气候变化领域集成服务门户(CCPortal): Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes

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DOI	10.5194/acp-21-13077-2021
	Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes
	Chai J.; Dibb J.E.; Anderson B.E.; Bekker C.; Blum D.E.; Heim E.; Jordan C.E.; Joyce E.E.; Kaspari J.H.; Munro H.; Walters W.W.; Hastings M.G.
发表日期	2021
ISSN	1680-7316
起始页码	13077
结束页码	13098
卷号	21 期号:17
英文摘要	Nitrous acid (HONO) is an important precursor to hydroxyl radical (OH) that determines atmospheric oxidative capacity and thus impacts climate and air quality. Wildfire is not only a major direct source of HONO, it also results in highly polluted conditions that favor the heterogeneous formation of HONO from nitrogen oxides (NOx D NO C NO2) and nitrate on both ground and particle surfaces. However, these processes remain poorly constrained. To quantitatively constrain the HONO budget under various fire and/or smoke conditions, we combine a unique dataset of field concentrations and isotopic ratios (15N = 14N and 18O = 16O) of NOx and HONO with an isotopic box model. Here we report the first isotopic evidence of secondary HONO production in near-ground wildfire plumes (over a sample integration time of hours) and the subsequent quantification of the relative importance of each pathway to total HONO production. Most importantly, our results reveal that nitrate photolysis plays a minor role (<5 %) in HONO formation in daytime aged smoke, while NO2-to-HONO heterogeneous conversion contributes 85 %-95 % to total HONO production, followed by OH C NO (5 %-15 %). At nighttime, heterogeneous reduction of NO2 catalyzed by redox active species (e.g., iron oxide and/or quinone) is essential (= 75 %) for HONO production in addition to surface NO2 hydrolysis. Additionally, the 18O = 16O of HONO is used for the first time to constrain the NO-to-NO2 oxidation branching ratio between ozone and peroxy radicals. Our approach provides a new and critical way to mechanistically constrain atmospheric chemistry and/or air quality models on a diurnal timescale. © 2021 The Author(s).
语种	英语
scopus关键词	air quality; atmospheric chemistry; data set; hydrolysis; hydroxyl radical; isotopic ratio; nitrogen oxides; nitrous acid; ozone; peroxy radical; secondary production; wildfire
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/246611
作者单位	Institute at Brown for Environment and Society, Brown University, Providence, RI, United States; Department of Earth, Environmental and Planetary Sciences, Brown University, Providence, RI, United States; Institute for the Study of Earth, Oceans and Space, University of New Hampshire, Durham, NH, United States; Nasa Langley Research Center, Hampton, VA, United States; Department of Chemistry, Brown University, Providence, RI, United States; National Institute of Aerospace, Hampton, VA, United States; Department of Chemistry, University of New Hampshire, Durham, NH, United States
推荐引用方式 GB/T 7714	Chai J.,Dibb J.E.,Anderson B.E.,et al. Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes[J],2021,21(17).
APA	Chai J..,Dibb J.E..,Anderson B.E..,Bekker C..,Blum D.E..,...&Hastings M.G..(2021).Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(17).
MLA	Chai J.,et al."Isotopic evidence for dominant secondary production of HONO in near-ground wildfire plumes".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.17(2021).