Atmospheric Measurement Techniques
www.atmos-meas-tech.net
1867-1381
1867-8548
3
4
2010
10.5194/amt-3-1063-2010
http://www.atmos-meas-tech.net/3/1063/2010/
http://www.atmos-meas-tech.net/3/1063/2010/amt-3-1063-2010.html
http://www.atmos-meas-tech.net/3/1063/2010/amt-3-1063-2010.pdf
1063
1074
2010-08-18
High time-resolution chemical characterization of the water-soluble fraction of ambient aerosols with PILS-TOC-IC and AMS
H. Timonen
hilkka.timonen@fmi.fi
M. Aurela
S. Carbone
K. Saarnio
S. Saarikoski
T. Mäkelä
M. Kulmala
V.-M. Kerminen
D. R. Worsnop
R. Hillamo
Air Quality Research, Finnish Meteorological Institute, P.O. Box 503, 00101 Helsinki, Finland
Department of Physics, University of Helsinki, P.O. Box 64, 00014 University of Helsinki, Finland
Aerodyne Research, Inc., 45 Manning Road, Billerica, MA 01821-3976, USA
A particle-into-liquid sampler (PILS) was coupled with a total organic
carbon analyzer (TOC) and two ion chromatographs (IC) to enable high
time-resolution measurements of water-soluble ions and water-soluble organic
carbon (WSOC) by a single sampling and analytical set-up. The new high
time-resolution measurement system, the PILS-TOC-IC, was able to provide
essential chemical and physical information about fast changes in
composition, concentrations and likely sources of the water-soluble fraction
of atmospheric aerosol. The concentrations of major water-soluble ions and
WSOC were measured by the PILS-TOC-IC system from 25 April to 28 May 2009.
<br><br>
The data of the PILS-TOC-IC setup was compared with the data from the
High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) data
measured from 25 April to 8 May 2009. The measured water-soluble
particulate organic matter (WSPOM) concentration varied typically from 0.10
to 8.8 μg m<sup>−3</sup> (on average 1.5 μg m<sup>−3</sup>). The WSPOM
contributed on average 51% to particulate organic matter (POM) measured
with the AMS. The correlation between the data of all the online measurement
devices (AMS, PILS-TOC-IC, semicontinuous EC/OC carbon analyzer and TEOM)
was excellent. For sulfate, nitrate and ammonium the correlations between
the PILS-TOC-IC and AMS were 0.93, 0.96 and 0.96, respectively. The
correlation between WSPOM and POM was also strong (<I>r</I> = 0.88). The identified
sources of WSPOM were long-range transported biomass burning and secondary
organic aerosol (SOA) formation. WSPOM and oxalate produced in biomass
burning were clearly correlated with carbon monoxide.
Arhami, M., Kuhn, T., Fine, P. M., Delfino, R. J., and Sioutas, C.: Effects of Sampling Artifacts and Operating Parameters on the Performance of a semicontinuous Particulate Elemental Carbon/Organic Carbon Monitor, Environ. Sci. Technol., 40, 945–954, 2006.
Bae, M.-S., Schwab, J. J., Zhang, Q., Hogrefe, O., Demerjian, K. L., Weimer, S., Rhoads, K., Orsini, D., Venkatachari, P., and Hopke, P. K.: Interference of organic signals in highly time resolved nitrate measurements by low mass resolution aerosol mass spectrometry, J. Geophys. Res., 112, D22305, doi:10.1029/2007JD008614, 2007.
Broekhuizen, K., Chang, R.Y.-W., Leaitch, W. R., Li, S.-M., and Abbatt, J. P. D.: Closure between measured and modeled cloud condensation nuclei (CCN) using size-resolved aerosol compositions in downtown Toronto, Atmos. Chem. Phys., 6, 2513–2524, doi:10.5194/acp-6-2513-2006, 2006.
Claeys, M., Graham, B., Vas, G., Wang, W., Vermeylen, R., Pashynska, V., Cafmeyer, J., Guyon, P., Andreae, M. O., Artaxo, P., and Maenhaut, W.: Formation of secondary organic aerosols through photooxidation of isoprene, Science, 303, 1173–1176, doi:10.1126/science.1092805, 2004.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop, D. R., and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, 2006.
Decesari, S., Facchini, M. C., Fuzzi, S., and Tagliavini, E.: Characterization of water-soluble organic compounds in atmospheric aerosols: a new approach, J. Geophys. Res., 105, 1481–1489, 2000.
