Rickly, Pamela S. and Guo, Hongyu and Campuzano-Jost, Pedro and Jimenez, Jose L. and Wolfe, Glenn M. and Bennett, Ryan and Bourgeois, Ilann and Crounse, John D. and Dibb, Jack E. and DiGangi, Joshua P. and Diskin, Glenn S. and Dollner, Maximilian and Gargulinski, Emily M. and Hall, Samuel R. and Halliday, Hannah S. and Hanisco, Thomas F. and Hannun, Reem A. and Liao, Jin and Moore, Richard and Nault, Benjamin A. and Nowak, John B. and Peischl, Jeff and Robinson, Claire E. and Ryerson, Thomas and Sanchez, Kevin J. and Schöberl, Manuel and Soja, Amber J. and St. Clair, Jason M. and Thornhill, Kenneth L. and Ullmann, Kirk and Wennberg, Paul O. and Weinzierl, Bernadett and Wiggins, Elizabeth B. and Winstead, Edward L. and Rollins, Andrew W. (2022) Emission factors and evolution of SO₂ measured from biomass burning in wildfires and agricultural fires. Atmospheric Chemistry and Physics, 22 (23). pp. 15603-15620. ISSN 1680-7324. doi:10.5194/acp-22-15603-2022. https://resolver.caltech.edu/CaltechAUTHORS:20230123-451320900.31
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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 wildfires and agricultural fires, as well as 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. 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 yields similar production and loss rates as 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 organosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content >10⁻⁷ g sm⁻³. This can facilitate long-range transport of sulfur emissions, resulting in increased SO₂ and eventually sulfate in transported smoke.
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Alternate Title: | Emission factors and evolution of SO2 measured from biomass burning in wildfires and agricultural fires | ||||||||||||||||
Additional Information: | Pamela S. Rickly and Andrew W. Rollins acknowledge support from NASA's Upper Atmosphere Composition Observations program. Maximilian Dollner, Manuel Schöberl, and Bernadett Weinzierl have received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation framework program under grant agreement no. 640458 (A-LIFE) and from the University of Vienna. Hongyu Guo, Pedro Campuzano-Jost, and Jose L. Jimenez were supported by NASA 80NSSC18K0630 and 80NSSC21K1451 and NSF AGS-1822664. Glenn M. Wolfe, Thomas F. Hanisco, Reem A. Hannun, Jason M. St. Clair, and Jin Liao acknowledge support from the NASA Tropospheric Composition program and the NOAA AC4 program (NA17OAR4310004). Samuel R. Hall and Kirk Ullmann are funded under NASA grant 80NSSC18K0638. The National Center for Atmospheric Research is sponsored by the National Science Foundation. We would like to thank the NASA DC-8 crew and management team for support during FIREX-AQ integration and flights. Data from FIREX-AQ are available at https://www-air.larc.nasa.gov/cgi-bin/ArcView/firexaq (last access: 1 October 2021). This research has been supported by the National Aeronautics and Space Administration (grant no. 20-UACO20-0021). | ||||||||||||||||
Group: | Division of Geological and Planetary Sciences | ||||||||||||||||
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Issue or Number: | 23 | ||||||||||||||||
DOI: | 10.5194/acp-22-15603-2022 | ||||||||||||||||
Record Number: | CaltechAUTHORS:20230123-451320900.31 | ||||||||||||||||
Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20230123-451320900.31 | ||||||||||||||||
Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||
ID Code: | 118898 | ||||||||||||||||
Collection: | CaltechAUTHORS | ||||||||||||||||
Deposited By: | Research Services Depository | ||||||||||||||||
Deposited On: | 01 Feb 2023 18:16 | ||||||||||||||||
Last Modified: | 01 Feb 2023 18:16 |
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