气候变化领域集成服务门户(CCPortal): Global inorganic nitrate production mechanisms: Comparison of a global model with nitrate isotope observations

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DOI	10.5194/acp-20-3859-2020
	Global inorganic nitrate production mechanisms: Comparison of a global model with nitrate isotope observations
	Alexander B.; Sherwen T.; D Holmes C.; A Fisher J.; Chen Q.; J Evans M.; Kasibhatla P.
发表日期	2020
ISSN	1680-7316
起始页码	3859
结束页码	3877
卷号	20 期号:6
英文摘要	The formation of inorganic nitrate is the main sink for nitrogen oxides (NOx DNOCNO2). Due to the importance of NOx for the formation of tropospheric oxidants such as the hydroxyl radical (OH) and ozone, understanding the mechanisms and rates of nitrate formation is paramount for our ability to predict the atmospheric lifetimes of most reduced trace gases in the atmosphere. The oxygen isotopic composition of nitrate (117O(nitrate)) is determined by the relative importance of NOx sinks and thus can provide an observational constraint for NOx chemistry. Until recently, the ability to utilize 117O(nitrate) observations for this purpose was hindered by our lack of knowledge about the oxygen isotopic composition of ozone (117O.O3/). Recent and spatially widespread observations of 117O.O3/ motivate an updated comparison of modeled and observed 117O(nitrate) and a reassessment of modeled nitrate formation pathways. Model updates based on recent laboratory studies of heterogeneous reactions render dinitrogen pentoxide (N2O5) hydrolysis as important as NO2 COH (both 41 %) for global inorganic nitrate production near the surface (below 1 km altitude). All other nitrate production mechanisms individually represent less than 6% of global nitrate production near the surface but can be dominant locally. Updated reaction rates for aerosol uptake of NO2 result in significant reduction of nitrate and nitrous acid (HONO) formed through this pathway in the model and render NO2 hydrolysis a negligible pathway for nitrate formation globally. Although photolysis of aerosol nitrate may have implications for NOx , HONO, and oxidant abundances, it does not significantly impact the relative importance of nitrate formation pathways. Modeled 117O(nitrate) (28:64:5 ) compares well with the average of a global compilation of observations (27:65:0 ) when assuming 117O.O3/D26 , giving confidence in the model's representation of the relative importance of ozone versus HOx (DOHCHO2 CRO2) in NOx cycling and nitrate formation on the global scale. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
语种	英语
scopus关键词	atmospheric chemistry; hydrolysis; inorganic nitrogen; isotopic composition; nitrate; oxygen isotope; ozone; troposphere
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/247879
作者单位	Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, United States; Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, YO10 5DD, United Kingdom; National Center for Atmospheric Science, University of York, York, YO10 5DD, United Kingdom; Department of Earth Ocean and Atmospheric Science, Florida State University, Tallahassee, FL 32306, United States; Centre for Atmospheric Chemistry, University of Wollongong, Wollongong, NSW 2522, Australia; Nicholas School of the Environment, Duke University, Durham, Durham, NC 27708, United States; Department of Chemistry, University of Michigan, Ann Arbor, MI 48109, United States
推荐引用方式 GB/T 7714	Alexander B.,Sherwen T.,D Holmes C.,et al. Global inorganic nitrate production mechanisms: Comparison of a global model with nitrate isotope observations[J],2020,20(6).
APA	Alexander B..,Sherwen T..,D Holmes C..,A Fisher J..,Chen Q..,...&Kasibhatla P..(2020).Global inorganic nitrate production mechanisms: Comparison of a global model with nitrate isotope observations.ATMOSPHERIC CHEMISTRY AND PHYSICS,20(6).
MLA	Alexander B.,et al."Global inorganic nitrate production mechanisms: Comparison of a global model with nitrate isotope observations".ATMOSPHERIC CHEMISTRY AND PHYSICS 20.6(2020).