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, Atmos. Environ., 36, 3691–3699, 2001.
Decesari, S., Fuzzi, S., Facchini, M. C., Mircea, M., Emblico, L., Cavalli, F., Maenhaut, W., Chi, X., Schkolnik, G., Falkovich, A., Rudich, Y., Claeys, M., Pashynska, V., Vas, G., Kourtchev, I., Vermeylen, R., Hoffer, A., Andreae, M. O., Tagliavini, E., Moretti, F., and Artaxo, P.: Characterization of the organic composition of aerosols from Rondônia, Brazil, during the LBA-SMOCC 2002 experiment and its representation through model compounds, Atmos. Chem. Phys., 6, 375–402, doi:10.5194/acp-6-375-2006, 2006.
Decesari, S., Mircea, M., Cavalli, F., Fuzzi, S., Moretti, F., Tagliavini, E., and Facchini, M. C.: Source attribution of water-soluble organic aerosol by nuclear magnetic resonance spectroscopy, Environ. Sci. Technol., 41, 2479–2484, 2007.
Ding, X., Zheng, M., Yu, L., Luzhang, X., Weber, R., Yan, B., Russell, A. G., Edgerton, E. S., and Wang, X.: Spatial and Seasonal Trends in Biogenic Secondary Organic Aerosol Tracers and Water-Soluble Organic Carbon in the Southeastern United States, Environ. Sci. Technol., 42, 5171–5176, 2008.
Facchini, M. C., Mircea, M., Fuzzi, S., and Charlson, R. J.: Cloud albedo enhancement by surface-active organic solutes in growing droplets, Nature, 401, 257–259, doi:10.1038/45758, 1999.
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, doi:10.5194/acp-6-2017-2006, 2006.
de Gouw, J. A., Brock, C. A., Atlas, E. L., Bates, T. S., Fehsenfeld, F. C., Goldan, P. D., Holloway, J. S., Kuster, W. C., Lerner, B. M., Matthew, B. M., Middlebrook, A. M., Onasch, T. B., Peltier, R. E., Quinn, P. K., Senff, C. J., Stohl, A., Sullivan, A. P., Trainer, M., Warneke, C., Weber, R. J., and Williams, E. J.: Sources of particulate matter in the northeastern United States in summer: Direct emissions and secondary formation of organic matter in urban plumes, J. Geophys. Res., 113, D08301, doi:10.1029/2007JD009243, 2008.
Graber, E. R. and Rudich, Y.: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Chem. Phys., 6, 729–753, doi:10.5194/acp-6-729-2006, 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.
Hennigan, C. J., Sandholm, S., Kim, S., Stickel, R. E., Huey, L. G., and Weber, R. J.: Influence of Ohio River valley emissions on fine particle sulfate measured from aircraft over large regions of the eastern United States and Canada during INTEX-NA, J. Geophys. Res., 111, D24S04, doi:10.1029/2006JD007282, 2006.
Hennigan, C. J., Bergin, M. H., Dibb, J. E., and Weber, R. J.: Enhanced secondary organic aerosol formation due to water uptake by fine particles, Geophys. Res. Lett., 35, L18801, doi:10.1029/2008GL035046, 2008a.
Hennigan, C. J., Bergin, M. H., and Weber, R. J.: Correlations between water-soluble organic aerosol and water vapor: A synergistic effect from biogenic emissions?, Environ. Sci. Technol., 42, 9079–9085, 2008b.
Hennigan, C. J., Sullivan, A. P., Fountoukis, C. I., Nenes, A., Hecobian, A., Vargas, O., Peltier, R. E., Case Hanks, A. T., Huey, L. G., Lefer, B. L., Russell, A. G., and Weber, R. J.: On the volatility and production mechanisms of newly formed nitrate and water soluble organic aerosol in Mexico City, Atmos. Chem. Phys., 8, 3761–3768, doi:10.5194/acp-8-3761-2008, 2008c.
Hennigan, C. J., Bergin, M. H., Russell, A. G., Nenes, A., and Weber, R. J.: Gas/particle partitioning of water-soluble organic aerosol in Atlanta, Atmos. Chem. Phys., 9, 3613–3628, doi:10.5194/acp-9-3613-2009, 2009.
Hsieh, L.-Y., Kuo, S.-C., Chen, C.-L., and Tsai, Y. I.: Origin of low-molecular-weight dicarboxylic acids and their concentration and size distribution variation in suburban aerosol, Atmos. Environ., 41, 6648–6661, 2007.
