Abstract
A 12 months study on urban atmospheric concentrations of polycyclic aromatic hydrocarbons (PAH) contained in the particulate matter with an aerodynamic diameter less than or equal to 10 microns (PM10) was carried out in Zaragoza (Spain) from July 12th, 2001 to July 26th, 2002 by using a high-volume air sampler able to collect the PAH supported on a Teflon-coated fibre glass filter. Samples were analysed by using Gas Chromatography Mass Spectrometry (GC-MS/MS). PAH of high molecular weight, indeno[1,2,3-cd]pyrene (IcdP), benzo[g,h,i]perylene (BghiP) and coronene (Co) were the most abundant compounds. The concentrations of benz[a]pyrene equivalent carcinogenic power (BaP-eq) showed a mean value of 0.7 ng/m3 with 22.5% of the samples exceeding the 1.0 ng/m3 guide value established by the European Directive. These episodes were mainly produced during cold season. Regarding meteorological variables, a positive effect of the prevalent wind “cierzo” (NW direction) over the Zaragoza city was confirmed from the environmental point of view. The NE, E and S directions, corresponding to highway and industrial areas were the directions showing the high PAH atmospheric concentrations. Despite the proximity of a high-level traffic highway, stationary sources related to industry were the dominant source of PAH in the sampled area. Vehicular emissions and natural gas home heating also contributed to PAH concentrations. The predominance of local pollution sources versus long-range transport on PAH concentrations was shown. However, the contribution of long-range transport of anthropogenic origin from other European areas was reflected for specific dates on PAH concentrations and PM10 levels.
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References
Ambient Air Pollution by PAH. Position Paper, July 27th 2001. Prepared by the Working Group on PAH.
Barrero Mazquiarán, M. A., & Cantón Ortiz de Pinedo, L. (2007). Organic composition of atmospheric urban aerosol: Variations and sources of aliphatic and polycyclic aromatic hydrocarbons. Atmospheric Research, 85(3–4), 288–299.
Borbély-Kiss, I., Kiss, A. Z., Koltay, E., Szabó, G., & Bozó, L. (2004). Saharan dust episodes in Hungarian aerosol: Elemental signatures and transport trajectories. Aerosol Science, 35, 1205–1224.
Caricchia, A. M., Chiavarini, S., & Pezza, M. (1999). Polycyclic aromatic hydrocarbons in the urban atmospheric particulate matter in the city of Naples (Italy). Atmospheric Environment, 33, 3731–3738.
Cecinato, A., Marino, F., Di Filippo, P., Lepore, L., & Possanzini, M. (1999). Distribution of n-alkanes, PAH and nitrates-PAH between the fine and coarse fractions of inhalable atmospheric particulates. Journal of Chromatography, 846, 255–264.
Constantino, J. P., Redmond, C. K., & Bearden, A. (1995). Occupationally related cancer risk among coke oven workers: 30 years of follow-up. Journal of Occupational and Environmental Medicine, 37, 597–604.
Daisey, J. M., Cheney, J. L., & Lioy, P. J. (1986). Profiles of organic particulate emissions from air pollution sources: status and need for receptor source apportionment modelling. Journal of Air Pollution & Control Association, 36, 17–33.
Daisey, J. M., Leyko, M. A., & Kneip, T. J. (1979). Polynuclear aromatic hydrocarbons. In: Ann Arbor Science Publishers, Ann Arbor, MI, p. 201.
Dallarosa, J. B., Monego, J. G., Teixeira, E. C., Stefens, J. L., & Wiegand, F. (2005b). PAH in atmospheric particles in the metropolitan area of Porto Alegre, Brazil. Atmospheric Environment, 39, 1609–1625.
Dallarosa, J. B., Teixeira, E. C., Pires, M., & Fachel, J. (2005a). Study of the profile of PAHs in atmospheric particles PM10 using multivariate methods. Atmospheric Environment, 39, 6587–6596.
Dickhut, R. M., & Gustafson, K. E. (1997). Particle/gas concentrations and distributions of PAHs in the atmosphere of southern Chesapeake Bay. Environmental Science& Technology, 31(1), 140–147.
Dimashki, M., Lim, M. H., Harrison, R. M., & Harrad, S. (2001). Temporal trends, temperature dependence and relative reactivity of atmospheric PAH. Environmental Science & Technology, 35, 2264–2267.
