Effect of oligomerization reactions of Criegee intermediate with organic Chock for acid/peroxy radical on secondary organic aerosol formation from isoprene ozonolysis

doi:10.1016/j.atmosenv.2018.06.001

CORC > 地球环境研究所 > 中国科学院地球环境研究所 > 粉尘与环境研究室

	Effect of oligomerization reactions of Criegee intermediate with organic Chock for acid/peroxy radical on secondary organic aerosol formation from isoprene ozonolysis
	Chen, Long 1,3; Huang, Yu 1,3; Xue, Yonggang 1,3; Cao, Junji 1,3; Wang, Werthang 2
刊名	ATMOSPHERIC ENVIRONMENT
	2018-08-01
卷号	187 页码:218-229
关键词	Isoprene ozonolysis Criegee intermediates Oligomerization reactions Reaction mechanisms Rate coefficients
ISSN号	1352-2310
DOI	10.1016/j.atmosenv.2018.06.001
通讯作者	Huang, Yu(huangyu@ieecas.cn) ; Cao, Junji(cao@loess.llqg.ac.cn)
英文摘要	Secondary organic aerosols (SOA) have significant effects on atmospheric chemistry, human health and climate forcing, but their formation mechanisms via Criegee chemistry are still poorly understood. Here we present a comprehensive theoretical investigation on the oligomerization reaction of stabilized Criegee intermediates (SCIs) with organic acid/peroxy radical by using ab initio quantum-chemical methodologies. Our results show that the ozonolysis of isoprene easily leads to a series of C3 and C4 stable CIs due to its larger exothermicity and spontaneity. The formed SCIs have two isomers: syn- and anti-, and anti- is more stable in energy than that of synby about 2-5 kcal mol(-1). The barrier heights of oligomerization reactions are very sensitive to the size and structure of functional groups near the central carbon atom site, indicating they can be tuned by the substitutions. Reaction between SCIs and peroxy radical contributes significantly to the formation of oligomer which is the dominant component of SOA. However, the reaction between SCIs and organic acid plays an important role in aerosol nucleation in some regions where high SCI and low H2O concentrations occur such as in terrestrial equatorial area. Such knowledge should be useful for understanding the mechanism of SOA formation from alkenes ozonolysis and for developing atmospheric chemistry models.
资助项目	National Key Research and Development Program of China[2016YFA0203000] ; National Science Foundation of China[41401567] ; National Science Foundation of China[41573138] ; National Science Foundation of China[21473108] ; Key Project of International Coperation of the Chinese Academy of Sciences[GJHZ1543] ; Research Grants Council of Hong Kong[PolyU 152083/14E] ; Open foundation of State Key Laboratory of Loess and Quaternary Geology[SKLLQG1627] ; Shaanxi Province Postdoctoral Science Foundation[2017BSHEDZZ62]
WOS关键词	GAS-PHASE OZONOLYSIS ; WATER-VAPOR ; ATMOSPHERIC IMPLICATIONS ; CARBONYL OXIDES ; FORMIC-ACID ; AIR/WATER INTERFACE ; SULFURIC-ACID ; METHYL PEROXY ; SELF-REACTION ; OH RADICALS
WOS研究方向	Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
语种	英语
出版者	PERGAMON-ELSEVIER SCIENCE LTD
WOS记录号	WOS:000439672800019
资助机构	National Key Research and Development Program of China ; National Science Foundation of China ; Key Project of International Coperation of the Chinese Academy of Sciences ; Research Grants Council of Hong Kong ; Open foundation of State Key Laboratory of Loess and Quaternary Geology ; Shaanxi Province Postdoctoral Science Foundation
内容类型	期刊论文
源URL	[http://ir.ieecas.cn/handle/361006/13219]
专题	地球环境研究所_粉尘与环境研究室
通讯作者	Huang, Yu; Cao, Junji
作者单位	1.Chinese Acad Sci, Key Lab Aerosol Chem & Phys, Inst Earth Environm, Xian 710061, Shaanxi, Peoples R China 2.Shaanxi Normal Univ, Sch Chem & Chem Engn, Key Lab Macromol Sci Shaanxi Prov, Xian 710119, Shaanxi, Peoples R China 3.Chinese Acad Sci, State Key Lab Loess & Quaternary Geol, Inst Earth Environm, Xian 710061, Shaanxi, Peoples R China
推荐引用方式 GB/T 7714	Chen, Long,Huang, Yu,Xue, Yonggang,et al. Effect of oligomerization reactions of Criegee intermediate with organic Chock for acid/peroxy radical on secondary organic aerosol formation from isoprene ozonolysis[J]. ATMOSPHERIC ENVIRONMENT,2018,187:218-229.
APA	Chen, Long,Huang, Yu,Xue, Yonggang,Cao, Junji,&Wang, Werthang.(2018).Effect of oligomerization reactions of Criegee intermediate with organic Chock for acid/peroxy radical on secondary organic aerosol formation from isoprene ozonolysis.ATMOSPHERIC ENVIRONMENT,187,218-229.
MLA	Chen, Long,et al."Effect of oligomerization reactions of Criegee intermediate with organic Chock for acid/peroxy radical on secondary organic aerosol formation from isoprene ozonolysis".ATMOSPHERIC ENVIRONMENT 187(2018):218-229.