Nighttime and daytime dark oxidation chemistry in wildfire plumes: an observation and model analysis of FIREX-AQ aircraft data
Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of e...
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| Veröffentlicht in: | Atmospheric chemistry and physics Jg. 21; H. 21; S. 16293 - 16317 |
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| Format: | Journal Article |
| Sprache: | Englisch |
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Katlenburg-Lindau
Copernicus GmbH
08.11.2021
Copernicus Publications |
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| ISSN: | 1680-7324, 1680-7316, 1680-7324 |
| Online-Zugang: | Volltext |
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| Abstract | Wildfires are increasing in size across the western US, leading to
increases in human smoke exposure and associated negative health impacts.
The impact of biomass burning (BB) smoke, including wildfires, on regional
air quality depends on emissions, transport, and chemistry, including
oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl
radical (OH), nitrate radical (NO3), and ozone (O3). During the
daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by
O3 and OH. In contrast, at night or in optically dense plumes, BBVOCs
are oxidized mainly by O3 and NO3. This work focuses on the
transition between daytime and nighttime oxidation, which has significant
implications for the formation of secondary pollutants and loss of nitrogen
oxides (NOx=NO+NO2) and has been understudied. We present
wildfire plume observations made during FIREX-AQ (Fire Influence on Regional
to Global Environments and Air Quality), a field campaign involving multiple
aircraft, ground, satellite, and mobile platforms that took place in the
United States in the summer of 2019 to study both wildfire and agricultural
burning emissions and atmospheric chemistry. We use observations from two
research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed
chemical box model, including updated phenolic mechanisms, to analyze smoke
sampled during midday, sunset, and nighttime. Aircraft observations suggest
a range of NO3 production rates (0.1–1.5 ppbv h−1) in plumes
transported during both midday and after dark. Modeled initial instantaneous
reactivity toward BBVOCs for NO3, OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10–104
times greater than typical values in forested or urban environments, and
reactions with BBVOCs account for >97 % of NO3 loss in
sunlit plumes (jNO2 up to 4×10-3s-1), while
conventional photochemical NO3 loss through reaction with NO and
photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH
and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split between
NO3, O3, and OH (26 %–52 %, 22 %–43 %, 16 %–33 %,
respectively). Nitrate radical oxidation accounts for 26 %–52 % of
phenolic chemical loss in sunset plumes and in an optically thick plume.
Nitrocatechol yields varied between 33 % and 45 %, and NO3
chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol
formation and controls nitrophenolic formation overall. As a result,
overnight nitrophenolic formation pathways account for 56 %±2 % of
NOx loss by sunrise the following day. In all but one overnight plume
we modeled, there was remaining NOx (13 %–57 %) and BBVOCs
(8 %–72 %) at sunrise. |
|---|---|
| AbstractList | Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical ( NO3 ), and ozone ( O3 ). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by O3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O3 and NO3 . This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides ( NO x= NO + NO 2 <svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="85pt" height="13pt" class="svg-formula" dspmath="mathimg" md5hash="f0add4bbe2151ecfa7cd944e28fa7e9e"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-21-16293-2021-ie00001.svg" width="85pt" height="13pt" src="acp-21-16293-2021-ie00001.png"/></svg:svg> ) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO3 production rates (0.1–1.5 ppbv h−1 ) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO3 , OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10– 104 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for >97 % of NO3 loss in sunlit plumes ( jNO2 up to 4 × 10 - 3 s - 1 <svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="59pt" height="14pt" class="svg-formula" dspmath="mathimg" md5hash="75fd83c3fc1e7202c7ef5bff89e9ecd3"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-21-16293-2021-ie00002.svg" width="59pt" height="14pt" src="acp-21-16293-2021-ie00002.png"/></svg:svg> ), while conventional photochemical NO3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split between NO3 , O3 , and OH (26 %–52 %, 22 %–43 %, 16 %–33 %, respectively). Nitrate radical oxidation accounts for 26 %–52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO3 chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56 %±2 % of NOx loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NOx (13 %–57 %) and BBVOCs (8 %–72 %) at sunrise. Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical (NO3), and ozone (O3). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by O3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O3 and NO3. This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides (NOx=NO+NO2) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO3 production rates (0.1–1.5 ppbv h−1) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO3, OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10–104 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for >97 % of NO3 loss in sunlit plumes (jNO2 up to 4×10-3s-1), while conventional photochemical NO3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split between NO3, O3, and OH (26 %–52 %, 22 %–43 %, 16 %–33 %, respectively). Nitrate radical oxidation accounts for 26 %–52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO3 chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56 %±2 % of NOx loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NOx (13 %–57 %) and BBVOCs (8 %–72 %) at sunrise. Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical (NO3), and ozone (O3). