpine Research, University of Colorado, Boulder, CO, USA
  • 8NASA Langley Research Center, Hampton, VA, USA
  • 9Department of Environmental Sciences, University of Virginia, Charlottesville, VA, USA
  • 10Atmospheric Chemistry Observations and Modeling, National Center for Atmospheric Research, Boulder, CO, USA
  • 11School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
  • 12Earth Systems Research Center, Institute for the Study of Earth, Oceans, and Space, University of New Hampshire, Durham, NH, USA
  • 13Model-Based Environmental Exposure Science, Faculty of Medicine, University of Augsburg, Germany
  • anow at: Troposphere (IEK-8), Institute of Energy and Climate Research, Forschungszentrum Jülich, 52425 Jülich, Germany
  • bnow at: Environmental Assessment group, Korea Environment Institute, Sejong, Korea
  • cnow at: Center for Aerosol and Cloud Chemistry, Aerodyne Research Inc., Billerica, MA, USA
  • dnow at: Colorado Department of Public Health and Environment, Denver, CO, USA

Abstract. Glyoxal (CHOCHO), the simplest dicarbonyl in the troposphere, is an important precursor for secondary organic aerosol (SOA) and brown carbon (BrC) affecting air-quality and climate. The airborne measurement of CHOCHO concentrations during the KORUS-AQ (KORea-US Air Quality study) campaign in 2016 enables detailed quantification of  loss mechanisms, pertaining to SOA formation in the real atmosphere. The production of this molecule was mainly from oxidation of aromatics (59 %) initiated by hydroxyl radical (OH), of which glyoxal forming mechanisms are relatively well constrained. CHOCHO loss to aerosol was found to be the most important removal path (69 %) and contributed to roughly ~20 % (3.7 μg sm−3 ppmv−1 hr−1, normalized with excess CO) of SOA growth in the first 6 hours in Seoul Metropolitan Area. To our knowledge, we show the first field observation of aerosol surface-area (Asurf)-dependent CHOCHO uptake, which  diverges from the simple surface uptake assumption as Asurf increases in ambient condition. Specifically, under the low (high) aerosol loading, the CHOCHO effective uptake rate coefficient, keff,uptake, linearly increases (levels off) with Asurf, thus, the irreversible surface uptake is a reasonable (unreasonable) approximation for simulating CHOCHO loss to aerosol. Dependency of photochemical impact, as well as aerosol viscosity, are discussed as other possible factors influencing CHOCHO uptake rate. Our inferred Henry's law coefficient of CHOCHO, 7.0 × 108 M atm−1, is ~2 orders of magnitude  higher than those estimated from salting-in effects constrained by inorganic salts only, which urges more understanding on CHOCHO solubility under real atmospheric conditions.

Dongwook Kim et al.

Status: final response (author comments only)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2021-672', Anonymous Referee #1, 01 Oct 2021
  • RC2: 'Comment on acp-2021-672', Anonymous Referee #2, 09 Oct 2021

Dongwook Kim et al.

Dongwook Kim et al.

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Short summary
CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. High CHOCHO concentrations were observed over highly populated cities and industrial areas. Aromatics were the most important precursors of CHOCHO production. Loss path to aerosol was the highest sink contributing to ~20 % of SOA formation. CHOCHO uptake rate can be affected by aerosol viscosity and irradiation. Finally, our work highlights the lacking knowledge to explain the CHOCHO solubility.
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