Preprints
https://doi.org/10.5194/acp-2022-309
https://doi.org/10.5194/acp-2022-309
 
13 May 2022
13 May 2022
Status: a revised version of this preprint is currently under review for the journal ACP.

Emission factors and evolution of SO2 measured from biomass burning in wild and agricultural fires

Pamela Rickly1,2, Hongyu Guo1,3, Pedro Campuzano-Jost1,3, Jose L. Jimenez1,3, Glenn M. Wolfe4, Ryan Bennett5, Ilann Bourgeois1,2, John D. Crounse6, Jack E. Dibb7, Joshua P. DiGangi8, Glenn S. Diskin8, Maximilian Dollner9, Emily M. Gargulinski16, Samuel R. Hall10, Hannah S. Halliday11, Thomas F. Hanisco4, Reem A. Hannun4,12, Jin Liao4,13, Richard Moore8, Benjamin A. Nault14, John B. Nowak8, Claire E. Robinson8,15, Thomas Ryerson2,a, Kevin J. Sanchez8, Manuel Schöberl9, Amber J. Soja8,16, Jason M. St. Clair4,12, Kenneth L. Thornhill8, Kirk Ullmann10, Paul O. Wennberg6,17, Bernadett Weinzierl9, Elizabeth B. Wiggins8, Edward L. Winstead8, and Andrew W. Rollins2 Pamela Rickly et al.
  • 1Cooperative Institute for Research in Environmental Science, University of Colorado, Boulder, CO, USA
  • 2Chemical Sciences Laboratory, NOAA, Boulder, CO, USA
  • 3Department of Chemistry, University of Colorado, Boulder, CO, USA
  • 4Atmospheric Chemistry and Dynamics Lab, NASA Goddard Space Flight Center, Greenbelt, MD, USA
  • 5Bay Area Environmental Research Institute, NASA Ames Research Center, Moffett Field, CA
  • 6Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA, USA
  • 7Earth System Research Center, University of New Hampshire, Durham, NH, USA
  • 8NASA Langley Research Center, Hampton, VA, USA
  • 9Faculty of Physics, Aerosol Physics and Environmental Physics, University of Vienna, 1090 Vienna, Austria
  • 10Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, USA
  • 11Environmental Protection Agency, Research Triangle, NC, USA
  • 12Joint Center for Earth Systems Technology, University of Maryland Baltimore County, Baltimore, MD 21250, USA
  • 13Goddard Earth Science Technology and Research (GESTAR) II, University of Maryland Baltimore County, Baltimore, MD, USA
  • 14CACC, Aerodyne Research, Inc.
  • 15Science Systems and Applications, Inc., Hampton, VA, USA
  • 16National Institute of Aerospace, Resident at NASA Langley Research Center, Hampton, VA, USA
  • 17Division of Engineering and Applied Science, California Institute of Technology, Pasadena, CA, USA
  • anow at: Scientific Aviation, Boulder, CO, USA

Abstract. Fires emit sufficient sulfur to affect local and regional air quality and climate. This study analyzes SO2 emission factors and variability in smoke plumes from US wild and agricultural fires, and their relationship to sulfate and hydroxymethanesulfonate (HMS) formation. Observed SO2 emission factors for various fuel types show good agreement with the latest reviews of biomass burning emission factors, producing an emission factor range of 0.47–1.2 g SO2 kg-1 C in the emissions. These emission factors vary with geographic location in a way that suggests that deposition of coal burning emissions and application of sulfur-containing fertilizers likely play a role in the larger observed values, which are primarily associated with agricultural burning. A 0-D box model generally reproduces the observed trends of SO2 and total sulfate (inorganic + organic) in aging wildfire plumes. In many cases, modeled HMS is consistent with the observed organosulfur concentrations. However, a comparison of observed organosulfur and modeled HMS suggests that multiple organosulfur compounds are likely responsible for the observations, but that the chemistry of these compounds yield similar production and loss rates to that of HMS, resulting in good agreement with the modeled results. We provide suggestions for constraining the organosulfur compounds observed during these flights and we show that the chemistry of HMS can allow for organosulfur to act as a S(IV) reservoir under conditions of increased pH (>6) and liquid water content (>10-7 g m-3). This can facilitate long-range transport of sulfur emissions resulting in increased SO2 and eventually sulfate in transported smoke.

Pamela Rickly 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-2022-309 Please check rate constant', Anonymous Referee #1, 19 May 2022
    • AC1: 'Reply on RC1', Pamela Rickly, 19 May 2022
  • RC2: 'Comment on acp-2022-309', Anonymous Referee #2, 19 May 2022
  • RC3: 'Comment on acp-2022-309', Anonymous Referee #1, 06 Jun 2022

Pamela Rickly et al.

Pamela Rickly et al.

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Short summary
Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources, but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
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