References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-8-5635-2008

Size distributions, sources and source areas of water-soluble organic carbon in urban background air

Timonen

¹ Saarikoski

¹ Tolonen-Kivimäki

¹ Aurela

¹ Saarnio

¹ Petäjä

² ³ Aalto

P. P.

² Kulmala

² Pakkanen

¹ Hillamo

Finnish Meteorological Institute, Air Quality, Erik Palménin Aukio 1, P.O. Box 503, 00101 Helsinki, Finland

University of Helsinki, Department of Physical Sciences, P.O. Box 64, 00014 University of Helsinki, Finland

Earth and Sun Systems Laboratory, Atmospheric Chemistry Division National Center for Atmospheric Research, P.O. Box 3000, Boulder, CO 80305-3000, USA

26 09 2008

8 18 5635 5647

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This paper represents the results of one year long measurement period of the size distributions of water-soluble organic carbon (WSOC), inorganic ions and gravimetric mass of particulate matter. Measurements were done at an urban background station (SMEAR III) by using a micro-orifice uniform deposit impactor (MOUDI). The site is located in northern European boreal region in Helsinki, Finland. The WSOC size distribution measurements were completed with the chemical analysis of inorganic ions, organic carbon (OC) and monosaccharide anhydrides from the filter samples (particle aerodynamic diameter smaller than 1 μm, PM1). Gravimetric mass concentration varied during the MOUDI samplings between 3.4 and 55.0 μg m−3 and the WSOC concentrations were between 0.3 and 7.4 μg m−3. On average, water-soluble particulate organic matter (WSPOM, WSOC multiplied by 1.6 to convert the analyzed carbon mass to organic matter mass) comprised 25±7.7% and 7.5±3.4% of aerosol PM1 mass and the PM1–10 mass, respectively. Inorganic ions contributed 33±12% and 28±19% of the analyzed PM1 and PM1–10 aerosol mass. Five different aerosol categories corresponding to different sources or source areas were identified (long-range transport aerosols, biomass burning aerosols from wild land fires and from small-scale wood combustion, aerosols originating from marine areas and from the clean arctic areas). Categories were identified mainly using levoglucosan concentration level for wood combustion and air mass backward trajectories for other groups. Clear differences in WSOC concentrations and size distributions originating from different sources or source areas were observed, although there are also many other factors which might affect the results. E.g. the local conditions and sources of volatile organic compounds (VOCs) and aerosols as well as various transformation processes are likely to have an impact on the measured aerosol composition. Using the source categories, it was identified that especially the oxidation products of biogenic VOCs in summer had a clear effect on WSOC concentrations.

References 1

Anttila, T., Kiendler-Scharr, A., Mentel, T. F., and Tillmann, R.: Size dependent partitioning of organic material: evidence for the formation of organic coatings on aqueous aerosols, J. Atmos. Chem., 57, 215–237, 2007.

Arp, H. P., Schwarzenbach, R. P., and Goss, K.: Equilibrium sorption of gaseous organic chemicals to fiber filters used for aerosol studies, Atmos. Environ., 41, 8241–8252, 2007.

Berner, A. and Lürzer, C.: Mass size distribution of traffic aerosols at Vienna, J. Phys. Chem., 84, 2079–2083, 1980.

Boy, M., Kulmala, M., Ruuskanen, T. M., Pihlatie, M., Reissell, A., Aalto, P. P., Keronen, P., Dal Maso, M., Hellen, H., Hakola, H., Jansson, R., Hanke, M., and Arnold, F.: Sulphuric acid closure and contribution to nucleation mode particle growth, Atmos. Chem. Phys., 5, 863–878, 2005.

Cavalli, F., Facchini, M. C., Decesari, S., Emblico, L., Mircea, M., Jensen, N. R., and Fuzzi, S.: Size-segregated aerosol chemical composition at a boreal site in southern Finland, during the QUEST project, Atmos. Chem. Phys., 6, 993–1002, 2006.

Chan, A. W. H., Kroll, J. H., Ng, N. L., and Seinfeld, J. H.: Kinetic modeling of secondary organic aerosol formation: effects of particle- and gas-phase reactions of semivolatile products, Atmos. Chem. Phys., 7, 4135–4147, 2007.

Decesari, S., Facchini, M. C., Matta, E., Lettini, F., Mircea, M., Fuzzi, S., Tagliavini, E., and Putaud, J.-P.: Chemical features and seasonal variation of fine aerosol water-soluble organic compounds in the Po Valley, Italy, Atmos. Environ., 35, 3691–3699, 2001.

