气候变化领域集成服务门户(CCPortal): Evaluation of the chemical composition of gas- And particle-phase products of aromatic oxidation

CCPortal

DOI	10.5194/acp-20-9783-2020
	Evaluation of the chemical composition of gas- And particle-phase products of aromatic oxidation
	Mehra A.; Wang Y.; E. Krechmer J.; Lambe A.; Majluf F.; A. Morris M.; Priestley M.; J. Bannan T.; J. Bryant D.; L. Pereira K.; F. Hamilton J.; R. Rickard A.; J. Newland M.; Stark H.; Croteau P.; T. Jayne J.; R. Worsnop D.; R. Canagaratna M.; Wang L.; Coe H.
发表日期	2020
ISSN	1680-7316
起始页码	9783
结束页码	9803
卷号	20 期号:16
英文摘要	Aromatic volatile organic compounds (VOCs) are key anthropogenic pollutants emitted to the atmosphere and are important for both ozone and secondary organic aerosol (SOA) formation in urban areas. Recent studies have indicated that aromatic hydrocarbons may follow previously unknown xidation chemistry pathways, including autoxidation that can lead to the formation of highly oxidised products. In this study we evaluate the gas- and particle-phase ions measured by online mass spectrometry during the hydroxyl radical oxidation of substituted C9-aromatic isomers (1,3,5-trimethylbenzene, 1,2,4-trimethylbenzene, propylbenzene and isopropylbenzene) and a substituted polyaromatic hydrocarbon (1-methylnaphthalene) under low- and medium-NOx conditions. A time-of-flight chemical ionisation mass spectrometer (ToF-CIMS) with iodide anion ionisation was used with a filter inlet for gases and aerosols (FIGAERO) for the detection of products in the particle phase, while a Vocus protontransfer- reaction mass spectrometer (Vocus-PTR-MS) was sed for the detection of products in the gas phase. The signal of product ions observed in the mass spectra were compared or the different precursors and experimental conditions. The majority of mass spectral product signal in both the gas and particle phases comes from ions which are common to all precursors, though signal distributions are distinct for different VOCs. Gas- and particle-phase composition are distinct from one another. Ions corresponding to products contained in the near-explicit gas phase Master Chemical Mechanism (MCM version 3.3.1) are utilised as a benchmark of current scientific understanding, and a comparison of these with observations shows that the MCM is missing a range of highly oxidised products from its mechanism. In the particle phase, the bulk of the product signal from all precursors comes from ring scission ions, a large proportion of which are more oxidised than previously reported and ave undergone further oxidation to form highly oxygenated organic molecules (HOMs). Under the perturbation of OH oxidation with increased NOx , the contribution of HOM-ion signals to the particle-phase signal remains elevated for more substituted aromatic precursors. Up to 43%of product signal comes from ring-retaining ions including HOMs; this is most mportant for the more substituted aromatics. Unique products are a minor component in these systems, and many of the dominant ions have ion formulae concurrent with other systems, highlighting the challenges in utilising marker ions for SOA. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
语种	英语
scopus关键词	aerosol; aromatic hydrocarbon; atmospheric pollution; chemical composition; gas phase reaction; hydroxyl radical; mass spectrometry; oxidation; 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/141147
作者单位	Centre for Atmospheric Science, School of Earth and Environmental Sciences, University of Manchester, Manchester, United Kingdom; Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, Jiangwan Campus, Shanghai, China; Center for Aerosol and Cloud Chemistry, Aerodyne Research, Inc., Billerica, MA, United States; Wolfson Atmospheric Chemistry Laboratories, Department of Chemistry, University of York, York, United Kingdom; National Centre for Atmospheric Science (NCAS), University of York, York, United Kingdom; Department of Chemistry, University of Colorado Boulder, Boulder, CO, United States; Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO, United States; Now At: Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden; Department of Chemistry, University of Colorado Boulder, Boulder, CO, United States
推荐引用方式 GB/T 7714	Mehra A.,Wang Y.,E. Krechmer J.,et al. Evaluation of the chemical composition of gas- And particle-phase products of aromatic oxidation[J],2020,20(16).
APA	Mehra A..,Wang Y..,E. Krechmer J..,Lambe A..,Majluf F..,...&Coe H..(2020).Evaluation of the chemical composition of gas- And particle-phase products of aromatic oxidation.Atmospheric Chemistry and Physics,20(16).
MLA	Mehra A.,et al."Evaluation of the chemical composition of gas- And particle-phase products of aromatic oxidation".Atmospheric Chemistry and Physics 20.16(2020).