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Atmospheric oxidation of 1-butene initiated by OH radical: Implications for ozone and nitrous acid formations
Chen, Long1,2; Huang, Yu1,2; Xue, Yonggang1,2; Jia, Zhihui3; Wang, Wenliang4
通讯作者Chen, Long(chenlong@ieecas.cn) ; Huang, Yu(huangyu@ieecas.cn)
2020
发表期刊ATMOSPHERIC ENVIRONMENT
ISSN1352-2310
卷号244页码:12
摘要The present study combines (i) field measurements of 1-butene over Xi'an and surrounding areas during a heavy ozone pollution episode with (ii) quantum chemical calculations on the photochemical transformation of 1butene initiated by OH radical. The measurements show that the diurnal variation of both 1-butene and ozone exhibits a negative relationship during the sampling campaign. The concentrations of 1-butene vary from 0.04 to 0.67 ppbv, and the lowest and highest values emerge in the noon time (1 p.m.-3 p.m.) and in the night time (1 a.m.-3 a.m.). The concentrations of O-3 range from 32.36 to 88.82 ppbv, and the high values appear in the noon time. Quantum chemical calculations show that the OH-addition pathways are more energetically preferable than H-abstraction channels, and the rate coefficient exhibits a negative T-dependence in the temperature range of 273-400 K. The autoxidation of peroxy radicals (RO2) formed from the addition of molecular oxygen to OH-addition products S2 and S3 leads to the formation of highly oxygenated molecules (HOMs), C4H9O5, in which the 1,5-H shift reaction is favoured. In the low-NOx regions, RO2 radicals mainly react with HO2 radical leading to hydroperoxide ROOH on both the singlet and triplet PESs, in which the triplet PES is preferable. In the high-NOx regions, RO2 radicals mainly react with NO leading to the formation of RO. + NO2, aldehyde + HONO and organic nitrate, in which the HONO formation appears to be previously unconsidered in the photochemical transformation of alkenes. The branching ratio of RO. + NO2 increases slowly with increasing temperature (from 51.3 to 52.7%), whereas aldehyde + HONO gradually decreases with the temperature rising (from 48.7 to 47.3%). The formation of organic nitrate is negligible over the temperature range of 273-400 K. These findings are expected to deepen our understanding the photochemistry oxidation of alkene under realistic atmospheric conditions.
关键词1-Butene Atmospheric oxidation Reaction mechanism Rate coefficients O-3 HONO
DOI10.1016/j.atmosenv.2020.118010
关键词[WOS]SECONDARY ORGANIC AEROSOL ; LOW-TEMPERATURE KINETICS ; H-ATOM ABSTRACTION ; GAS-PHASE ; MULTIFUNCTIONAL PRODUCTS ; CHEMICAL-REACTIONS ; OLIGOMER FORMATION ; RATE CONSTANTS ; DECOMPOSITION ; VOLATILITY
收录类别SCI ; SCI
语种英语
资助项目National Natural Science Foundation of China[41805107] ; National Natural Science Foundation of China[21473108] ; National Key Research and Development Program of China[2016YFA0203000] ; Key Projects of Chinese Academy of Sciences, China[ZDRW-ZS-2017-6] ; Strategic Priority Research Program of the Chinese Academy of Sciences, China[XDA23010300] ; Strategic Priority Research Program of the Chinese Academy of Sciences, China[XDA23010000] ; Key Project of International Cooperation of the Chinese Academy of Sciences, China[GJHZ1543] ; Research Grants Council of Hong Kong, China[PolyU 152083/14E] ; CAS Light of West China Program[XAB 2019B01] ; General Project of Shaanxi Province[2020JQ-432]
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
项目资助者National Natural Science Foundation of China ; National Key Research and Development Program of China ; Key Projects of Chinese Academy of Sciences, China ; Strategic Priority Research Program of the Chinese Academy of Sciences, China ; Key Project of International Cooperation of the Chinese Academy of Sciences, China ; Research Grants Council of Hong Kong, China ; CAS Light of West China Program ; General Project of Shaanxi Province
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS记录号WOS:000591732600001
出版者PERGAMON-ELSEVIER SCIENCE LTD
引用统计
被引频次:3[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ieecas.cn/handle/361006/15535
专题粉尘与环境研究室
第四纪科学与全球变化卓越创新中心
通讯作者Chen, Long; Huang, Yu
作者单位1.Chinese Acad Sci, Key Lab Aerosol Chem & Phys, State Key Lab Loess & Quaternary Geol SKLLQG, Inst Earth Environm, Xian 710061, Peoples R China
2.Chinese Acad Sci, Ctr Excellence Quaternary Sci & Global Change, Xian 710061, Peoples R China
3.Shaanxi Normal Univ, Sch Mat Sci & Engn, Xian 710119, Shaanxi, Peoples R China
4.Shaanxi Normal Univ, Sch Chem & Chem Engn, Key Lab Macromol Sci Shaanxi Prov, Xian 710119, Shaanxi, Peoples R China
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GB/T 7714
Chen, Long,Huang, Yu,Xue, Yonggang,et al. Atmospheric oxidation of 1-butene initiated by OH radical: Implications for ozone and nitrous acid formations[J]. ATMOSPHERIC ENVIRONMENT,2020,244:12.
APA Chen, Long,Huang, Yu,Xue, Yonggang,Jia, Zhihui,&Wang, Wenliang.(2020).Atmospheric oxidation of 1-butene initiated by OH radical: Implications for ozone and nitrous acid formations.ATMOSPHERIC ENVIRONMENT,244,12.
MLA Chen, Long,et al."Atmospheric oxidation of 1-butene initiated by OH radical: Implications for ozone and nitrous acid formations".ATMOSPHERIC ENVIRONMENT 244(2020):12.
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