Evolution of organic carbon in the laboratory oxidation of biomass-burning emissions
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Published:2023-07-17
Issue:14
Volume:23
Page:7887-7899
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Nihill Kevin J.ORCID, Coggon Matthew M., Lim Christopher Y.ORCID, Koss Abigail R., Yuan BinORCID, Krechmer Jordan E.ORCID, Sekimoto Kanako, Jimenez Jose L.ORCID, de Gouw JoostORCID, Cappa Christopher D.ORCID, Heald Colette L.ORCID, Warneke Carsten, Kroll Jesse H.ORCID
Abstract
Abstract. Biomass burning (BB) is a major source of reactive organic carbon
into the atmosphere. Once in the atmosphere, these organic BB emissions, in
both the gas and particle phases, are subject to atmospheric oxidation,
though the nature and impact of the chemical transformations are not
currently well constrained. Here we describe experiments carried out as part
of the FIREX FireLab campaign, in which smoke from the combustion of fuels
typical of the western United States was sampled into an environmental chamber and
exposed to high concentrations of OH, to simulate the equivalent of up to
2 d of atmospheric oxidation. The evolution of the organic mixture was
monitored using three real-time time-of-flight mass spectrometric
instruments (a proton transfer reaction mass spectrometer, an iodide
chemical ionization mass spectrometer, and an aerosol mass spectrometer),
providing measurements of both individual species and ensemble properties of
the mixture. The combined measurements from these instruments achieve a
reasonable degree of carbon closure (within 15 %–35 %), indicating that most
of the reactive organic carbon is measured by these instruments. Consistent
with our previous studies of the oxidation of individual organic species,
atmospheric oxidation of the complex organic mixture leads to the formation
of species that on average are smaller and more oxidized than those in the
unoxidized emissions. In addition, the comparison of mass spectra from the
different fuels indicates that the oxidative evolution of BB emissions
proceeds largely independent of fuel type, with different fresh smoke
mixtures ultimately converging into a common, aged distribution of gas-phase
compounds. This distribution is characterized by high concentrations of
several small, volatile oxygenates, formed from fragmentation reactions, as
well as a complex pool of many minor oxidized species and secondary organic
aerosol, likely formed via functionalization processes.
Funder
NOAA Research National Aeronautics and Space Administration
Publisher
Copernicus GmbH
Subject
Atmospheric Science
Reference48 articles.
1. Akagi, S. K., Yokelson, R. J., Burling, I. R., Meinardi, S., Simpson, I., Blake, D. R., McMeeking, G. R., Sullivan, A., Lee, T., Kreidenweis, S., Urbanski, S., Reardon, J., Griffith, D. W. T., Johnson, T. J., and Weise, D. R.: Measurements of reactive trace gases and variable O3 formation rates in some South Carolina biomass burning plumes, Atmos. Chem. Phys., 13, 1141–1165, https://doi.org/10.5194/acp-13-1141-2013, 2013. 2. Akherati, A., He, Y., Coggon, M. M., Koss, A. R., Hodshire, A. L., Sekimoto,
K., Warneke, C., De Gouw, J. A., Yee, L., Seinfeld, J. H., Onasch, T. B.,
Herndon, S. C., Knighton, W. B., Cappa, C. D., Kleeman, M. J., Lim, C. Y.,
Kroll, J. H., Pierce, J. R., and Jathar, S. H.: Oxygenated Aromatic
Compounds are Important Precursors of Secondary Organic Aerosol in
Biomass-Burning Emissions, Environ. Sci. Technol., 54, 8568–8579,
https://doi.org/10.1021/acs.est.0c01345, 2020. 3. Andreae, M. O.: Emission of trace gases and aerosols from biomass burning – an updated assessment, Atmos. Chem. Phys., 19, 8523–8546, https://doi.org/10.5194/acp-19-8523-2019, 2019. 4. Andreae, M. O., Browell, E. V., Garstang, M., Gregory, G. L., Harriss, R.
C., Hill, G. F., Jacob, D. J., Pereira, M. C., Sachse, G. W., Setzer, A. W.,
Silva Dias, P. L., Talbot, R. W., Torres, A. L., and Wofsy, S. C.:
Biomass-Burning Emissions and Associated Haze Layers Over Amazonia, J.
Geophys. Res., 93, 1509–1527, 1988. 5. Bahreini, R., Ervens, B., Middlebrook, A. M., Warneke, C., De Gouw, J. A.,
DeCarlo, P. F., Jimenez, J. L., Brock, C. A., Neuman, J. A., Ryerson, T. B.,
Stark, H., Atlas, E., Brioude, J., Fried, A., Holloway, J. S., Peischl, J.,
Richter, D., Walega, J., Weibring, P., Wollny, A. G., and Fehsenfeid, F. C.:
Organic Aerosol Formation in Urban and Industrial Plumes near Houston and
Dallas, Texas, J. Geophys. Res.-Atmos., 114, 1–17,
https://doi.org/10.1029/2008JD011493, 2009.
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