Ding, X., Wang, X.-M., Xie, Z.-Q., Xiang, C.-H., Mai, B. X., Sun, L.-G., et al. (2007). Atmospheric PAH observed over the North Pacific Ocean and the Arctic area: Spatial distribution and source identification. Atmospheric Environment, 41, 2061–2072.
Directive 1999/30/EC of 22 April 1999 relating to limit values for sulphur dioxide, nitrogen dioxide and oxides of nitrogen, particulate matter and lead in ambient air. (1999), OJL 163, 29.6.1999, p.41.
Directive 2004/107/EC of the European Parliament and of the Council of 15 December 2004 relating to arsenic, cadmium, mercury, nickel and PAH in ambient air.
Duval, M. M., & Friedlander, S. K. (1981). Source resolution of PAH in the Los Angeles atmosphere. Application of a CMB with first order decay. Technical Report No. EPA 600/2-81-161, US Government Printing Office, Washington DC, USA.
Gogou, A., Stratigakis, N., Kanakidou, M., & Stephanou, E. G. (1996). Organic aerosols in Eastern Mediterranean: components source reconciliation by using molecular markers and atmospheric back trajectories. Organic Geochemistry, 25, 79–96.
Gutiérrez-Dabán, A., Fernández-Espinosa, A. J., Ternero-Rodríguez, M., & Fernández-Alvarez, F. (2005). Particle size distribution of PAH in urban air in southern Spain. Analytical and Bioanalytical Chemistry, 381, 721–736.
Halsall, C. J., Sweetman, A. J., Barrie, L. A., & Jones, K. C. (2001). Modeling the behavior of PAHs during atmospheric transport from UK to the Artic. Atmospheric Environment, 35, 255–267.
Harkov, R., & Greenberg, A. (1985). BaP in New Hersey results from a 27 site study. Journal of Air Pollution & Control Association, 35, 238–243.
Harrison, R. M., Smith, D. J. T., & Luhana, L. (1996). Source apportionment of atmospheric PAH collected from an urban location in Birmingham, UK. Environmental Science & Technology, 30, 825–832.
HYSPLIT 4, (Hybrid Single-Particle Lagrangian Integrated Trajectory) Model (1997). NOAA Air Resources Laboratory, Silver Spring, MD. from http://www.arl.noaa.gov/ready/hysp_info.html.
Karar, K., & Gupta, A. K. (2006). Seasonal variations and chemical characterization of ambient PM10 at residencial and industrial sites o fan urban region of Kolkata (Calcuta), India. Atmospheric Research, 84(1), 30–41.
Khalili, N. R., Scheff, P. A., & Holsen, T. M. (1995). PAH source fingerprints for coke ovens, diesel and gasoline engines, highway tunnels and wood combustion emissions. Atmospheric Environment, 33, 4977–4986.
Kulkarni, K., & Venkataraman, C. (2000). Atmospheric polycyclic aromatic hydrocarbons in Mumbai, India. Atmospheric Environment, 34(17), 2785–2790.
Larsen, J. C., & Larsen, P. B. (1998). Chemical carcinogens. In R. E. Hester, & R. M. Harrison (Eds.) Air pollution and health (pp. 33–56). Cambridge: The Royal Society of Chemistry.
Lee, M. L., Prado, G. P., Howard, J. B., & Hites, R. A. (1977). Source identification of urban airborne PAH by gas chromatographic mass spectrometry and high resolution mass spectrometry. Biomedical Mass Spectrometry, 4, 182–186.
Li, C. K., & Kamens, R. M. (1993). The use of PAH as source signatures in receptor modeling. Atmospheric Environment, 27A, 523–532.
Lim, L. H., Harrison, R. M., & Harrad, S. (1999). The contribution of traffic to atmospheric concentrations of PAH. Environmental Science & Technology, 33, 3538–3542.
López, J. M., Callén, M. S., Murillo, R., García, T., Navarro, M. V., de la Cruz, M. T., et al. (2005). Levels of selected metals in ambient air PM10 in an urban site of Zaragoza (Spain). Environmental Research, 99, 58–67.
Mantis, J., Chaloulakou, A., & Samara, C. (2005). PM10-bound PAH in the Greater Area of Athens, Greece. Chemosphere, 59, 593–604.
Marino, F., Cecinato, A., & Siskos, P. (2000). Nitro-PAH in ambient particulate matter in the atmosphere of Athens. Chemosphere, 40, 533–537.
Masclet, P., Bresson, M. A., & Mouvier, G. (1987). PAH emitted by power stations, and influence of combustion conditions. Fuel, 66, 556–562.
