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Abstract. A portion of Alaska's Fairbanks North Star Borough was designated as nonattainment for the 2006 24 h fine particulate matter 2.5 µm or less in diameter (PM2.5) National Ambient Air Quality Standards (NAAQS) in 2009. PM2.5 NAAQS exceedances in Fairbanks mainly occur during dark and cold winters, when temperature inversions form and trap high emissions at the surface. Sulfate (SO42-), often the second-largest contributor to PM2.5 mass during these wintertime PM episodes, is underpredicted by atmospheric chemical transport models (CTMs). Most CTMs account for primary SO42- and secondary SO42- formed via gas-phase oxidation of sulfur dioxide (SO2) and in-cloud aqueous oxidation of dissolved S(IV). Dissolution and reaction of SO2 in aqueous aerosols are generally not included in CTMs but can be represented as heterogeneous reactive uptake and may help better represent the high SO42- concentrations observed during Fairbanks winters. In addition, hydroxymethanesulfonate (HMS), a particulate sulfur species sometimes misidentified as SO42-, is known to form during Fairbanks winters. Heterogeneous formation of SO42- and HMS in aerosol liquid water (ALW) was implemented in the Community Multiscale Air Quality (CMAQ) modeling system. CMAQ simulations were performed for wintertime PM episodes in Fairbanks (2008) as well as over the Northern Hemisphere and Contiguous United States (CONUS) for 2015–2016. The added heterogeneous sulfur chemistry reduced model mean sulfate bias by ∼ 0.6 µg m−3 during a cold winter PM episode in Fairbanks, AK. Improvements in model performance are also seen in Beijing during wintertime haze events (reducing model mean sulfate bias by ∼ 2.9 µg S m−3). This additional sulfur chemistry also improves modeled summertime SO42- bias in the southeastern US, with implications for future modeling of biogenic organosulfates.
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Emission factors and evolution of SO 2 measured from biomass burning in wildfires and agricultural fires
Abstract. Fires emit sufficient sulfur to affect local and regional airquality and climate. This study analyzes SO2 emission factors andvariability in smoke plumes from US wildfires and agricultural fires, as well as theirrelationship to sulfate and hydroxymethanesulfonate (HMS) formation.Observed SO2 emission factors for various fuel types show goodagreement 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 suggeststhat deposition of coal burning emissions and application ofsulfur-containing fertilizers likely play a role in the larger observedvalues, which are primarily associated with agricultural burning. A 0-D boxmodel generally reproduces the observed trends of SO2 and total sulfate(inorganic + organic) in aging wildfire plumes. In many cases, modeled HMSis consistent with the observed organosulfur concentrations. However, acomparison of observed organosulfur and modeled HMS suggests that multipleorganosulfur compounds are likely responsible for the observations but thatthe chemistry of these compounds yields similar production and loss rates asthat of HMS, resulting in good agreement with the modeled results. Weprovide suggestions for constraining the organosulfur compounds observedduring these flights, and we show that the chemistry of HMS can alloworganosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content>10−7 g sm−3. This canfacilitate long-range transport of sulfur emissions, resulting in increasedSO2 and eventually sulfate in transported smoke.
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- Award ID(s):
- 1822664
- PAR ID:
- 10386150
- Author(s) / Creator(s):
- ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; more »
- Date Published:
- Journal Name:
- Atmospheric Chemistry and Physics
- Volume:
- 22
- Issue:
- 23
- ISSN:
- 1680-7324
- Page Range / eLocation ID:
- 15603 to 15620
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.5194/acp-22-15603-2022
