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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
AbstractIn 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.
Department大气环境与污染控制实验室 ; 大气环境与污染控制实验室
Document Type期刊论文
Affiliation1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China
2.Univ Orleans, CNES, CNRS, Lab Phys & Chim Environm & Espace LPC2E, F-45071 Orleans 2, France
3.Chinese Acad Sci, Ctr Excellence Reg Atmospher Environm, Inst Urban Environm, Xiamen 361021, Peoples R China
4.Ctr Natl Rech Sci ICARE CNRS, Inst Combust Aerotherm Reactivite & Environm, F-45071 Orleans 2, France
5.Univ Wuppertal, Phys & Theoret Chem, Gaussstr 20, D-42119 Wuppertal, Germany
Recommended Citation
GB/T 7714
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]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2022,22(2):1035-1057.
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),1035-1057.
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):1035-1057.
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