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly byO3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O3 and NO3. This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides (NOx=NO+NO2) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO3 production rates (0.1–1.5 ppbvh-1) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO3, OH, and O3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO3 reactivity is 10–104 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for >97 % of NO3 loss in sunlit plumes (jNO2 up to 4×10-3s-1), while conventional photochemical NO3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O3 (11 %–43 %, 54 %–88 % for alkenes; 18 %–55 %, 39 %–76 %, for furans, respectively), but phenolic oxidation is split betweenNO3, O3, and OH (26 %–52 %, 22 %–43 %, 16 %–33 %, respectively). Nitrate radical oxidation accounts for 26 %–52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO3 chemistry in BB plumes emitted late in the day is responsible for 72 %–92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56%±2% ofNOx loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NOx (13 %–57 %) and BBVOCs (8 %–72 %) at sunrise. Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of biomass burning (BB) smoke, including wildfires, on regional air quality depends on emissions, transport, and chemistry, including oxidation of emitted BB volatile organic compounds (BBVOCs) by the hydroxyl radical (OH), nitrate radical (NO.sub.3 ), and ozone (O.sub.3). During the daytime, when light penetrates the plumes, BBVOCs are oxidized mainly by O.sub.3 and OH. In contrast, at night or in optically dense plumes, BBVOCs are oxidized mainly by O.sub.3 and NO.sub.3 . This work focuses on the transition between daytime and nighttime oxidation, which has significant implications for the formation of secondary pollutants and loss of nitrogen oxides (NOx=NO+NO2) and has been understudied. We present wildfire plume observations made during FIREX-AQ (Fire Influence on Regional to Global Environments and Air Quality), a field campaign involving multiple aircraft, ground, satellite, and mobile platforms that took place in the United States in the summer of 2019 to study both wildfire and agricultural burning emissions and atmospheric chemistry. We use observations from two research aircraft, the NASA DC-8 and the NOAA Twin Otter, with a detailed chemical box model, including updated phenolic mechanisms, to analyze smoke sampled during midday, sunset, and nighttime. Aircraft observations suggest a range of NO.sub.3 production rates (0.1-1.5 ppbv h.sup.-1) in plumes transported during both midday and after dark. Modeled initial instantaneous reactivity toward BBVOCs for NO.sub.3, OH, and O.sub.3 is 80.1 %, 87.7 %, and 99.6 %, respectively. Initial NO.sub.3 reactivity is 10-10.sup.4 times greater than typical values in forested or urban environments, and reactions with BBVOCs account for 97 % of NO.sub.3 loss in sunlit plumes (jNO.sub.2 up to 4x10-3s-1), while conventional photochemical NO.sub.3 loss through reaction with NO and photolysis are minor pathways. Alkenes and furans are mostly oxidized by OH and O.sub.3 (11 %-43 %, 54 %-88 % for alkenes; 18 %-55 %, 39 %-76 %, for furans, respectively), but phenolic oxidation is split between NO.sub.3, O.sub.3, and OH (26 %-52 %, 22 %-43 %, 16 %-33 %, respectively). Nitrate radical oxidation accounts for 26 %-52 % of phenolic chemical loss in sunset plumes and in an optically thick plume. Nitrocatechol yields varied between 33 % and 45 %, and NO.sub.3 chemistry in BB plumes emitted late in the day is responsible for 72 %-92 % (84 % in an optically thick midday plume) of nitrocatechol formation and controls nitrophenolic formation overall. As a result, overnight nitrophenolic formation pathways account for 56 %±2 % of NO.sub.x loss by sunrise the following day. In all but one overnight plume we modeled, there was remaining NO.sub.x (13 %-57 %) and BBVOCs (8 %-72 %) at sunrise. |
| Audience | Academic |
| Author | Lee, Young Ro Gkatzelis, Georgios I. Rickly, Pamela S. Decker, Zachary C. J. Palm, Brett B. Warneke, Carsten Wiggins, Elizabeth Rollins, Andrew W. Winstead, Edward Neuman, J. Andrew Diskin, Glenn S. Womack, Caroline Moore, Richard Hall, Samuel R. Van Rooy, Paul Middlebrook, Ann M. Ullmann, Kirk Robinson, Michael A. Barsanti, Kelley C. Thornton, Joel A. Wisthaler, Armin DiGangi, Joshua P. Thornhill, Lee Schwantes, Rebecca H. Sekimoto, Kanako Ryerson, Thomas B. Halliday, Hannah Bourgeois, Ilann Lindaas, Jakob Montzka, Denise D. Piel, Felix Weinheimer, Andrew J. Fredrickson, Carley D. Tyndall, Geoffrey S. Washenfelder, Rebecca A. Nowak, John B. Veres, Patrick R. Franchin, Alessandro Brown, Steven S. Peischl, Jeff Flocke, Frank M. Holmes, Christopher D. Coggon, Matthew M. Huey, L. Gregory |
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| Snippet | Wildfires are increasing in size across the western US, leading to
increases in human smoke exposure and associated negative health impacts.
The impact of... Wildfires are increasing in size across the western US, leading to increases in human smoke exposure and associated negative health impacts. The impact of... |
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| SubjectTerms | Aerosols Air quality Aircraft Aircraft observations Alkenes Atmospheric chemistry Biomass Biomass burning Burning Chemistry Climate change Daytime Emissions Fire plumes Flying-machines Furans Hydroxyl radicals Investigations Mobile platforms Modelling Night Night-time Nighttime Nitrates Nitrogen compounds Nitrogen dioxide Nitrogen oxide Nitrogen oxides Organic compounds Oxidation Oxidation-reduction reaction Ozone Pesticides Phenolic compounds Phenols Photochemical reactions Photochemicals Photochemistry Photolysis Plumes Pollutants Research aircraft Smoke Sunrise Sunset Urban environments VOCs Volatile organic compounds Wildfires Work platforms |
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| Title | Nighttime and daytime dark oxidation chemistry in wildfire plumes: an observation and model analysis of FIREX-AQ aircraft data |
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