气候变化领域集成服务门户(CCPortal): Chemical characterisation of benzene oxidation products under high- And low-NOx conditions using chemical ionisation mass spectrometry

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DOI	10.5194/acp-21-3473-2021
	Chemical characterisation of benzene oxidation products under high- And low-NOx conditions using chemical ionisation mass spectrometry
	Priestley M.; Bannan T.J.; Le Breton M.; Worrall S.D.; Kang S.; Pullinen I.; Schmitt S.; Tillmann R.; Kleist E.; Zhao D.; Wildt J.; Garmash O.; Mehra A.; Bacak A.; Shallcross D.E.; Kiendler-Scharr A.; Hallquist A.M.; Ehn M.; Coe H.; Percival C.J.; Hallquist M.; Mentel T.F.; McFiggans G.
发表日期	2021
ISSN	1680-7316
起始页码	3473
结束页码	3490
卷号	21 期号:5
英文摘要	Aromatic hydrocarbons are a class of volatile organic compounds associated with anthropogenic activity and make up a significant fraction of urban volatile organic compound (VOC) emissions that contribute to the formation of secondary organic aerosol (SOA). Benzene is one of the most abundant species emitted from vehicles, biomass burning and industry. An iodide time-of-flight chemical ionisation mass spectrometer (ToF-CIMS) and nitrate ToF-CIMS were deployed at the Jülich Plant Atmosphere Chamber as part of a series of experiments examining benzene oxidation by OH under high- and low-NOx conditions, where a range of organic oxidation products were detected. The nitrate scheme detects many oxidation products with high masses, ranging from intermediate volatile organic compounds (IVOCs) to extremely low volatile organic compounds (ELVOCs), including C12 dimers. In comparison, very few species with C≥6 and O≥8 were detected with the iodide scheme, which detected many more IVOCs and semi-volatile organic compounds (SVOCs) but very few ELVOCs and low volatile organic compounds (LVOCs). A total of 132 and 195 CHO and CHON oxidation products are detected by the iodide ToF-CIMS in the low- and high-NOx experiments respectively. Ring-breaking products make up the dominant fraction of detected signal and 21 and 26 of the products listed in the Master Chemical Mechanism (MCM) were detected. The time series of highly oxidised (O≥6) and ring-retaining oxidation products (C6 and double-bond equivalentD4) equilibrate quickly, characterised by a square form profile, compared to MCM and ring-breaking products which increase throughout oxidation, exhibiting sawtooth profiles. Under low-NOx conditions, all CHO formulae attributed to radical termination reactions of first-generation benzene products, and first-generation auto-oxidation products are observed. Several N-containing species that are either first-generation benzene products or first-generation auto-oxidation products are also observed under high-NOx conditions. Hierarchical cluster analysis finds four clusters, of which two describe photo-oxidation. Cluster 2 shows a negative dependency on the NO2/NOx ratio, indicating it is sensitive to NO concentration and thus likely to contain NO addition products and alkoxy-derived termination products. This cluster has the highest average carbon oxidation state (OSC/ and the lowest average carbon number. Where nitrogen is present in a cluster member of cluster 2, the oxygen number is even, as expected for alkoxy-derived products. In contrast, cluster 1 shows no dependency on the NO2/NOx ratio and so is likely to contain more NO2 addition and peroxy-derived termination products. This cluster contains fewer fragmented species, as the average carbon number is higher and OSC lower than cluster 2, and more species with an odd number of oxygen atoms. This suggests that clustering of time series which have features pertaining to distinct chemical regimes, for example, NO2/NOx perturbations, coupled with a priori knowledge, can provide insight into identification of potential functionality. © 2021 EDP Sciences. All rights reserved.
语种	英语
scopus关键词	aerosol composition; benzene; ionization; mass spectrometry; nitrous oxide; oxidation; PAH; source apportionment; volatile organic compound; Germany; Julich; North Rhine-Westphalia
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/247084
作者单位	Centre for Atmospheric Science, Department of Earth and Environmental Sciences, University of Manchester, Manchester, United Kingdom; Institut für Energie und Klimaforschung, IEK-8, Forschungszentrum Jülich, Jülich, Germany; School of Chemistry, University of Bristol, Cantock's Close, Bristol, United Kingdom; Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland; Department of Chemistry, University of the Western Cape, Bellville, South Africa; Department of Chemistry and Molecular Biology, University of Gothenburg, Gothenburg, Sweden; Institut für Bio- und Geowissenschaften, IBG-2, Forschungszentrum Jülich GmbH, Jülich, Germany; Ivl Swedish Environmental Research Institute, Gothenburg, Sweden; Jet Propulsion Laboratory, 4800 Oak Grove Drive, Pasadena, CA, United States; Department of Applied Physics, University of Eastern Finland, Kuopio, Finland; Aston Institute of Materials Research, School of Engineering and Applied Science, Aston Uni...
推荐引用方式 GB/T 7714	Priestley M.,Bannan T.J.,Le Breton M.,et al. Chemical characterisation of benzene oxidation products under high- And low-NOx conditions using chemical ionisation mass spectrometry[J],2021,21(5).
APA	Priestley M..,Bannan T.J..,Le Breton M..,Worrall S.D..,Kang S..,...&McFiggans G..(2021).Chemical characterisation of benzene oxidation products under high- And low-NOx conditions using chemical ionisation mass spectrometry.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(5).
MLA	Priestley M.,et al."Chemical characterisation of benzene oxidation products under high- And low-NOx conditions using chemical ionisation mass spectrometry".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.5(2021).