Mastral, A., & Callén, M. S. (2000). A review on PAH emissions from energy generation. Environmental Science & Technology, 34(15), 3051–3057.
Mastral, A., López, J. M., Callén, M. S., García, T., Murillo, T., & Navarro, M. V. (2003). Spatial and temporal evolution of atmospheric PAH concentration in Zaragoza, Spain. Science of the Total Environment, 307, 111–124.
Nielsen, T. (1996). Traffic contribution of PAH in the centre of a large city. Atmospheric Environment, 20, 3481–90.
Park, S. S., Kim, Y. J., & Kang, C. H. (2002). Atmospheric PAH in Seoul, Korea. Atmospheric Environment, 36, 2917–2924.
Pott, P. (1962). Chirurgical observations relative to the cataract, the polypus of the nose, the cancer of the scrotum, the different kinds of ruptures, and the mortification of the toes and feet. London, England, Hawes, Clark & Collins, 1775, In: National Cancer Institute Monograph, 1962, pp 7–13.
Prevedouros, K., Jones, K. C., & Sweetman, A. J. (2004). Modeling the atmospheric fate and seasonality of polycyclic aromatic hydrocarbons in the UK. Chemosphere, 56, 195–208.
Rogge, W. F., Hildemann, L. M., Mazurek, M. A., Cass, G. R., & Simoneit, B. R. T. (1993). Sources of fine organic aerosol:2. Non-catalyst and catalyst equipped automobiles and heavy duty diesel trucks. Environmental Science & Technology, 27, 636–651.
Salvador, P. (2004). Caracterización de la contaminación atmosférica producida por partículas en suspensión en Madrid. Thesis, University of Madrid.
Schulte, A., Ernst, H., Peters, L., & Heinrich, U. (1994). Induction of squamous-cell carcinomas in the mouse lung after long-term inhalation of PAH rich exhausts. Experimental and Toxicologic Pathology, 45(7), 415–421.
Simcik, M. F., Eisenreich, S. J., & Lioy, P. J. (1999). Source apportionment and source/sink relationships of PAHs in the coastal atmosphere of Chicago and Lake Michigan. Atmospheric Environment, 33, 5071–5079.
Simo, R., Grimalt, J. O., & Albaiges, J. (1997). Background levels of atmospheric hydrocarbons, sulphate and nitrate over the western Mediterranean. Environmental Science & Technology, 31, 2697–2700.
Smith, D. J. T., Harrison, R. M., Luhana, L., Pio, C. A., Castro, L. M., Tariq, M. N., et al. (1996). Concentrations of particulate airborne PAH and metals collected in Lahore, Pakistan. Atmospheric Environment, 30(23), 4031–4040.
Tolosa, I., Bayona, J. M., & Albaiges, J. (1996). Aliphatic and PAH and sulphur oxygen derivatives in northwestern Mediterranean sediments: Spatial and temporal variability, fluxes, budgets. Environmental Science & Technology, 30, 2495–2503.
Van der Wal, J. T., & Janssen, L. H. J. M. (2000). Analysis of spatial and temporal variation of PM10 concentrations in the Netherlands using Kalman filtering. Atmospheric Environment, 34, 3675–3687.
Venkataraman, C., & Friedlander, S. K. (1994). Source resolution of fine particulate PAH using a receptor model modified for reactivity. Journal of the Air & Waste Management Association, 44, 1103–1108.
Yassaa, N., Meklati, B. Y., Cecinato, A., & Marino, F. (2001). Particulate n-alkanes, n-alkanoic acids and PAH in the atmosphere of Algiers City Area. Atmospheric Environment, 35, 1843–1851.
Acknowledgments
Authors would like to thank the Spanish National Institute of Meteorology, for the Zaragoza meteorological data and the Government of Aragon (D.G.A. Spain) for the grant to M.T. de la Cruz.
We also acknowledge the NASA for the Earth Probe TOMS maps and satellite images; the NOAA Air Data Resources Laboratory and the Australia’s Bureau of Meteorology for the HYSPLIT model, the synoptic charts of pressure and the FLN meteorological data set.
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Callén, M.S., de la Cruz, M.T., López, J.M. et al. Long-Range Atmospheric Transport and Local Pollution Sources on PAH Concentrations in a South European Urban Area. Fulfilling of the European Directive. Water Air Soil Pollut 190, 271–285 (2008). https://doi.org/10.1007/s11270-007-9599-2
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DOI: https://doi.org/10.1007/s11270-007-9599-2