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.
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, doi:10.5194/acp-5-2809-2005, 200.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., et al.: Evolution of Organic Aerosols in the Atmosphere, Science, 326, 1525–1529, 2009.
Järvi, L., Hannuniemi, H., Hussein, T., Junninen, H., Aalto, P. P., Hillamo, R., Mäkelä, T., Keronen, P., Siivola, E., Vesala, T., and Kulmala, M.: The urban measurement station SMEAR III: Continuous monitoring of air pollution and surface–atmosphere interactions in Helsinki, Finland, Boreal Env. Res., 14(suppl. A), 86–109, 2009.
Kokkola, H., Sorjamaa, R., Peräniemi, A., Raatikainen, T., and Laaksonen. A.: Cloud formation of particles containing humic-like substances, Geophys. Res. Lett., 33, L10816, doi:10.1029/2006GL026107, 2006.
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.
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, doi:10.5194/acp-4-557-2004, 2004.
Kuokka, S., Teinilä, K., Saarnio, K., Aurela, M., Sillanpää, M., Hillamo, R., Kerminen, V.-M., Pyy, K., Vartiainen, E., Kulmala, M., Skorokhod, A. I., Elansky, N. F., and Belikov, I. B.: Using a moving measurement platform for determining the chemical composition of atmospheric aerosols between Moscow and Vladivostok, Atmos. Chem. Phys., 7, 4793–4805, doi:10.5194/acp-7-4793-2007, 2007.
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.
Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B., Hueglin, C., and Prévôt, A. S. H.: Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra, Atmos. Chem. Phys., 7, 1503–1522, doi:10.5194/acp-7-1503-2007, 2007.
Miyazaki, Y., Kondo, Y., Takegawa, N., Komazaki, Y., Fukuda, M., Kawamura, K., Mochida, M., Okuzawa, K., and Weber, R. J.: Time-resolved measurements of water-soluble organic carbon in Tokyo, J. Geophys. Res., 111, D23206, doi:10.1029/2006JD007125, 2006.
Miyazaki, Y., Kondo, Y., Shiraiwa, M., Takegawa, N., Miyakawa, T., Han, S., Kita, K., Hu, M., Deng, Z. Q., Zhao, Y., Sugimoto, N., Blake, D. R., and Weber, R. J.: Chemical characterization of water-soluble organic carbon aerosols at a rural site in the Pearl River Delta, China, in the summer of 2006, J. Geophys. Res., 114, D14208, doi:10.1029/2009JD011736, 2009.
Orsini, D., Ma, Y., Sullivan, A., Sierau, B., Baumann, K., and Weber, R.: Refinements to the particle-into-liquid sampler (PILS) for ground and airborne measurements of water-soluble aerosol composition, Atmos. Environ., 37, 1243–1259, 2003.
Ovadnevaitë, J., Kvietkus, K., and MarÅ¡alka, A.: 2002 summer fires in Lithuania: Impact on the Vilnius city air quality and the inhabitants health, Sci. Total Environ., 356, 11–21, 2006.
Parshintsev, J., Räsänen, R., Hartonen, K., Kulmala, M., and Riekkola, M.-L.: Analysis of organic compounds in ambient aerosols collected with the particle-into-liquid sampler, Boreal Env. Res., 14, 630–640, 2009.
Peltier, R. E., Weber, R. J., and Sullivan, A. P.: Investigating a Liquid-Based Method for Online Organic Carbon Detection in Atmospheric Particles, Aerosol Sci. Technol., 41(12), 1117–1127, 2007.
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 fine particulate matter in northern European urban air, Atmos. Chem. Phys., 8, 6281–6295, doi:10.5194/acp-8-6281-2008, 2008.
Saarnio, K., Aurela, M., Timonen, H., Saarikoski, S., Teinilä, K., Mäkelä, T., Sofiev, M., Koskinen, J., Aalto, P. P., Kulmala, M., Kukkonen, J., and Hillamo, R.: Chemical composition of fine particles in fresh smoke plumes from boreal wild-land fires in Europe, Sci. Total Environ., 405, 2527–2542, 2010.
Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric particles: a critical review of the literature and application of thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57–109, 1996.
Sillanpää, M., Saarikoski, S., Hillamo, R., Pennanen, A., Makkonen, U., Spolnik, Z., 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.
