Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides

doi:10.5194/acp-19-4075-2019

IEECAS OpenIR > 粉尘与环境研究室

	Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides
	Chen, Long 1,2,3; Huang, Yu 1,2,3; Xue, Yonggang 1,2,3; Shen, Zhenxing 4; Cao, Junji 1,2,3; Wang, Wenliang 5
通讯作者	Huang, Yu(huangyu@ieecas.cn) ; Cao, Junji(cao@loess.llqg.ac.cn)
	2019-04-02
发表期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN	1680-7316
卷号	19 期号:6 页码:4075-4091
摘要	Although secondary organic aerosol (SOA) is a major component of PM2.5 and organic aerosol (OA) particles and therefore profoundly influences air quality, climate forcing, and human health, the mechanism of SOA formation via Criegee chemistry is poorly understood. Herein, we perform high-level theoretical calculations to study the gasphase reaction mechanism and kinetics of four Criegee intermediate (CI) reactions with four hydroxyalkyl hydroperoxides (HHPs) for the first time. The calculated results show that the consecutive reactions of CIs with HHPs are both thermochemically and kinetically favored, and the oligomers contain CIs as chain units. The addition of an -OOH group in HHPs to the central carbon atom of CIs is identified as the most energetically favorable channel, with a barrier height strongly dependent on both CI substituent number (one or two) and position (syn- or anti-). In particular, the introduction of a methyl group into the anti-position significantly increases the rate coefficient, and a dramatic decrease is observed when the methyl group is introduced into the synposition. These findings are expected to broaden the reactivity profile and deepen our understanding of atmospheric SOA formation processes.
DOI	10.5194/acp-19-4075-2019
关键词[WOS]	SECONDARY ORGANIC AEROSOL ; GAS-PHASE OZONOLYSIS ; CONFORMER-DEPENDENT REACTIVITY ; DENSITY FUNCTIONALS ; UNIMOLECULAR DECAY ; ALKENE OZONOLYSIS ; CARBONYL OXIDES ; SULFUR-DIOXIDE ; WATER CLUSTERS ; OH RADICALS
收录类别	SCI ; SCI
语种	英语
资助项目	National Key Research and Development Program of China[2016YFA0203000] ; National Natural Science Foundation of China[41805107] ; National Natural Science Foundation of China[41573138] ; National Natural Science Foundation of China[21473108] ; Key Project of International Cooperation 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[SKL-LQG1627] ; Shaanxi Province Postdoctoral Science Foundation[2017BSHEDZZ62] ; Hundred Talents Program of the Chinese Academy of Sciences
WOS研究方向	Meteorology & Atmospheric Sciences
项目资助者	National Key Research and Development Program of China ; National Natural Science Foundation of China ; Key Project of International Cooperation 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 ; Hundred Talents Program of the Chinese Academy of Sciences
WOS类目	Meteorology & Atmospheric Sciences
WOS记录号	WOS:000463091600002
出版者	COPERNICUS GESELLSCHAFT MBH
引用统计	被引频次：22[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/361006/14224
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	Huang, Yu; Cao, Junji
作者单位	1.Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, Xian 710061, Shaanxi, Peoples R China 2.Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Xian 710061, Shaanxi, Peoples R China 3.CAS Ctr Excellence Quaternary Sci & Global Change, Xian 710061, Shaanxi, Peoples R China 4.Xi An Jiao Tong Univ, Dept Environm Sci & Engn, Xian 710049, Shaanxi, Peoples R China 5.Shaanxi Normal Univ, Sch Chem & Chem Engn, Key Lab Macromol Sci Shaanxi Prov, Xian 710119, Shaanxi, Peoples R China
推荐引用方式 GB/T 7714	Chen, Long,Huang, Yu,Xue, Yonggang,et al. Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2019,19(6):4075-4091.
APA	Chen, Long,Huang, Yu,Xue, Yonggang,Shen, Zhenxing,Cao, Junji,&Wang, Wenliang.(2019).Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides.ATMOSPHERIC CHEMISTRY AND PHYSICS,19(6),4075-4091.
MLA	Chen, Long,et al."Mechanistic and kinetics investigations of oligomer formation from Criegee intermediate reactions with hydroxyalkyl hydroperoxides".ATMOSPHERIC CHEMISTRY AND PHYSICS 19.6(2019):4075-4091.