Preprints
https://doi.org/10.5194/acp-2022-438
https://doi.org/10.5194/acp-2022-438
 
07 Jul 2022
07 Jul 2022
Status: this preprint is currently under review for the journal ACP.

An Improved Representation of Fire Non-Methane Organic Gases (NMOGs) in Models: Emissions to Reactivity

Therese S. Carter1, Colette L. Heald1,2, Jesse H. Kroll1, Eric C. Apel3, Donald Blake4, Matthew Coggon5, Achim Edtbauer6, Georgios Gkatzelis5,7,a, Rebecca S. Hornbrook3, Jeff Peischl5,7, Eva Y. Pfannerstill6,b, Felix Piel8,9, Nina G. Reijrink6,10, Akima Ringsdorf6, Carsten Warneke5, Jonathan Williams6, Armin Wisthaler9,11, and Lu Xu12,c,d Therese S. Carter et al.
  • 1Civil and Environmental Engineering Department, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
  • 2Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
  • 3Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80301, USA
  • 4Chemistry Department, University of California Irvine 92697
  • 5NOAA Chemical Sciences Laboratory, Boulder, CO, 80305, USA
  • 6Atmospheric Chemistry Department, Max Planck Institute for Chemistry, 55128, Mainz, Germany
  • 7Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO, USA
  • 8Ionicon Analytik, Innsbruck, Austria
  • 9Department of Chemistry, University of Oslo, Oslo, Norway
  • 10IMT Nord Europe, Institut Mines-Télécom, Univ. Lille, Center for Energy and Environment, F-59000 Lille, France
  • 11Institute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, Austria
  • 12Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
  • anow at: Institute of Energy and Climate Research, IEK-8: Troposphere, Forschungszentrum Jülich GmbH, Jülich, Germany
  • bnow at: Department of Environmental Science, Policy, and Management, University of California, Berkeley, CA 94720, USA
  • cnow at: Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO, USA
  • dnow at: NOAA Chemical Sciences Laboratory, Boulder, CO, 80305, USA

Abstract. Fires emit a substantial amount of non-methane organic gases (NMOGs); the atmospheric oxidation of which can contribute to ozone and secondary particulate matter formation. However, the abundance and reactivity of these fire NMOGs are uncertain and historically not well constrained. In this work, we expand the representation of fire NMOGs in a global chemical transport model, GEOS-Chem. We update emission factors to Andreae (2019) and the chemical mechanism to include recent aromatic and ethene/ethyne model improvements (Bates et al., 2021; Kwon et al., 2021). We expand the representation of NMOGs by adding lumped furans to the model (including their fire emission and oxidation chemistry) and by adding fire emissions of nine species already included in the model, prioritized for their reactivity using data from the FIREX laboratory studies. Based on quantified emissions factors, we estimate that our improved representation captures 72 % of emitted, identified NMOG carbon mass and 49 % of OH reactivity from savanna and temperate forest fires, a substantial increase from the standard model (49 % of mass, 28 % of OH reactivity). We evaluate fire NMOGs in our model with observations from the Amazon Tall Tower Observatory (ATTO), FIREX-AQ and DC3 in the US, and ARCTAS in boreal Canada. We show that NMOGs, including furan, are well simulated in the eastern US with some underestimates in the western US and that adding fire emissions improves our ability to simulate ethene in boreal Canada. We estimate that fires provide 15 % of annual mean simulated surface OH reactivity globally, and exceeding 75 % over fire source regions. Over continental regions about half of this simulated fire reactivity comes from NMOG species. We find that furans and ethene are important globally for reactivity, while phenol is more important at a local level in the boreal regions. This is the first global estimate of the impact of fire on atmospheric reactivity.

Therese S. Carter et al.

Status: open (until 18 Aug 2022)

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on acp-2022-438', Anonymous Referee #1, 29 Jul 2022 reply
  • RC2: 'Comment on acp-2022-438', Anonymous Referee #2, 02 Aug 2022 reply

Therese S. Carter et al.

Therese S. Carter et al.

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Short summary
Fires emit many gases, which can contributed to smog and air pollution. However, the amount and properties of these chemicals is not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
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