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© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 10 Jan 2020

Submitted as: research article | 10 Jan 2020

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A revised version of this preprint is currently under review for the journal ACP.

One-year characterization of organic aerosol composition and sources using an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF)

Lu Qi1,2, Alexander L. Vogel1,a, Sepideh Esmaeilirad1, Liming Cao3, Jing Zheng4, Jean-Luc Jaffrezo5, Paola Fermo6, Anne Kasper-Giebl7, Kaspar R. Daellenbachb, Mindong Chen2, Xinlei Ge2, Urs Baltensperger1, André S. H. Prévôt1, and Jay G. Slowik1 Lu Qi et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute (PSI), 5232 Villigen, Switzerland
  • 2Collavorative Innovation Center of Atmospheric Environment and Equipment Technology, Nanjing University of Information Science & Technology, Nanjing, 210044, China
  • 3Key Laboratory for Urban Habitat Environmental Science and Technology, School of Environment and Energy, Peking University Shenzhen Graduate School, Shenzhen, 518055, China
  • 4State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing 100871, China
  • 5University Grenoble Alpes, CNRS, IGE, 38000 Grenoble, France
  • 6Department of Chemistry, University of Milan, 20133 Milan, Italy
  • 7Institute of Chemical Technologies and Analytics, Vienna University of Technology, 1060 Vienna, Austria
  • anow at: Institute for Atmospheric and Environmental Sciences, Goethe University, Frankfurt am Main, Germany
  • bnow at: Institute for Atmospheric and Earth System Research, University of Helsinki, Finland

Abstract. The aerosol mass spectrometer (AMS), combined with statistical methods such as positive matrix factorization (PMF), has greatly advanced the quantification of primary organic aerosol (POA) sources and total secondary organic aerosol (SOA) mass. However, the use of thermal vaporization and electron ionization yields extensive thermal decomposition and ionization-induced fragmentation, which destroy chemical information needed for SOA source apportionment. The recently developed extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF) provides mass spectra of the organic aerosol fraction with a linear response to mass and no thermal decomposition or ionization-induced fragmentation. However, the costs and operational requirements of online instruments make their use impractical for long-term or spatially dense monitoring applications. This challenge was overcome for AMS measurements by measuring re-nebulized water extracts from ambient filter samples. Here, we apply the same strategy for EESI-TOF measurements of 1 year of 24-hour filter samples collected approximately every 4th day throughout 2013 at the NABEL monitoring station at Zurich-Kaserne, an urban site. The nebulized water extracts were measured simultaneously with an AMS. The application of positive matrix factorization (PMF) to EESI-TOF spectra resolved seven factors, which describe water-soluble OA: less and more aged biomass burning aerosol (LABBEESI and MABBEESI, respectively), cigarette smoke-related organic aerosol (CS-OAEESI), primary biological organic aerosol (PBOAEESI), biogenic secondary organic aerosol (BSOAEESI), and a summer mixed oxygenated organic aerosol (SMOAEESI) factor. Seasonal trends and relative contributions of the EESI-TOF OA sources were compared with AMS source apportionment factors, measured water-soluble ions, cellulose, and meteorological data. Cluster analysis was utilized to identify key factor-specific ions based on PMF. Both LABB and MABB contribute strongly during winter. LABB is distinguished by very high signals from C6H10O5 (levoglucosan and isomers) and C8H12O6, whereas MABB is characterized by a large number of CxHyOz and CxHyOzN species two distinct populations: one with low H : C and high O : C, and the other with high H : C and low O : C. Two oxygenated summertime SOA sources were attributed to terpene-derived biogenic SOA, a major summertime aerosol source in Central Europe. Furthermore, a primary biological organic aerosol factor was identified, which was dominated by plant-derived fatty acids and correlated with free cellulose. The CS-OA factor contained a high contribution of nicotine and high abundance of organic nitrate ions with low m/z.

Lu Qi et al.

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Lu Qi et al.


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Latest update: 02 Jun 2020
Publications Copernicus
Short summary
We present the first application of this online/offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
We present the first application of this online/offline strategy using the new extractive...