Atmospheric Chemistry and Physics
www.atmos-chem-phys.net
1680-7316
1680-7324
7
9
2007
10.5194/acp-7-2217-2007
http://www.atmos-chem-phys.net/7/2217/2007/
http://www.atmos-chem-phys.net/7/2217/2007/acp-7-2217-2007.html
http://www.atmos-chem-phys.net/7/2217/2007/acp-7-2217-2007.pdf
2217
2232
2007-05-03
A study on the relationship between mass concentrations, chemistry and number size distribution of urban fine aerosols in Milan, Barcelona and London
S. Rodríguez
srodriguez@inm.es
R. Van Dingenen
J.-P. Putaud
A. Dell'Acqua
J. Pey
X. Querol
A. Alastuey
S. Chenery
K.-F. Ho
R. Harrison
R. Tardivo
B. Scarnato
V. Gemelli
European Commission – DG Joint Research Centre, Institute for Environment and Sustainability, T.P. 290, Ispra (VA) 21020, Italy
British Geological Survey, Keyworth, Nottingham, NG12 5GG, UK
Institute of Earth Science "Jaume Almera", CSIC, Solé i Sabarís, S/N, 08028, Barcelona, Spain
University of Birmingham, Division of Environmental Health and Risk Management, Edgbaston, Birmingham B15 2TT, UK
Hong Kong Polytechnic University, Department of Civil and Structural Engineering, TU418, Hung Hom, Kowloon, Hong Kong
Politecnico di Milano, Piazza Leonardo da Vinci, 32-20133 Milan, Italy
ARPA-Lombardia, Viale Francesco Restelli, 3/1, 20124 Milan, Italy
currently at: University of Huelva (Spain) at the Izaña Atmospheric Observatory, INM-CSIC, La Marina 20, 6a planta, 38071, Santa Cruz de Tenerife, Canary Islands, Spain
A physicochemical characterization, including aerosol number size
distribution, chemical composition and mass concentrations, of the urban
fine aerosol captured in MILAN, BARCELONA and LONDON is presented in this
article. The objective is to obtain a comprehensive picture of the
microphysical processes involved in aerosol dynamics during the: 1) regular
evolution of the urban aerosol (daily, weekly and seasonal basis) and in the
day-to-day variations (from clean-air to pollution-events), and 2) the link
between "aerosol chemistry and mass concentrations" with the "number size
distribution".
<br><br>
The mass concentrations of the fine PM<sub>2.5</sub> aerosol exhibit a high correlation
with the number concentration of >100 nm particles N>100 (nm) ("accumulation mode particles")
which only account for <20% of the total number concentration N of fine
aerosols; but do not correlate with the number of <100 nm particles ("ultrafine particles"),
which accounts for >80% of fine particles number concentration.
Organic matter and black-carbon are the only aerosol components showing a
significant correlation with the ultrafine particles, attributed to vehicles
exhausts emissions; whereas ammonium-nitrate, ammonium-sulphate and also
organic matter and black-carbon correlate with N>100 (nm) and attributed to
condensation mechanisms, other particle growth processes and some primary
emissions. Time series of the aerosol DpN diameter (dN/dlogD mode), mass
PM<sub>2.5</sub> concentrations and number N>100 (nm) concentrations exhibit
correlated day-to-day variations, which point to a significant involvement
of condensation of semi-volatile compounds during urban pollution events.
This agrees with the observation that ammonium-nitrate is the component
exhibiting the highest increases from mid-to-high pollution episodes, when
the highest DpN increases are observed. The results indicates that "fine
PM<sub>2.5</sub> particles urban pollution events" tend to occur when condensation
processes have made particles grow large enough to produce significant
number concentrations of N>100 (nm) ("accumulation mode particles"). In
contrast, because the low contribution of ultrafine particles to the fine
aerosol mass concentrations, high "ultrafine particles N<100(nm) events"
frequently occurs under low PM<sub>2.5</sub> conditions. The results of this study
demonstrate that vehicles exhausts emissions are strongly involved in this
ultrafine particles aerosol pollution.
Alastuey, A., Querol, X., Rodríguez, S., Plana, F., Lopez-Soler, A., Ruiz, C., and Mantilla, E.: Monitoring of atmospheric particulate matter around sources of secondary inorganic aerosol, Atmos. Environ., 38, 4979–4992, 2004.
Cabada, J. C., Rees, S., Takahama, S., Khlystov, S. A., Pandis, S. N., Davidson, C. I., and Robinson, A. L.: Mass size distributions and size resolved chemical composition of fine particulate matter at the Pittsburgh supersite, Atmos. Environ., 38, 3127–3141, 2004.
Casati, R., Scheer, V., Vogt, R., and Benter, T.: Measurement of nucleation and soot mode particle emission from a diesel passenger car in real world and laboratory in situ dilution, Atmos. Environ., 41, 2125–2135, 2007.
Cao, J. J. Lee, S. C., Ho, K. F., Zou, S. C., Fung, K., Li, Y., Watson, J. G., and Chow, J. C.: Spatial and seasonal variations of atmospheric organic carbon and elemental carbon in Pearl River Delta Region, China, Atmos. Environ., 38, 4447–4456, 2004.
Gidhagen, L., Johansson, C., Langner, J., and Foltescu, V. L.: Urban scale modelling of particle number concentration in Stockholm, Atmos. Environ., 1711–1725, 2005.
Götschi, T., Hazenkamp-von Arx, M. E., Heinrichc, J., Bono, R., Burney, P., Forsberg, B., Jarvis, D., Maldonado, J., Norbäch, D., Stern, W. B., Sunyer, J., Torén, K., Verlato, G., Simona, V., and Künzl, N.: Elemental composition and reflectance of ambient fine particles at 21 European locations, Atmos. Environ., 39, 5947–5958, 2005.
