Organic aerosol source apportionment by offline-AMS over a full year in Marseille

Article, 0038 English OPEN
Bozzetti , Carlo ; El Haddad , Imad ; Salameh , Dalia ; Daellenbach , Kaspar Rudolf ; Fermo , Paola ; Gonzalez , Raquel ; Minguillón , María Cruz ; Iinuma , Yoshiteru ; Poulain , Laurent ; Elser , Miriam ; Müller , Emanuel ; Slowik , Jay Gates ; Jaffrezo , Jean-Luc ; Baltensperger , Urs ; Marchand , Nicolas ; Prévôt , André Stephan Henry (2017)
  • Publisher: European Geosciences Union
  • Journal: (issn: 1680-7324)
  • Related identifiers: doi: 10.5194/acp-17-8247-2017, doi: 10.5194/acp-2017-54
  • Subject: Settore CHIM/01 - Chimica Analitica | [ SDU.OCEAN ] Sciences of the Universe [physics]/Ocean, Atmosphere | [ CHIM.ANAL ] Chemical Sciences/Analytical chemistry | [ SDE.MCG ] Environmental Sciences/Global Changes

International audience; We investigated the seasonal trends of OA sources affecting the air quality of Marseille (France), which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). In total 216 PM 2.5 (particulate matter with an aerodynamic diameter < 2.5 µm) filter samples were collected over 1 year from August 2011 to July 2012. These filters were used to create 54 composite samples which were analyzed by offline-AMS. The same samples were also analyzed for major water-soluble ions, metals, elemental and organic carbon (EC / OC), and organic markers, including n-alkanes, hopanes, polycyclic aromatic hydrocarbons (PAHs), lignin and cellulose pyrolysis products , and nitrocatechols. The application of positive matrix factorization (PMF) to the water-soluble AMS spectra enabled the extraction of five factors, related to hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), oxygenated OA (OOA), and an industry-related OA (INDOA). Seasonal trends and relative contributions of OA sources were compared with the source apportionment of OA spectra collected from the AMS field deployment at the same station but in different years and for shorter monitoring periods (February 2011 and July 2008). Online-and offline-AMS source apportionment revealed comparable seasonal contribution of the different OA sources. Results revealed that BBOA was the dominant source during winter, representing on average 48 % of the OA, while during summer the main OA component was OOA (63 % of OA mass on average). HOA related to traffic emissions contributed on a yearly average 17 % to the OA mass, while COA was a minor source contributing 4 %. The contribution of INDOA was enhanced during winter (17 % during winter and 11 % during summer), consistent with an increased contribution from light alkanes, light PAHs (fluoranthene, pyrene, phenanthrene), and selenium, which is commonly considered as a unique coal combustion and coke production marker. Online-and offline-AMS source apportionments revealed evolving lev-oglucosan : BBOA ratios, which were higher during late autumn and March. A similar seasonality was observed in the ratios of cellulose combustion markers to lignin combustion markers, highlighting the contribution from cellulose-rich biomass combustion, possibly related to agricultural activities .
  • References (73)
    73 references, page 1 of 8

    Aceves, M. and Grimalt, J. O.: Seasonally dependent size distributions of aliphatic and polycyclic aromatic hydrocarbons in urban aerosols from densely populated areas, Environ. Sci. Technol., 27, 2896-2908,, 1993.

    Aiken, A. C., DeCarlo, P. F., Kroll, J. H., Worsnop, D. R., Huffmann, J. A., Docherty, K. S., Ulbrich, I. M., Mohr, C., Kimmel, J. R., Sueper, D., Sun, Y., Zhang, Q., Trimborn, A., Northway, M., Ziemann, P. J., Canagaratna, M. R., Onasch, T. B., Alfarra, M. R., Prevot, A. S. H., Dommen, J., Duplissy, J., Metzger, A., Baltensperger, U., and Jimenez J. L.: O = C and OM : OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry, Environ. Sci. Technol., 42, 4478-4485, 2008.

    Alfarra, M. R., Prévôt, A. S. H., Szidat, S., Sandradewi, J., Weimer, S., Lanz, V. A., Schreiber, D., Mohr, M., and Baltensperger, U.: Identification of the mass spectral signature of organic aerosols from wood burning emissions, Environ. Sci. Technol., 41, 5770- 5777, 2007.

    Allan, J. D., Jimenez, J. L., Williams, P. I., Alfarra, M. R., Bower, K. N., Jayne, J. T., Coe, H., and Worsnop, D. R.: Quantitative sampling using an Aerodyne aerosol mass spectrometer: 1. Techniques of data interpretation and error analysis, J. Geophys. Res.-Atmos., 108, 4090,, 2003.

    Atkinson, R. and Arey, J.: Atmospheric degradation of volatile organic compounds, Chem. Rev., 103, 4605-4638, 2003.

    Birch, M. E. and Cary, R. A.: Elemental carbon-based method for monitoring occupational exposures to particulate diesel exhaust, Aerosol Sci. Tech., 25, 221-241, 1996.

    Bozzetti, C.: Recovery combinations,, 2017.

    Bozzetti, C., Daellenbach, K., R., Hueglin, C., Fermo, P., Sciare, J., Kasper-Giebl, A., Mazar, Y., Abbaszade, G., El Kazzi, M., Gonzalez, R., Shuster Meiseles, T., Flasch, M., Wolf, R., Krˇepelová, A., Canonaco, F., Schnelle-Kreis, J., Slowik, J. G., Zimmermann, R., Rudich, Y., Baltensperger, U., El Haddad, I., and Prévôt, A. S. H.: Size-resolved identification, characterization, and quantification of primary biological organic aerosol at a European rural site, Environ. Sci. Technol., 50, 3425-3434,, 2016.

    Bozzetti, C., Sosedova, Y., Xiao, M., Daellenbach, K. R., Ulevicius, V., Dudoitis, V., Mordas, G., Bycenkiene, S., Plauškaite, K., Vlachou, A., Golly, B., Chazeau, B., Besombes, J.-L., Baltensperger, U., Jaffrezo, J.-L., Slowik, J. G., El Haddad, I., and Prévôt, A. S. H.: Argon offline-AMS source apportionment of organic aerosol over yearly cycles for an urban, rural, and marine site in northern Europe, Atmos. Chem. Phys., 17, 117-141,, 2017.

    Brown, S. G., Eberly, S., Paatero, P., and Norris, G. A.: Methods for estimating uncertainty in PMF solutions: Examples with ambient air and water quality data and guidance on reporting PMF results, Sci. Total Environ., 518-519, 626-635, 2015.

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