Decesari, S., Facchini, M. C., Fuzzi, S., McFiggans, G. B., Coe, H., and Bower, K. N.: The water-soluble organic component of size-segregated aerosol, cloud water and wet depositions from Jeju Island during ACE-Asia, Atmos. Environ., 39, 211–222, 2005.

Dye, C. and Yttri, K. E.: Determination of monosaccharide anhydrides in atmospheric aerosols by use of high-performance liquid chromatography combined with high-resolution mass spectrometry, Anal. Chem., 77, 1853–1858, 2005.

Ehn, M., Petäjä, T., Aufmhoff, H., Aalto, P., Hämeri, K., Arnold, F., Laaksonen, A., and Kulmala, M.: Hygroscopic properties of ultrafine aerosol particles in the boreal forest: diurnal variation, solubility and the influence of sulfuric acid, Atmos. Chem. Phys., 7, 211–222, 2007.

Frey, A., Virkkula, A., Saarnio, K., Timonen, H., Tolonen-Kivimäki, O., Aurela, M., Hillamo, R., Tissari, J., Hytönen, K., Willman, P., Jokiniemi, J., Mannila, R., Saari, H., and Näkki, I.: Aerosol composition in fireplace emissions, Report series in aerosol science, 83, 325–329, 2006.

Fuzzi, S., Andreae, M. O., Huebert, B. J., Kulmala, M., Bond, T. C., Boy, M., Doherty, S. J., Guenther, A., Kanakidou, M., Kawamura, K., Kerminen, V.-M., Lohmann, U., Russell, L. M., and Pöschl, U.: Critical assessment of the current state of scientific knowledge, terminology, and research needs concerning the role of organic aerosols in the atmosphere, climate, and global change, Atmos. Chem. Phys., 6, 2017–2038, 2006.

Glasius, M., Ketzel, M., Wåhlin, P., Jensen, B., Mønster, J., Berkowicz, R., and Palmgren, F.: Impact of wood combustion on particle levels in a residential area in Denmark, Atmos. Environ., 40, 7115–7124, 2006.

Hakola, H., Tarvainen, V., Laurila, T., Hiltunen, V., Hellen, H., and Keronen, P.: Seasonal variation of VOC concentrations above a boreal coniferous forest, Atmos. Environ., 37, 1623–1634, 2003.

Ho, K. F., Lee, S. C., Cao, J. J., Li, Y. S., Chow, J. C., Watson, J. G., and Fung, K.: Variability of organic and elemental carbon, water soluble organic carbon, and isotopes in Hong Kong, Atmos. Chem. Phys., 6, 4569–4576, 2006.

Huang, X.-F., Yu, J. Z., He, L.-Y., and Yuan, Z.: Water-soluble organic carbon and oxalate in aerosols at a coastal urban site in China: Size distribution characteristics, sources, and formation mechanisms, J. Geophys. Res., 111, D22212, doi:10.1029/2006JD007408, 2006.

Hämeri, K., Väkevä, M., Aalto, P. P., Kulmala, M., Swietlicki, E., Zhou, J., Seidl, W., Becker, E., and O'Dowd, C. D.: Hygroscopic and CCN properties of aerosol particles in boreal forests, Tellus B, 53, 359–379, 2001.

Jacobson, M. C., Hansson, H.-C., Noone, K. L., and Charlson, R. J.: Organic atmospheric aerosols: review and state of the science, Rev. Geophys., 38, 267–294, 2000.

Jaffrezo, J.-L., Aymoz, G., Delaval, C., and Cozic, J.: Seasonal variations of the water soluble organic carbon mass fraction of aerosol in two valleys of the French Alps, Atmos. Chem. Phys., 5, 2809–2821, 2005.

Jordan, T. B., Seen, A. J., and Jacobsen, G. E.: Levoglucosan as an atmospheric tracer for wood smoke, Atmos. Environ., 40, 5316–5321, 2006.

Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, 2005.

Kondo, Y., Miyazaki, Y., Takegawa, N., Miyakawa, T., Weber, R. J., Jimenez, J. L., Zhang, Q., and Worsnop, D. R.: Oxygenated and water-soluble organic aerosols in Tokyo, J. Geophys. Res., 112, D011203, doi:10.1029/2006JD007056, 2007.

Kourtchev, I., Ruuskanen, T., Maenhaut, W., Kulmala, M., and Claeys, M.: Observation of 2-methyltetrols and related photo-oxidation products of isoprene in boreal forest aerosols from Hyytiälä, Finland, Atmos. Chem. Phys., 5, 2761–2770, 2005.