Harris, J. S. and Maricq, M. M.: Signature size distributions for diesel and gasoline engine exhaust particulate matter, J. Aerosol Sci., 32, 749–764, 2001.
Hussein, T., Puustinen, A., Aalto, P. P., Mäkela, J. M., Hämeri, K., and Kulmala, M.: Urban aerosol number size distributions, Atmos. Chem. Phys., 4, 391–411, 2004.
IPCC, 2001: Climate Change 2001: The Scientific Basis, Cambridge University Press, 2001.
Janson, R., Rosman, K., Karlsson, A., and Hansson, H. C.: Biogenic emissions and gaseous precursors to forest aerosols, Tellus, Series B, Chemical and physical meteorology, 53, 423–440, 2001.
Jung, J. G., Adams, P. J., and Pandis, S. N.: Simulating the size distribution and chemical composition of ultrafine particles during nucleation events, Atmos. Environ., 40, 2248–2259, 2006.
Ketzel, M., Wåhlin, P., Kristensson, A., Swietlicki, E., Berkowicz, R., Nielsen, O. J., and Palmgren, F.: Particle size distribution and particle mass measurements at urban, near-city and rural level in the Copenhagen area and Southern Sweden, Atmos. Chem. Phys., 4, 281–292, 2004.
Kittelson, D. B.: Engines and nanoparticles: a review, J. Aerosol Sci., 29, 575–588, 1998.
Kulmala, M., Vehkamäki, H., Petäjä, T., Dal Maso, M., Lauri, A., Kerminen, V. M., Birmili, W., and McMurry, P. H.: Formation and growth rates of ultrafine atmospheric particles: a review of observations, J. Aerosol Sci., 35, 143–176, 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.
Millán, M. M., Sanz, M. J., Salvador, R., and Mantilla, E.: Atmospheric dynamics and ozone cycles related to nitrogen deposition in the western Mediterranean, Environ. Pollut., 118, 167–186, 2002.
Putaud, J. P., Raes, F., Van Dingenen, R., et al.: A European Aerosol Phenomenology. 2: physical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe, Atmos. Environ., 38, 2579–2595, 2004.
Querol, X., Alastuey, A., Rodriguez, S., Plana, F., Ruiz, C. R., Cots, N., Massague, G., and Puig, O.: PM$_10$ and PM$_2.5$ source apportionment in the Barcelona Metropolitan area, Catalonia, Spain, Atmos. Environ., 35, 6407–6419, 2001.
Querol, X., Alastuey, A., Ruiz, C. R., Artíñano, B., Hansson, H. C., Harrison, R. M., Buringh, E., ten Brink, H. M., Lutz, M., Bruckmann, P., Straehl, P., and Schneide, J.: Speciation and origin of PM$_10$ and PM$_2.5$ in selected European cities, Atmos. Environ., 38, 6547–6555, 2004.
Rodríguez, S., Van Dingenen, R., Putaud, J. P., Martins-Dos Santos, S., and Roselli, D.: Nucleation and growth of new particles in the rural atmosphere of Northern Italy – Relationship to Air Quality Monitoring, Atmos. Environ., 39, 6734–6746, 2005.
Rodríguez, S., Querol, X., Alastuey, A., and de la Rosa, J.: Atmospheric particulate matter and air quality in the Mediterranean: a review, Environ. Chem. Lett., 5, 1–7, doi:10.1007/s10311-006-0071-0, 2006.
Ruuskanen, J., Tuch, Th., Ten Brink, H., Peters, A., Khlystov, A., Mirme, A., Kos, G. P. A., Brunekreef, B., Wichmann, H. E., Buzorius, G., Vallius, M., Kreyling, W. G., and Pekkanen, J.: Concentrations of ultrafine, fine and PM$_2.5$ particles in three European cities, Atmos. Environ., 35, 3729–3738, 2001.
Sun, Q., Wang, A., Jin, X., Natanzon, A., Duquaine, D., Brook, R. D., Aguinaldo, J. G. S., Fayad, Z. A., Fuster, V., Lippman, M., Chen, L. C., and Rajagopalan, S.: Long-term Air Pollution Exposure and Acceleration of Atherosclerosis and Vascular Inflammation in an Animal Model, J. Amer. Medical Assoc., 294(23), 3003–3010, 2005.
Van Dingenen, R., Raes, F., Putaud, J. P., et al.: A European Aerosol Phenomenology. 1: physical characteristics of particulate matter at kerbside, urban, rural and background sites in Europe, Atmos. Environ., 38, 2561–2577, 2004.
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.
Wehner, B., Birmili, W., Gnauk, T., and Widensohler, A.: Particle number size distributions in a street canyon and their transformation into the urban-air background: measurements and a simple model study, Atmos. Environ., 36, 2215–2223, 2002.
Wehner, B. and Widensohler, A.: Long term measurements of submicron urban aerosols: statistical analysis for correlations with meteorological conditions and trace gases, Atmos. Chem. Phys., 3, 867–879, 2003.
WHO, World Health Organization: Health Aspects of Air Pollution with Particulate Matter, Ozone and Nitrogen Dioxide, Report on a WHO Working Group, Bonn, Germany, 13–15 January 2003.
Wichmann, H. E., Spix, C., Tuch, T., Wölke, G., Peters, A., Heinrich, J., Kreyling, G., and Heyder, J.: Daily mortality and fine and ultrafine particles in Erfurt, Germany. Part-I: Role of particle number and particle mass, Health Effects Institute, Research Report, number 98, November 2000.