气候变化领域集成服务门户(CCPortal): Mechanistic study of the formation of ring-retaining and ring-opening products from the oxidation of aromatic compounds under urban atmospheric conditions

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DOI	10.5194/acp-19-15117-2019
	Mechanistic study of the formation of ring-retaining and ring-opening products from the oxidation of aromatic compounds under urban atmospheric conditions
	Zaytsev A.; Koss A.R.; Breitenlechner M.; Krechmer J.E.; Nihill K.J.; Lim C.Y.; Rowe J.C.; Cox J.L.; Moss J.; Roscioli J.R.; Canagaratna M.R.; Worsnop D.R.; Kroll J.H.; Keutsch F.N.
发表日期	2019
ISSN	16807316
起始页码	15117
结束页码	15129
卷号	19 期号:23
英文摘要	Aromatic hydrocarbons make up a large fraction of anthropogenic volatile organic compounds and contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Four toluene and four 1,2,4-trimethylbenzene (1,2,4-TMB) photooxidation experiments were performed in an environmental chamber under relevant polluted conditions (NOx ~ 10 ppb). An extensive suite of instrumentation including two proton-transferreaction mass spectrometers (PTR-MS) and two chemical ionisation mass spectrometers (NHC 4 CIMS and I- CIMS) allowed for quantification of reactive carbon in multiple generations of hydroxyl radical (OH)-initiated oxidation. Oxidation of both species produces ring-retaining products such as cresols, benzaldehydes, and bicyclic intermediate compounds, as well as ring-scission products such as epoxides and dicarbonyls. We show that the oxidation of bicyclic intermediate products leads to the formation of compounds with high oxygen content (an O V C ratio of up to 1.1). These compounds, previously identified as highly oxygenated molecules (HOMs), are produced by more than one pathway with differing numbers of reaction steps with OH, including both auto-oxidation and phenolic pathways. We report the elemental composition of these compounds formed under relevant urban high-NO conditions. We show that ringretaining products for these two precursors are more diverse and abundant than predicted by current mechanisms. We present the speciated elemental composition of SOA for both precursors and confirm that highly oxygenated products make up a significant fraction of SOA. Ring-scission products are also detected in both the gas and particle phases, and their yields and speciation generally agree with the kinetic model prediction. © 2019 Author(s).
语种	英语
scopus关键词	aerosol; anthropogenic source; aromatic hydrocarbon; atmospheric chemistry; concentration (composition); hydroxyl radical; prediction; volatile organic compound
来源期刊	Atmospheric Chemistry and Physics
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/143976
作者单位	John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, United States; Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, United States; Aerodyne Research Inc., Billerica, MA 01821, United States; Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, United States; Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, United States; TOFWERK USA, Boulder, CO 80301, United States
推荐引用方式 GB/T 7714	Zaytsev A.,Koss A.R.,Breitenlechner M.,et al. Mechanistic study of the formation of ring-retaining and ring-opening products from the oxidation of aromatic compounds under urban atmospheric conditions[J],2019,19(23).
APA	Zaytsev A..,Koss A.R..,Breitenlechner M..,Krechmer J.E..,Nihill K.J..,...&Keutsch F.N..(2019).Mechanistic study of the formation of ring-retaining and ring-opening products from the oxidation of aromatic compounds under urban atmospheric conditions.Atmospheric Chemistry and Physics,19(23).
MLA	Zaytsev A.,et al."Mechanistic study of the formation of ring-retaining and ring-opening products from the oxidation of aromatic compounds under urban atmospheric conditions".Atmospheric Chemistry and Physics 19.23(2019).