Sorooshian, A., Varutbangkul, V., Brechtel, F. J., Ervens, B., Feingold, G., Bahreini, R., Murphy, S. M., Holloway, J. S., Atlas, E. L., Buzorius, G., Jonsson, H., Flagan, R. C., and Seinfeld, J. H.: Oxalic acid in clear and cloudy atmospheres: Analysis of data from International Consortium for Atmospheric Research on Transport and Transformation 2004, J. Geophys. Res., 111, D23S45, doi:10.1029/2005JD006880, 2006.
Sorooshian, A., Ng, N. L., Chan, A. W. H., Feingold, G., Flagan, R. C., and Seinfeld, J. H.: Particulate organic acids and overall water-soluble aerosol composition measurements from the 2006 Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS), J. Geophys. Res., 112, D13201, doi:10.1029/2007JD008537, 2007.
Stohl, A. and Wotawa, G.: A method for computing single trajectories representing boundary layer transport, Atmos. Environ., 29, 3235–3239, 1995.
Sueper, D.: ToF-AMS High resolution analysis software- available online at: http://cires.colorado.edu/jimenez-group/ToFAMSResources/ToFSoftware/index.html, 2009.
Sullivan, A. P., Peltier, R. E., Brock, C. A., de Gouw, J. A., Holloway, J. S., Warneke, C., Wollny, A. G., and Weber, R. J.: Airborne measurements of carbonaceous aerosol soluble in water over northeastern United States: Method development and an investigation into water-soluble organic carbon sources, J. Geophys. Res., 111, D23S46, doi:10.1029/2006JD007072, 2006.
Szidat, S., Jenk, T. M., Synal, H. -A., Kalberer, M., Wacker, L., Hajdas, I., Kasper-Giebl, A., and Baltensperger, U.: Contributions of fossil fuel, biomass-burning, and biogenic emissions to carbonaceous aerosols in Zurich as traced by $^14$C, J. Geophys. Res., 111, D07206, doi:10.1029/2005JD006590, 2006.
Szidat, S., Ruff, M., Perron, N., Wacker, L., Synal, H.-A., Hallquist, M., Shannigrahi, A. S., Yttri, K. E., Dye, C., and Simpson, D.: Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden, Atmos. Chem. Phys., 9, 1521–1535, doi:10.5194/acp-9-1521-2009, 2009.
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.
Ten Brink, H., Maenhaut, W., Hitzenberger, R., Gnauk, T., Spindler, G., Even, A., Chi, X., Bauer, H., Puxbaum, H., Putaud, J., Tursic, J., and Berner, A.: INTERCOMP2000: the comparability of methods in use in Europe for measuring the carbon content of aerosol, Atmos. Environ., 38, 6507–6519, 2004.
Turpin, B. J. and Lim, H.-J.: Species contributions to PM$_2.5 $mass concentrations: revisiting common assumptions for estimating organic mass, Aerosol Sci. Technol., 35, 602–610, 2001.
Viana, M., Maenhaut, W., ten Brink, H. M., Chi, X., Weijers, E., Querol, X., Alastuey, A., MikuÅ¡ka, P., Veèeøa, Z.: Comparative analysis of organic and elemental carbon concentrations in carbonaceous aerosols in three European cities, Atmos. Environ., 41, 5972–5983, 2007.
Warren, B., Austin, R., and Cocker III, D. R.: Temperature dependence of secondary organic aerosol, Atmos. Environ., 43, 3548–3555, 2009.
Watson, J. G., Chow, J. C., Lu, Z., Fujita, E. M., Lowenthal, D. H., and Lawson, D. R.: Chemical mass balance source apportionment of PM$_10$ during the Southern California air quality study, Aerosol Sci. Technol., 21, 1–36, 1994.
Weber, R. J. Orsini, D., Daun, Y., Lee, Y.-N., Klotz, P. J., and Brechtel, F.: A Particle-into-Liquid Collector for Rapid Measurement of Aerosol Bulk Chemical Composition, Aerosol Sci. Technol., 35, 718–727, 2001.
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.
Yang, H., Yu, J. Z., Ho, S. S. H., Xu, J., Wu, W., Wan, C. H., Wang, X., Wang, X. and Wang, L.: The chemical composition of inorganic and carbonaceous materials in PM$_2.5 $in Nanjing, China, Atmos. Environ., 39, 3735–3749, 2005.
Zhang, Y., Schauer, J., Shafer, M., Hannigan, M., and Dutton, S.: Source apportionment of in Vitro Reactive Oxygen Species Bioassay Activity from Atmospheric Particulate Matter, Environ. Sci. Technol., 42, 7502–7509, 2008.