Abstract
Ambient concentrations of polycyclic aromatic hydrocarbons (PAHs) were measured in Helsinki (Finland). Particle mass size distributions were obtained with a cascade impactor (12 stages) with glass fibre filters as substrates. Simultaneously with the impactor measurements, particulate and gaseous PAHs were collected on a quartz filter and XAD-2 adsorbent, respectively, for evaluation of gas-partition coefficients. Samples were analysed for PAHs by on-line coupled supercritical fluid extraction — liquid chromatography — gas chromatography — mass spectrometry. The impactor results showed that most of the PAHs in Helsinki urban area were concentrated in fine particles (<2.5 μm diameter) with unimode peak at about 1 μm. The results were comparable with the number distribution measured with a differential mobility particle sizer. Total amounts of PAHs (gas + particle) varied from 15 (acenaphthylene) to 1990 (fluorene) pg/m3. The PAHs lighter than 202 amu (pyrene and fluoranthene) were exclusively in gas phase, whereas those heavier than 202 amu were mostly associated with particles. A plot of the partition coefficients (logKp) versus the temperature dependent sub-cooled vapour pressures (logp 0L ) showed a gradient of −0.66, which deviated from equilibrium state (gradient = −1).
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Allen, J. O., Dookeran, N. M., Smith, K. A., Sarofim, A. F., Taghizadeh, K., and Lafleur, A. L., 1996: Measurement of polycyclic aromatic hydrocarbons associated with size-segregated atmospheric aerosols in Massachusetts, Environ. Sci. Technol. 30(3), 1023–1031.
Alves, C. A., Pio, C. A., and Duarte, A. C., 2000: Particulate size distributed organic compounds in a forest atmosphere, Environ. Sci. Technol. 34(20), 4287–4293.
Buehler, S. S., Basu, I., and Hites, R. A., 2001: A comparison of PAH, PCB, and pesticide concentrations in air at two rural site on Lake Superior, Environ. Sci. Tecchnol. 35(12), 2417–2422.
Bøwadt, S. and Hawthorne, S. B., 1995: Supercritical fluid extraction in environmental analysis, J. Chromatogr. A 703(1+2), 549–571.
Cecinato, A., Marino, F., Di Filippo, P., Lepore, L., and Possanzini, M., 1999: Distribution of nalkanes, polynuclear aromatic hydrocarbons and nitrated polynuclear aromatic hydrocarbons between the fine and coarse fractions of inhalable atmospheric particulates, J. Chromatogr. A 846(1+2), 255–264.
Chester, T. L., Pinkiston, J. D., and Raynie, D. E., 1998: Supercritical fluid chromatography and extraction, Anal. Chem. 70(12), 301–319.
Dachs, J. D. and Eisenreich, S. J., 2000: Adsorption onto aerosol soot carbon dominates gas-particle partitioning of polycyclic aromatic hydrocarbons, Environ. Sci. Technol. 34(17), 3690–3697.
Didyk, B. M., Simoneit, B. R. T., Pezoa, L. A., Riveros, M. L., and Flores, A. A., 2000: Urban aerosol particle of Santiago, Chile: organic contents and molecular characterization, Atmos. Environ. 34(8), 1167–1179.
European Commission, 2001: Ambient air pollution by polycyclic aromatic hydrocarbons (PAH), Position Paper, Luxembourg.
Fernández, P., Grimalt, J. O., and Vilanova, R. M., 2002: Atmospheric gas-particle partitioning of polycyclic aromatic hydrocarbons in high mountain regions of Europe, Environ. Sci. Technol. 36(6), 1162–1168.
Finlayson-Pitts, B. J. and Pitts, J. N. Jr., 1999: Chemistry of the Upper and Lower Atmosphere: Theory, Experiments, and Applications, Academic Press, California, pp. 21–23.
Garivait, H., Polprasert, C., Yoshizumi, K., and Reutergardh, L. B., 1999: Airborne polycyclic aromatic hydrocarbons (PAH) in Bangkok urban air I. Characterization and quantification, Polycyclic Aromat. Compd. 13, 313–327.
Garivait, H., Polprasert, C., Yoshizumi, K., and Reutergardh, L. B., 2001: Airborne polycyclic aromatic hydrocarbons (PAH) in Bangkok urban air II. Level and distribution, Polycyclic Aromat. Compd. 18, 325–350.
Gigliotti, C. L., Dachs, J., Nelson, E. D., Brunciak, P. A., and Eisenreich, S. J., 2000: Polycyclic aromatic hydrocarbons in the New Jersey coastal atmosphere, Environ. Sci. Technol. 34(17), 3547–3554.
