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DOI10.5194/acp-22-3149-2022
Atmospheric measurements at Mt. Tai - Part I: HONO formation and its role in the oxidizing capacity of the upper boundary layer
Xue, Chaoyang; Ye, Can; Kleffmann, Jorg; Zhang, Chenglong; Catoire, Valery; Bao, Fengxia; Mellouki, Abdelwahid; Xue, Likun; Chen, Jianmin; Lu, Keding; Zhao, Yong; Liu, Hengde; Guo, Zhaoxin; Mu, Yujing
发表日期2022
ISSN1680-7316
EISSN1680-7324
起始页码3149
结束页码3167
卷号22期号:5页码:19
英文摘要A comprehensive field campaign, with measurements of HONO and related parameters, was conducted in summer 2018 at the foot (150 m a.s.l.) and the summit (1534 m a.s.l.) of Mt. Tai (Shandong province, China). At the summit station, high HONO mixing ratios were observed (mean +/- 1 sigma: 133 +/- 106 pptv, maximum: 880 pptv), with a diurnal noontime peak (mean +/- 1 sigma: 133 +/- 72 pptv at 12:30 local time). Constraints on the kinetics of aerosol-derived HONO sources (NO2 uptake on the aerosol surface and particulate nitrate photolysis) were performed and discussed, which enables a better understanding of the interaction of HONO and aerosols, especially in the polluted North China Plain. Various evidence of air mass transport from the ground to the summit level was provided. Furthermore, daytime HONO formation from different paths and its role in radical production were quantified and discussed. We found that the homogeneous reaction NO + OH could only explain 8.0 % of the daytime HONO formation, resulting in strong unknown sources (P-un). Campaigned-averaged P-un was about 290 +/- 280 pptv h(-1), with a maximum of about 1800 pptv h(-1). Aerosol-derived HONO formation mechanisms were not the major sources of P-un at the summit station. Their contributions to daytime HONO formation varied from negligible to moderate (similar to NO + OH), depending on the chemical kinetic parameters used. Coupled with sensitivity tests on the kinetic parameters used, the NO2 uptake on the aerosol surface and particulate nitrate photolysis contributed 1.5 %-19 % and 0.6 %-9.6 % of the observed P-un, respectively. Based on synchronous measurements at the foot and the summit station, an amount of field evidence was proposed to support the finding that the remaining majority (70 %-98 %) of P-un was dominated by the rapid vertical transport from the ground to the summit level and heterogeneous formation on the mountain surfaces during transport. HONO photolysis at the summit level initialized daytime photochemistry and still represented an essential OH source in the daytime, with a contribution of about one-quarter of O-3. We provided evidence that ground-derived HONO played a significant role in the oxidizing capacity of the upper boundary layer through the enhanced vertical air mass exchange driven by mountain winds. The follow-up impacts should be considered in regional chemistry transport models.
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:000768211200001
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/273375
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; University of Wuppertal; Chinese Academy of Sciences; Institute of Urban Environment, CAS; Max Planck Society; Centre National de la Recherche Scientifique (CNRS); Shandong University; Fudan University; Peking University
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Xue, Chaoyang,Ye, Can,Kleffmann, Jorg,et al. Atmospheric measurements at Mt. Tai - Part I: HONO formation and its role in the oxidizing capacity of the upper boundary layer[J],2022,22(5):19.
APA Xue, Chaoyang.,Ye, Can.,Kleffmann, Jorg.,Zhang, Chenglong.,Catoire, Valery.,...&Mu, Yujing.(2022).Atmospheric measurements at Mt. Tai - Part I: HONO formation and its role in the oxidizing capacity of the upper boundary layer.ATMOSPHERIC CHEMISTRY AND PHYSICS,22(5),19.
MLA Xue, Chaoyang,et al."Atmospheric measurements at Mt. Tai - Part I: HONO formation and its role in the oxidizing capacity of the upper boundary layer".ATMOSPHERIC CHEMISTRY AND PHYSICS 22.5(2022):19.
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