Kulmala, M., Suni, T., Lehtinen, K. E. J., Dal Maso, M., Boy, M., Reissell, A., Rannik, Ü., Aalto, P., Keronen, P., Hakola, H., Bäck, J., Hoffmann, T., Vesala, T., and Hari, P.: A new feedback mechanism linking forests, aerosols, and climate, Atmos. Chem. Phys., 4, 557–562, 2004.

Laakso, L., Hussein, T., Aarnio, P., Komppula, M., Hiltunen, V., Viisanen, Y., and Kulmala, M.: Diurnal and annual characteristics of particle mass and number concentrations in urban, rural and Arctic environments in Finland, Atmos. Environ., 37, 2629–2641, 2003.

Li, S.-M., Tang, J., Xue, H., and Toom-Sauntry, D.: Size-distribution and Estimated optical properties of carbonate, water soluble organic carbon, and sulfate in aerosols at a remote high altitude site in Western China, Geophys. Res. Lett., 27, 1107–1110, 2000.

Liu, B. Y. and Pui, D. Y.: Aerosol sampling inlets and inhalable particles. Atmos. Environ., 15, 585–600, 1981.

Marple, V. A., Rubow, K. L., and Behm, S. M.: A Microorifice Uniform Deposit Impactor (MOUDI): Description, calibration and use, Aerosol Sci. Tech., 14, 434–446, 1991.

Matta, E., Facchini, M. C., Decesari, S., Mircea, M., Cavalli, F., Fuzzi, S., Putaud, J.-P., and Dell'Acqua, A.: Mass closure on the chemical species in size-segregated atmospheric aerosol collected in an urban area of the Po Valley, Italy, Atmos. Chem. Phys., 3, 623–637, 2003.

Niemi, J V., Tervahattu, H., Vehkamäki, H., Kulmala, M., Koskentalo, T., Sillanpää, M., and Rantamäki, M.: Characterization and source identification of a fine particle episode in Finland, Atmos. Environ., 38, 5003–5012, 2004.

Niemi, J V., Tervahattu, H., Vehkamäki, H., Martikainen, J., Laakso, L., Kulmala, M., Aarnio, P., Koskentalo, T., Sillanpää, M., and Makkonen, U.: Characterization of aerosol particle episodes in Finland caused by wildfires in Eastern Europe, Atmos. Chem. Phys., 5, 2299–2310, 2005.

Pakkanen, T. A., Loukkola, K., Korhonen, C. H., Aurela M., Mäkelä, T., Hillamo, R., Aarnio, P., Koskentalo, T., Kousa, A., and Maenhaut, W.: Sources and chemical composition of atmospheric fine and coarse particles in the Helsinki area, Atmos. Environ., 35, 5381–5391, 2001.

Pio, C. A., Legrand, M., Oliveira,T., Afonso, J., Santos, C., Caseiro, A., Fialho, P., Barata, F., Puxbaum, H., Sanchez-Ochoa, A., Kasper-Giebl, A., Gelencsér, A., Preunkert, S., and Schock, M.: Climatology of aerosol composition (organic versus inorganic) at nonurban sites on a west-east transect across Europe, J. Geophys. Res., 112, D23S02, doi:10.1029/2006JD008038, 2007.

Saarikoski, S., Sillanpää, M., Saarnio, K., Timonen, H., Teinilä, K., and Hillamo, R.: Chemical composition of fine particles in major burning episodes observed in Finland in 2006, Report series in aerosol science, 83, 325–329, 2006.

Saarikoski, S., Sillanpää, M., Sofiev, M., Timonen, H., Saarnio, K., Teinilä, K., Karppinen, A., Kukkonen, J., and Hillamo, R.: Chemical composition of aerosols during a major biomass burning episode over northern Europe in spring 2006: Experimental and modeling assessments, Atmos. Environ., 41, 3577–3589, 2007.

Saarikoski, S., Timonen, H., Saarnio, K., Aurela, M., Järvi, L., Keronen, P., Kerminen, V.-M., and Hillamo, R.: Sources of organic carbon in PM$_1$ in Helsinki urban air, Atmos. Chem. Phys. Discuss., 8, 7805–7846, 2008.

Sillanpää, M., Frey, A., Hillamo, R., Pennanen, A. S., and Salonen, R. O.: Organic, elemental and inorganic carbon in particulate matter of six urban environments in Europe, Atmos. Chem. Phys., 5, 2869–2879, 2005

Sillanpää, M., Saarikoski, S., Hillamo, R., Pennanen, A., Makkonen, U., Spolnik, U., Van Grieken, R., Koskentalo, T., and Salonen, R. O.: Chemical composition, mass size distribution and source analysis of long-range transported wildfire smokes in Helsinki, Sci. Total Environ., 350, 119–135, 2005.