Goss, K-W. and Schwarzenbach, R. P., 1998: Gas/solid and gas/liquid partitioning of organic components: Critical evaluation of the interpretation of equilibrium constants, Environ. Sci. Technol. 32(14), 2025–2032.
Harrison, R. M., Smith, D. J. T., and Luhana, L., 1996: Source appointment of atmospheric polycyclic aromatic hydrocarbons collected from an urban location in Birmingham, U.K., Environ. Sci. Technol. 30(3), 825–832.
Hartonen, K., Bøwadt, S., Hawthorne, S., and Riekkola, M.-L., 1997: Supercritical fluid extraction with solid-phase trapping of chlorinated and brominated pollutants from sediment samples, J. Chromatogr. A 774, 229–242.
Hillamo, R. E. and Kauppinen, E. I., 1991: On the performance of the Berner low pressure impactor, Aerosol Sci. Technol. 14(1), 33–47.
Hinds, W. C., 1982: Aerosol Technology, Wiley, New York, p. 122.
Hyötyläinen, T. and Riekkola, M.-L., 2001: Potential of on-line coupled liquid chromatography-gas chromatography in the analysis of complex samples, Recent Res. Devel. Anal. Chem. 1, 21–43.
Kaupp, H. and McLachlan, M.S., 1999: Atmospheric particle size distributions of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polucyclic aromatic hydrocarbons (PAHs) and their implications for wet and dry deposition, Atmos. Environ. 33(1), 85–95.
Kaupp, H. and McLachlan, M. S., 2000: Distribution of polychlorinated dibenzo-P-dioxins and fibenzofurans (PCDD/Fs) and polycyclic aromatic hydrocarbons (PAHs) within the full size range of atmospheric particles, Atmos. Environ. 34(1) 73–83.
Kirchstetter, T. W., Corrigan, C. E., and Novakov, T., 2001: Laboratory and field investigation of the adsorption of gaseous organic compounds onto quartz filters, Atmos. Environ. 35(9), 1663–1671.
Kiss, G., Puchony-Varga, Z., Tolnai, B., Varga, B., Gelencśer, A., Krivácsy, Z., and Hlavay, J., 2001: The seasonal changes in the concentration of polycyclic aromatic hydrocarbons in precipitation and arosol near Lake Balaton, Hungary, Environ. Pollut. 114, 55–61.
Lim, L. H., Harrison, R. M., and Harrad, S., 1999: The concentration of traffic to atmospheric concentrations of polycyclic aromatic hydrocarbons, Environ. Sci. Technol. 33(20), 3538–3542.
Lohmann, R., Harner, T., Thomas, G. O., and Jones, K. C., 2000: A comparative study of the gas-particle partitioning of PCDD/Fs, PCBs, and PAHs, Environ. Sci. Technol. 34(23), 4943–4951.
Mader, B. T. and Pankow, J. F., 2000: Gas/solid partitioning of semivolatile organic compounds (SOCs) to air filters. 1. Partitioning of polychlorinated dibenzodioxins, polychlorinated dibenzofurans and polycyclic aromatic hydrocarbons to Teflon membrane filters, Atmos. Environ. 34(28), 4879–4887.
Mader, B. T. and Pankow, J.F., 2001a: Gas/solid partitioning of semivolatile organic compounds (SOCs) to air filters. 2. Partitioning of polychlorinated dibenzodioxins, polychlorinated dibenzofurans, and polycyclic aromatic hydrocarbons to quartz fiber filters, Atmos. Environ. 35(7), 1217–1223.
Mader, B. T. and Pankow, J. F., 2001b: Gas/solid partitioning of semivolatile organic compounds (SOCs) to air filters. 3. An analysis of gas adsorption artifacts in measurements of atmospheric SOCs and organic carbon (OC). When using teflon membrane filters and quartz fiber filters, Environ. Sci. Technol. 35(17), 3422–3432.
Mészáros, E., Barcza, T., Gelencsér, A., Hlavay, J., Kiss, G., Krivácsy, Z., Molnár, A., and Polyák, K., 1997: Size distributions of inorganic and organic species in the atmospheric aerosol in Hungary, J. Aerosol Sci. 28(7), 1163–1175.
Mondello, L., Dugo, P., Dugo, G., Lewis, A. C., and Bartle, K. D., 1999: High-performance liquid chromatography coupled on-line with high resolution gas chromatography. State of the art, J. Chromatogr. A. 842(1+2), 373–390.
