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DOI10.5194/acp-22-1035-2022
Atmospheric measurements at Mt. Tai - Part II: HONO budget and radical (ROx + NO3) chemistry in the lower boundary layer
Xue, Chaoyang; Ye, Can; Kleffmann, Joerg; Zhang, Wenjin; He, Xiaowei; Liu, Pengfei; Zhang, Chenglong; Zhao, Xiaoxi; Liu, Chengtang; Ma, Zhuobiao; Liu, Junfeng; Wang, Jinhe; Lu, Keding; Catoire, Valery; Mellouki, Abdelwahid; Mu, Yujing
发表日期2022
ISSN1680-7316
EISSN1680-7324
起始页码1035
结束页码1057
卷号22期号:2页码:23
英文摘要In the summer of 2018, a comprehensive field campaign, with measurements on HONO and related parameters, was conducted at the foot (150ma.s.l.) and the summit of Mt. Tai (1534ma.s.l.) in the central North China Plain (NCP). With the implementation of a 0-D box model, the HONO budget with six additional sources and its role in radical chemistry at the foot station were explored. We found that the model default source, NO C OH, could only reproduce 13% of the observed HONO, leading to a strong unknown source strength of up to 3 ppbv h(-1). Among the additional sources, the NO2 uptake on the ground surface dominated (similar to 70 %) nighttime HONO formation, and its photo-enhanced reaction dominated (similar to 80 %) daytime HONO formation. Their contributions were sensitive to the mixing layer height (MLH) used for the parameterizations, highlighting the importance of a reasonable MLH for exploring ground-level HONO formation in 0-D models and the necessity of gradient measurements. A Delta HONO/Delta NOx ratio of 0.7% for direct emissions from vehicle exhaust was inferred, and a new method to quantify its contribution to the observations was proposed and discussed. Aerosol-derived sources, including the NO2 uptake on the aerosol surface and the particulate nitrate photolysis, did not lead to significant HONO formation, with their contributions lower than NO + OH. HONO photolysis in the early morning initialized the daytime photochemistry at the foot station. It was also a substantial radical source throughout the daytime, with contributions higher than O-3 photolysis to OH initiation. Moreover, we found that OH dominated the atmospheric oxidizing capacity in the daytime, while modeled NO3 appeared to be significant at night. Peaks of modeled NO3 time series and average diurnal variation reached 22 and 9 pptv, respectively. NO3-induced reactions contribute 18% of nitrate formation potential (P (HNO3)) and 11% of the isoprene (C5H8) oxidation throughout the whole day. At night, NO3 chemistry led to 51% and 44% of P (HNO3) or the C5H8 oxidation, respectively, implying that NO3 chemistry could significantly affect nighttime secondary organic and inorganic aerosol formation in this high-O-3 region. Considering the severe O-3 pollution in the NCP and the very limited NO3 measurements, we suggest that besides direct measurements of HOx and primary HOx precursors (O-3, HONO, alkenes, etc.), NO3 measurements should be conducted to understand the atmospheric oxidizing capacity and air pollution formation in this and similar regions.
学科领域Environmental Sciences; Meteorology & Atmospheric Sciences
语种英语
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
WOS记录号WOS:000747697500001
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/273898
作者单位Chinese Academy of Sciences; Research Center for Eco-Environmental Sciences (RCEES); Centre National de la Recherche Scientifique (CNRS); Universite de Orleans; Chinese Academy of Sciences; Institute of Urban Environment, CAS; Centre National de la Recherche Scientifique (CNRS); University of Wuppertal; Peking University; Shandong Jianzhu University; Shandong University; Chinese Academy of Sciences; University of Chinese Academy of Sciences, CAS
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Xue, Chaoyang,Ye, Can,Kleffmann, Joerg,et al. Atmospheric measurements at Mt. Tai - Part II: HONO budget and radical (ROx + NO3) chemistry in the lower boundary layer[J],2022,22(2):23.
APA Xue, Chaoyang.,Ye, Can.,Kleffmann, Joerg.,Zhang, Wenjin.,He, Xiaowei.,...&Mu, Yujing.(2022).Atmospheric measurements at Mt. Tai - Part II: HONO budget and radical (ROx + NO3) chemistry in the lower boundary layer.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(2),23.
MLA Xue, Chaoyang,et al."Atmospheric measurements at Mt. Tai - Part II: HONO budget and radical (ROx + NO3) chemistry in the lower boundary layer".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.2(2022):23.
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