Abstract
Atmospheric particulate matter (PM) abundance, mass size distribution (MSD) and chemical composition are parameters relevant for human health effects. The MSD and phase state of semivolatile organic pollutants were determined at various polluted sites in addition to the PM composition and MSD. The distribution pattern of pollutants varied from side to side in correspondence to main particle sources and PM composition. Levels of particle-associated polycyclic aromatic hydrocarbons (PAHs) were 1–30 ng m−3 (corresponding to 15–35 % of the total, i.e., gas and particulate phase concentrations), of polychlorinated biphenyls (PCBs) were 2–11 pg m−3 (4–26 % of the total) and of DDT compounds were 2–12 pg m−3 (4–23 % of the total). The PM associated amounts of other organochlorine pesticides were too low for quantification. The organics were preferentially found associated with particles <0.45 μm of aerodynamic equivalent diameter. The mass fractions associated with sub-micrometer particles (PM0.95) were 73–90 %, 34–71 % and 36–81 % for PAHs, PCBs and DDT compounds, respectively. The finest particles fraction had the highest aerosol surface concentration (6.3–29.7)×10−6 cm−1 (44–70 % of the surface concentration of all size fractions). The data set was used to test gas-particle partitioning models for semivolatile organics for the first time in terms of the organics' MSD and size-dependent PM composition. The results of this study prove that at the various sites particles with diverse size, matrix composition, amount of contaminants and toxicological effects occur. Legislative regulation based on gravimetric determination of PM mass can clearly be insufficient for assessment.
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References
Arp HPH, Schwarzenbach RP, Goss KU (2008) Ambient gas/particle partitioning: 1. Sorption mechanisms of apolar, polar, and ionizable organic compounds. Environ Sci Technol 42:5541–5547
Balasubramanian R, He J (2010) Fate and transfer of persistent organic pollutants in a multi-media environment. In: Zereini F, Wiseman CLS (eds) Urban airborne particulate matter: origins, chemistry, fate and health impacts. Springer, Berlin, Germany, pp 277–307
Bartoš T, Čupr P, Klánová J, Holoubek I (2009) Which compounds are most responsible for elevated human health risks in the Western Balkans? Environ Int 35:1066–1071
Bidleman TF (1988) Atmospheric processes. Environ Sci Technol 22:361–367
Borm PJA, Robbins D, Haubold S, Kuhlbusch T, Fissan H, Donaldson K, Schins R, Stone V, Kreyling W, Lademann J, Krutmann J, Warheit D, Oberdörster E (2006) The potential risks of nanomaterials: a review carried out for ECETOC. Part Fibre Toxicol 3:11–45
Brantley SL, Mellott NP (2000) Surface area and porosity of primary silicate minerals. Am Mineral 85:1767–1783
Brüggemann E, Gerwig H, Gnauk T, Müller K, Herrmann H (2009) Influence of seasons, air mass origin and day of the week on size-segregated chemical composition of aerosol particles at a kerbside. Atmos Environ 43:2456–2463
Chrysikou LP, Gemenetzis PG, Samara CA (2009) Wintertime size distributions of polycyclic aromatic hydrocarbons (PAH), polychlorinated biphenyls (PCB) and organochlorine pesticides (OCPs) in the urban environment: street- vs. rooftop-level measurements. Atmos Environ 43:290–300
Covert DS, Heintzenberg J (1984) Measurements of the degree of internal/external mixing of hygroscopic compounds and soot in atmospheric aerosols. Sci Total Environ 36:347–352
Čupr P, Flegrová Z, Franců J, Landlová L, Klánová J (2013) Mineralogical, chemical and toxicological characterization of urban air particles. Environ Int 54:26–34
Dachs J, Eisenreich SJ (2000) Adsorption onto aerosol soot carbon dominates gas-particle partitioning of polycyclic aromatic hydrocarbons. Environ Sci Technol 34:3690–3697
de Kok TMCM, Driece HAL, Hogervorst JGF, Briedé JJ (2006) Toxicological assessment of ambient and traffic-related particulate matter: a review of recent studies. Mutat Res 613:103–122