Offenberg, J. H. and Baker, J. E., 1999: Aerosol size distributions of polycyclic aromatic hydrocarbons in urban and over-water atmosphere, Environ. Sci. Technol. 33(19), 3324–3331.
Offenberg, J. H. and Baker, J. E., 2000: The influence of aerosol size and organic carbon content on gas/particle partitioning of polycyclic aromatic hydrocarbons (PAHs), Atmos. Environ. 36(7), 1205–1220.
Peters, A. J., Lane, D. A., Gundel, L. A., Northcott, G. L., and Jones, K. C., 2000: A comparison of high volume and diffusion denuder samplers for measuring demivolatile organic compounds in the atmosphere, Environ. Sci. Technol. 34(23), 5001–5006.
Pio, C., Aves, C., and Duarte, A., 2001: Organic components of aerosols in a forested area of central Greece, Atmos. Environ. 35(2), 389–401.
Sanusi, A., Millet, M., Mirabel, P., and Wortham, H., 1999: Gas-particle partitioning of pesticides in atmospheric samples, Atmos. Environ. 33(29), 4941–4951.
Seinfeld, J. H. and Pandis, S. N., 1998: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, Wiley, New York, p. 426.
Sheu, H.-L., Lee, W.-J., Lin, S. J., Fang, G.-C., Chang, H.-C., and You, W.-C., 1997: Particle-bound PAH contents in ambient air, Environ. Pollut. 96(3), 369–382.
Shimmo, M., Hyötyläinen, T., Hartonen, K., and Riekkola, M.-L., 2001: On-line coupled supercritical fluid extraction-liquid chromatography-gas chromatography-mass spectrometry for the analysis of organic acids, J. Microcol. Sep. 13(5), 202–210.
Shimmo, M., Adler, H., Hyötyläinen, T., Hartonen, K., Kulmala, M., and Riekkola, M.-L., 2002: Analysis of particulate polycyclic aromatic hydrocarbons by on-line coupled supercritical fluid extraction-liquid chromatography-gas chromatography-mass spectrometry, Atmos. Environ. 36(18), 2985–2995.
Simcik, M. F., Franz, T.P., Zhang, H., and Eisenreich, S. J., 1998: Gas-particle partitioning of PCBs and PAHs in the Chicago urban and adjacent coastal atmosphere: States of equilibrium, Environ. Sci. Technol. 32(2), 251–257.
Sugiyama, T., Amagai, T., Matsushita, H., and Soma, M., 1999: Size distribution of indoor airborne particulates collected by a low, Indoor Built. Environ. 8, 361–369.
Tsai, P.-J., Shieh, H.-Y., Lee, W.-J., and Lai, S.-O., 2001: Health-risk assessment for workers exposed to polycyclic aromatic hydrocarbons (PAHs) in a carbon black manufacturing industry, Sci. Total. Environ. 278, 137–150.
Turpin, B. J., Saxena, P., and Andrews, E., 2000: Measuring and simulating particulate organics in the atmosphere: problems and prospects, Atmos. Environ 34(18), 2983–3013.
U.S. Environment Protection Agency, 1986: Modified method 5 sample train, Method 0010.
U.S. Environment Protection Agency, 1997: Determination of polycyclic aromatic hydrocarbons in ambient air using gas chromatography/mass spectrometry, Compendium method TO-13A.
Venkataraman, C., Thomas, S., and Kulkarni, P., 1999: Size distribution of polycyclic aromatic hydrocarbons — gas/particle partitioning to urban aerosols J. Aerosol Sci. 30(6), 759–770.
World Health Organization, 2000: Air Quality Guidelines for Europe, WHO European Series, WHO Regional Bureau, Copenhagen.
Yamasaki, H., Kuwata, K., and Kuge, Y., 1984, Determination of vapor pressure of polycyclic aromatic hyderocarbons in the supercooled liquid phase and their adsorption on airborne particulate matter, Nippon Kagaku Kaishi 8, 1324–1329.
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Shimmo, M., Saarnio, K., Aalto, P. et al. Particle Size Distribution and Gas-Particle Partition of Polycyclic Aromatic Hydrocarbons in Helsinki Urban Area. Journal of Atmospheric Chemistry 47, 223–241 (2004). https://doi.org/10.1023/B:JOCH.0000021088.37771.f7
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DOI: https://doi.org/10.1023/B:JOCH.0000021088.37771.f7