中国科学院机构知识库网格系统: Observationally Constrained Modeling of Peroxy Radical During an Ozone Episode in the Pearl River Delta Region, China

Observationally Constrained Modeling of Peroxy Radical During an Ozone Episode in the Pearl River Delta Region, China

文献类型：期刊论文


作者	Wang, Jun 3,4,5; Zhang, Yanli 2,4,5; Zhao, Weixiong1 ; Wu, Zhenfeng 3,4,5; Luo, Shilu 3,4,5; Zhang, Huina 3,4,5; Zhou, Huaishan 3,4,5; Song, Wei 4,5; Zhang, Weijun; Wang, Xinming 2,3,4,5
刊名	JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
出版日期	2023-06-27
卷号	128
ISSN号	2169-897X
DOI	10.1029/2022JD038279
通讯作者	Zhang, Yanli(zhang_yl86@gig.ac.cn) ; Wang, Xinming(wangxm@gig.ac.cn)
英文摘要	Peroxy radicals (RO2* = HO2 + RO2) play key roles in forming secondary air pollutants such as ozone, yet model underprediction of RO2* is a challenging radical closure problem. In this study, RO2* were measured by a dual-channel peroxy radical chemical amplification system during an ozone episode in October 2018 at an urban site in the Pearl River Delta region, China. The box model based on the Master Chemical Mechanism severely underpredicted RO2* levels, particularly at night and under high nitric oxide (NO) conditions. The observed-to-modeled ratio of RO2* increased from similar to 3 under 1 ppbv NO to & SIM;46 under >10 ppbv NO with a missing RO2* source up to 5.8 ppbv hr(-1). Observation data were used to constrain model predictions, and the results reveal that constraining nitrous acid (HONO) or glyoxal/methylglyoxal could not improve predictions, while constraining nitrate radicals (NO3) or other oxygenated volatile organic compounds (OVOCs), particularly phenolic compounds and improvements in their gas-phase mechanisms, could more effectively increase model-simulated RO2* concentrations. When OVOCs, NO3, and HONO were constrained, the simulated RO2* concentrations increased to the greatest extent with an observed-to-modeled RO2* ratio of 1.9 during the day and 1.3 at night, mainly due to the interaction between OVOCs and NO3 radicals. As the underestimated NO3 levels and the unmeasured reactive organic gases, as well as their unknown oxidation mechanisms, are among the major reasons for the underestimation of RO2, upgraded atmospheric chemistry involving more OVOC species and more accurate NO3 would improve model-simulated RO2 concentrations, especially during nighttime. Plain Language Summary Peroxy radicals (RO2* = HO2 + RO2), including hydroperoxy radicals (HO2) and organic peroxy radicals (RO2), are mainly formed by atmospheric oxidative degradation of trace gases, such as formaldehyde, carbon monoxide (CO) and volatile organic compounds (VOCs). They are important intermediates for the tropospheric forming secondary air pollutants, yet model underprediction of RO2* is a challenging radical closure problem. Here, we conducted a field campaign during an ozone episode in October 2018 at an urban site in the Pearl River Delta region and revealed that RO2* concentrations simulated by the AtChem2-MCM were much lower than those observed, particularly at nighttime and under high nitric oxide conditions. We found that using the observations of oxygenated volatile organic compounds (OVOCs) and nitrate radicals to constrain the model could more effectively reduce the gap between the simulated and observed RO2* radicals. Our results highlight that, more attention should be given to OVOCs that have not been measured or whose oxidation mechanisms are not well understood, but can be photolyzed or oxidized to form RO2, such as phenolic compounds, for the in-depth understanding of tropospheric RO2 chemistry.
WOS关键词	VOLATILE ORGANIC-COMPOUNDS ; NITROUS-ACID HONO ; RESPIRATORY ABSORPTION FACTORS ; MISSING OH SOURCE ; RURAL SITE ; TROPOSPHERIC DEGRADATION ; AROMATIC-HYDROCARBONS ; ATMOSPHERIC CHEMISTRY ; CHEMICAL MECHANISM ; CARBONYL-COMPOUNDS
资助项目	Natural Science Foundation of China[42022023] ; National Key Research and Development Program of China[2022YFC3701103] ; Department of Science and Technology of Guangdong Province[2020B1212060053] ; Guangzhou Municipal Science and Technology Bureau[202206010057]
WOS研究方向	Meteorology & Atmospheric Sciences
语种	英语
出版者	AMER GEOPHYSICAL UNION
WOS记录号	WOS:001022730700001
资助机构	Natural Science Foundation of China ; National Key Research and Development Program of China ; Department of Science and Technology of Guangdong Province ; Guangzhou Municipal Science and Technology Bureau
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/132464]
专题	中国科学院合肥物质科学研究院
通讯作者	Zhang, Yanli; Wang, Xinming
作者单位	1.Chinese Acad Sci, Anhui Inst Opt & Fine Mech, Lab Atmospher Phys Chem, Hefei, Peoples R China 2.Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen, Peoples R China 3.Univ Chinese Acad Sci, Beijing, Peoples R China 4.Chinese Acad Sci, Ctr Excellence Deep Earth Sci, Guangzhou, Peoples R China 5.Chinese Acad Sci, Guangzhou Inst Geochem, State Key Lab Organ Geochem, Guangdong Key Lab Environm Protect & Resources Uti, Guangzhou, Peoples R China
推荐引用方式 GB/T 7714	Wang, Jun,Zhang, Yanli,Zhao, Weixiong,et al. Observationally Constrained Modeling of Peroxy Radical During an Ozone Episode in the Pearl River Delta Region, China[J]. JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES,2023,128.
APA	Wang, Jun.,Zhang, Yanli.,Zhao, Weixiong.,Wu, Zhenfeng.,Luo, Shilu.,...&Wang, Xinming.(2023).Observationally Constrained Modeling of Peroxy Radical During an Ozone Episode in the Pearl River Delta Region, China.JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES,128.
MLA	Wang, Jun,et al."Observationally Constrained Modeling of Peroxy Radical During an Ozone Episode in the Pearl River Delta Region, China".JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES 128(2023).

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来源：合肥物质科学研究院

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Observationally Constrained Modeling of Peroxy Radical During an Ozone Episode in the Pearl River Delta Region, China

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