Stohl, A. and Wotawa, G.: A method for computing single trajectories representing boundary layer transport, Atmos. Environ., 29, 3235–3239, 1995.

Subramanian, R., Khlystov, A. Y., and Robinson, A. L.: Effect of Peak Inert-Mode Temperature on Elemental Carbon Measured Using Thermal-Optical Analysis, Aerosol Sci. Tech., 40, 763–780, 2006.

Timonen, H. J., Saarikoski, S. K., Aurela, M. A., Saarnio, K. M., and Hillamo, R. E. J.: Water-soluble organic carbon in urban aerosol: concentrations, size distributions and contribution to particulate matter, Boreal Environ. Res., 13, 335–346, 2008.

Turpin, B. J. and Lim, H.-J.: Species contributions to PM$_2.5$ mass concentrations: revisiting common assumptions for estimating organic mass, Aerosol Sci. Tech., 35, 602–610, 2001.

Tunved, P., Hansson, H.-C., Kerminen, V.-M., Ström, J., Dal Maso, M., Lihavainen, H., Viisanen, Y., Aalto, P. P., Komppula, M., and Kulmala, M.: High natural aerosol loading over boreal forests, Science, 312, 261–263, 2006.

Turšič, J., Podkrajšek, B., Grgic, I., Ctyroky, P., Berner, A., Dusek, U., and Hitzenberger, R.: Chemical composition and hygroscopic properties of size-segregated aerosol particles collected at the Adriatic coast of Slovenia, Chemosphere, 63, 1193–1202, 2006.

Viana, M., Chi X., Maenhaut, W., Querol, A., Alastuey, A., Mikuska, P., and Vecera, Z.: Organic and elemental carbon concentrations in carbonaceous aerosols during summer and winter sampling campaigns in Barcelona, Spain, Atmos. Environ., 40, 2180–2193, 2006.

Viidanoja, J., Sillanpää, M., Laakia, J., Kerminen, V.-M., Hillamo, R., Aarnio, P., and Koskentalo, T.: Organic and black carbon in PM$_2.5$ and PM$_10$: 1 year of data from an urban site in Helsinki, Finland, Atmos. Environ., 36, 3183–3193, 2002.

Virkkula, A., Van Dingenen, R., Raes, F., and Hjort, J.: Hygroscopic properties of aerosol formed by oxidation of limonene, alpha-pinene, and beta-pinene, J. Geophys. Res., 104(D3), 3569–3580, 1999.

Weber, R. J., Sullivan, A. P., Peltier, R. E., Russell, A., Yan, B., Zheng, M., de Gouw, J., Warneke, C., Brock, C., Holloway, J. S., Atlas, E. L., and Edgerton, E.: A study of secondary organic aerosol formation in the anthropogenic-influenced southeastern United States, J. Geophys. Res., 112, D13302, doi:10.1029/2007JD008408, 2007.

Yao, X., Fang, M., and Chan, C. K.: Size distributions and formation of dicarboxylic acids in atmospheric particles, Atmos. Environ., 36, 2099–2107, 2002.

Yoon, Y. J., Ceburnis, D., Cavalli, F., Jourdan, O., Putaud, J. P., Facchini, M. C., Decesari, S., Fuzzi, S., Sellegri, K., Jennings, S. G., and O'Dowd, C. D.: Seasonal characteristics of the physicochemical properties of North Atlantic marine atmospheric aerosols, J. Geophys. Res., 112, D04206, doi:10.1029/2005JD007044, 2007.

Yu, J. Z., Yang, H., Zhang, H., and Lau, A. K. H.: Size distributions of water-soluble organic carbon in ambient aerosols and its size-resolved thermal characteristics, Atmos. Environ., 38, 1061–1071, 2004.

Yttri, K. E., Dye, C., Slødal, L. H., and Braathen, O.-A.: Quantification of monosaccharide anhydrides by liquid chromatography combined with mass spectrometry: application to aerosol samples from an urban and a suburban site influenced by small-scale wood burning, J. Air Waste Manage., 55, 1169–1177, 2005.

Zdráhal, Z., Oliveira, J., Vermeylen, R., Claeys, M., and Maenhaut, W.: Improved method for quantifying levoglucosan and related monosaccharide anhydrides in atmospheric aerosols and application to samples from urban and tropical locations, Environ. Sci. Technol., 36, 747–753, 2002.