气候变化领域集成服务门户(CCPortal): Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain

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DOI	10.1029/2021JD034688
	Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain
	Chan Y.-C.; Evans M.J.; He P.; Holmes C.D.; Jaeglé L.; Kasibhatla P.; Liu X.-Y.; Sherwen T.; Thornton J.A.; Wang X.; Xie Z.; Zhai S.; Alexander B.
发表日期	2021
ISSN	2169897X
卷号	126 期号:9
英文摘要	Studies of wintertime air quality in the North China Plain (NCP) show that particulate-nitrate pollution persists despite rapid reduction in NOx emissions. This intriguing NOx-nitrate relationship may originate from non-linear nitrate-formation chemistry, but it is unclear which feedback mechanisms dominate in NCP. In this study, we re-interpret the wintertime observations of 17O excess of nitrate (∆17O(NO3−)) in Beijing using the GEOS-Chem (GC) chemical transport model to estimate the importance of various nitrate-production pathways and how their contributions change with the intensity of haze events. We also analyze the relationships between other metrics of NOy chemistry and [PM2.5] in observations and model simulations. We find that the model on average has a negative bias of −0.9‰ and −36% for ∆17O(NO3−) and [Ox,major] (≡ [O3] + [NO2] + [p-NO3−]), respectively, while overestimating the nitrogen oxidation ratio ([NO3−]/([NO3−] + [NO2])) by +0.12 in intense haze. The discrepancies become larger in more intense haze. We attribute the model biases to an overestimate of NO2-uptake on aerosols and an underestimate in wintertime O3 concentrations. Our findings highlight a need to address uncertainties related to heterogeneous chemistry of NO2 in air-quality models. The combined assessment of observations and model results suggest that N2O5 uptake in aerosols and clouds is the dominant nitrate-production pathway in wintertime Beijing, but its rate is limited by ozone under high-NOx-high-PM2.5 conditions. Nitrate production rates may continue to increase as long as [O3] increases despite reduction in [NOx], creating a negative feedback that reduces the effectiveness of air pollution mitigation. © 2021. American Geophysical Union. All Rights Reserved.
英文关键词	GEOS-Chem; heterogeneous chemistry; nitrate; NO2 uptake; winter air quality; Δ17O(NO3−)
语种	英语
来源期刊	Journal of Geophysical Research: Atmospheres
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/185254
作者单位	Department of Atmospheric Sciences, University of Washington, Seattle, WA, United States; National Centre for Atmospheric Science, University of York, York, United Kingdom; Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, United Kingdom; School of Environment and Tourism, West Anhui University, Lu'an, China; Department of Earth, Ocean and Atmospheric Science, Florida State University, Tallahassee, FL, United States; Nicholas School of the Environment, Duke University, Durham, NC, United States; School of Earth System Science, Tianjin University, Tianjin, China; School of Energy and Environment, City University of Hong Kong, Hong Kong; Anhui Key Laboratory of Polar Environment and Global Change, Department of Environmental Science and Engineering, University of Science and Technology of China, Hefei, China
推荐引用方式 GB/T 7714	Chan Y.-C.,Evans M.J.,He P.,et al. Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain[J],2021,126(9).
APA	Chan Y.-C..,Evans M.J..,He P..,Holmes C.D..,Jaeglé L..,...&Alexander B..(2021).Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain.Journal of Geophysical Research: Atmospheres,126(9).
MLA	Chan Y.-C.,et al."Heterogeneous Nitrate Production Mechanisms in Intense Haze Events in the North China Plain".Journal of Geophysical Research: Atmospheres 126.9(2021).