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DOI10.5194/acp-21-255-2021
Atmospheric evolution of emissions from a boreal forest fire: The formation of highly functionalized oxygen-; nitrogen-; and sulfur-containing organic compounds
Ditto J.C.; He M.; Hass-Mitchell T.N.; Moussa S.G.; Hayden K.; Li S.-M.; Liggio J.; Leithead A.; Lee P.; Wheeler M.J.; Wentzell J.J.B.; Gentner D.R.
发表日期2021
ISSN1680-7316
起始页码255
结束页码267
卷号21期号:1
英文摘要Forest fires are major contributors of reactive gas-and particle-phase organic compounds to the atmosphere. We used offline high-resolution tandem mass spectrometry to perform a molecular-level speciation of gas-and particle-phase compounds sampled via aircraft from an evolving boreal forest fire smoke plume in Saskatchewan, Canada. We observed diverse multifunctional compounds containing oxygen, nitrogen, and sulfur (CHONS), whose structures, formation, and impacts are understudied. The dilution-corrected absolute ion abundance of particle-phase CHONS compounds increased with plume age by a factor of 6.4 over the first 4 h of downwind transport, and their relative contribution to the observed functionalized organic aerosol (OA) mixture increased from 19 % to 40 %. The dilution-corrected absolute ion abundance of particle-phase compounds with sulfide functional groups increased by a factor of 13 with plume age, and their relative contribution to observed OA increased from 4 % to 40 %. Sulfides were present in up to 75 % of CHONS compounds and the increases in sulfides were accompanied by increases in ring-bound nitrogen; both increased together with CHONS prevalence. A complex mixture of intermediate-and semi-volatile gas-phase organic sulfur species was observed in emissions from the fire and depleted downwind, representing potential precursors to particle-phase CHONS compounds. These results demonstrate CHONS formation from nitrogen-and oxygen-containing biomass burning emissions in the presence of reduced sulfur species. In addition, they highlight chemical pathways that may also be relevant in situations with elevated emissions of nitrogen-and sulfur-containing organic compounds from residential biomass burning and fossil fuel use (e.g., coal), respectively. © Author(s) 2021. This work is distributed under the Creative Commons Attribution 4.0 License.
英文关键词atmospheric chemistry; biomass burning; boreal forest; dilution; forest fire; nitrogen; organic compound; oxygen; sulfur; Canada; Saskatchewan
语种英语
来源期刊Atmospheric Chemistry and Physics
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/168843
作者单位Department of Chemical and Environmental Engineering, Yale University, New Haven, CT 06511, United States; Air Quality Research Division, Environment and Climate Change Canada, Toronto, ON M3H 5T4, Canada; Solutions for Energy Air, Climate and Health (SEARCH), School of the Environment, Yale University, New Haven, CT 06511, United States
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Ditto J.C.,He M.,Hass-Mitchell T.N.,et al. Atmospheric evolution of emissions from a boreal forest fire: The formation of highly functionalized oxygen-; nitrogen-; and sulfur-containing organic compounds[J],2021,21(1).
APA Ditto J.C..,He M..,Hass-Mitchell T.N..,Moussa S.G..,Hayden K..,...&Gentner D.R..(2021).Atmospheric evolution of emissions from a boreal forest fire: The formation of highly functionalized oxygen-; nitrogen-; and sulfur-containing organic compounds.Atmospheric Chemistry and Physics,21(1).
MLA Ditto J.C.,et al."Atmospheric evolution of emissions from a boreal forest fire: The formation of highly functionalized oxygen-; nitrogen-; and sulfur-containing organic compounds".Atmospheric Chemistry and Physics 21.1(2021).
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