气候变化领域集成服务门户(CCPortal): Organic aerosol source apportionment in Zurich using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) - Part 1: Biogenic influences and day-night chemistry in summer

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DOI	10.5194/acp-19-14825-2019
	Organic aerosol source apportionment in Zurich using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) - Part 1: Biogenic influences and day-night chemistry in summer
	Stefenelli G.; Pospisilova V.; Lopez-Hilfiker F.D.; Daellenbach K.R.; Hüglin C.; Tong Y.; Baltensperger U.; Prevot A.S.H.; Slowik J.G.
发表日期	2019
ISSN	16807316
起始页码	14825
结束页码	14848
卷号	19 期号:23
英文摘要	Improving the understanding of the health and climate impacts of aerosols remains challenging and is restricted by the limitations of current measurement techniques. Detailed investigation of secondary organic aerosol (SOA), which is typically the dominating fraction of the organic aerosol (OA), requires instrumentation capable of real-time, in situ measurements of molecular composition. In this study, we present the first ambient measurements by a novel extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS). The EESI-TOF-MS was deployed along with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) during summer 2016 at an urban location (Zurich, Switzerland). Positive matrix factorization (PMF), implemented within the Multilinear Engine (ME-2), was applied to the data from both instruments to quantify the primary and secondary contributions to OA. From the EESI-TOF-MS analysis, a six-factor solution was selected as the most representative and interpretable solution for the investigated dataset, including two primary and four secondary factors. The primary factors are dominated by cooking and cigarette smoke signatures while the secondary factors are discriminated according to their daytime (two factors) and night-time (two factors) chemistry. All four factors showed strong influence by biogenic emissions but exhibited significant day-night differences. Factors dominating during daytime showed predominantly ions characteristic of monoterpene and sesquiterpene oxidation while the night-time factors included less oxygenated terpene oxidation products, as well as organonitrates which were likely derived from NO3 radical oxidation of monoterpenes. Overall, the signal measured by the EESI-TOF-MS and AMS showed a good correlation. Further, the two instruments were in excellent agreement in terms of both the mass contribution apportioned to the sum of POA and SOA factors and the total SOA signal. However, while the oxygenated organic aerosol (OOA) factors separated by AMS analysis exhibited a flat diurnal pattern, the EESI-TOF-MS factors illustrated significant chemical variation throughout the day. The captured variability, inaccessible from AMS PMF analysis, was shown to be consistent with the variations in the physiochemical processes influencing chemical composition and SOA formation. The improved source separation and interpretability of EESI-TOF-MS results suggest it to be a promising approach to source apportionment and atmospheric composition research. © Author(s) 2019.
语种	英语
scopus关键词	aerosol; atmospheric chemistry; biogenic emission; human activity; ionization; mass spectrometry; oxidation; source apportionment; summer; Switzerland; Zurich [Switzerland]
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/143986
作者单位	Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), Villigen, 5232, Switzerland; Empa Laboratory for Air Pollution and Environmental Technology, Dübendorf, 8600, Switzerland; Tofwerk AG, Uttigenstrasse 22, Thun, 3600, Switzerland; Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland
推荐引用方式 GB/T 7714	Stefenelli G.,Pospisilova V.,Lopez-Hilfiker F.D.,et al. Organic aerosol source apportionment in Zurich using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) - Part 1: Biogenic influences and day-night chemistry in summer[J],2019,19(23).
APA	Stefenelli G..,Pospisilova V..,Lopez-Hilfiker F.D..,Daellenbach K.R..,Hüglin C..,...&Slowik J.G..(2019).Organic aerosol source apportionment in Zurich using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) - Part 1: Biogenic influences and day-night chemistry in summer.Atmospheric Chemistry and Physics,19(23).
MLA	Stefenelli G.,et al."Organic aerosol source apportionment in Zurich using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF-MS) - Part 1: Biogenic influences and day-night chemistry in summer".Atmospheric Chemistry and Physics 19.23(2019).