Dvorská A, Lammel G, Holoubek I (2009) Recent trends of persistent organic pollutants in air in Central Europe – air monitoring in combination with air mass trajectory statistics as a tool to study the effectivity of regional chemical policy. Atmos Environ 43:1280–1287
ECS (2012) European Committee for Standardization: Sludge, treated biowaste, soil and waste – Determination of total organic carbon (TOC) by dry combustion. ICS 13.030.01, EN 15936:2012:E, Brussels
Erdinger L, Dürr M, Höpker KA (2005) Correlations between mutagenic activity of organic extracts of airborne particulate matter, NO x , and sulphur dioxide in southern Germany – results of a two-year study. Environ Sci Pollut Res 12:10–20
EU (2007) Regulation on type approval of motor vehicles with respect to emissions from light passenger and commercial vehicles (Euro 5 and Euro 6) and on access to vehicle repair and maintenance information, No. 715/2007, European Parliament and Council, 20 June 2007, Brussels
EU (2008) Air Quality Directive 2008/50/EC, Guidance on the quantification of the contribution of natural sources under the EU Air Quality Directive, European Commission, DG Environment, Office J Eur Union 11.6.2008, L152, 44 pp., Brussels
Finizio A, Mackay D, Bidleman T, Harner T (1997) Octanol–air partition coefficient as a predictor of partitioning of semi-volatile organic chemicals to aerosols. Atmos Environ 31:2289–2296
Finlayson-Pitts BJ, Pitts JN (2000) Chemistry of the upper and lower atmosphere: theory, experiments, application. Academic Press, San Diego
Gill PS, Graedel TE, Weschler CJ (1983) Organic films on atmospheric aerosol particles, fog droplets, cloud droplets, raindrops, and snowflakes. Rev Geophys Space Phys 21:903–920
Goss KU, Schwarzenbach RP (2001) Linear free energy relationships used to evaluate equilibrium partitioning of organic compounds. Environ Sci Technol 35:1–9
Grosjean D, Fung K, Harrison J (1983) Interactions of polycyclic aromatic hydrocarbons with atmospheric pollutants. Environ Sci Technol 17:673–679
Gundel L, Daisey JM, de Carvalho LRF, Kado NY, Schuetzle D (1993) Polar organic matter in airborne particles: chemical characterization and mutagenic activity. Environ Sci Technol 27:2112–2119
Harner T, Bidleman TF (1998) Octanol–air partition coefficient for describing particle/gas partitioning of organic compounds in urban air. Environ Sci Technol 32:1494–1502
Heal MR, Kumar P, Harrison RM (2012) Particles, air quality, policy and health. Chem Soc Rev 41:6606–6630
Holoubek I, Klánová J, Jarkovský J, Kohoutek J (2007) Assessment of the Central European trends in the background levels of persistent organic pollutants based on the results of the long-term integrated monitoring in Kosetice observatory. Czech Republic: Part I. Ambient air and wet deposition 1988–2005. J Environ Monit 9:557–563
Horvath H, Kasahara M, Pesava P (1996) The size distribution and composition of the atmospheric aerosol at a rural and nearby urban location. J Aerosol Sci 27:417–435
ICDD (2012) PDF-4/Minerals, power diffraction file database. International Centre for Diffraction Data, Newtown Square, USA, ISSN 1534–7672 (CD-ROM)
Invernizzi G, Boffi R, Ruprecht AA, Barnes PJ, Kharitonov SA, Paredi P (2006) Real-time measurement of particulate matter deposition in the lung. Biomarkers 11:221–232
Jacobson MC, Hansson HC, Noone KJ, Charlson RJ (2000) Organic atmospheric aerosols: review and state of the science. Rev Geophys 38:267–294
Jaenicke R (1988) Aerosol physics and chemistry. Landolt-Börnstein Neue Ser 4b:391–457
Junge CE (1977) Basic considerations about trace constituents in the atmosphere as related to the fate of global pollutants. In: Suffet IH (ed) Fate of Pollutants in the Air and Water Environments, Part I. Wiley, New York, pp 7–26
Kawanaka Y, Tsuchiya Y, Yun SJ, Sakamoto K (2009) Size distributions of polycyclic aromatic hydrocarbons in the atmosphere and estimation of the contribution of ultrafine particles to their lung deposition. Environ Sci Technol 43:6851–6856
Keyte IJ, Harrison RM, Lammel G (2013) Chemical reactivity and long-range transport potential of polycyclic aromatic hydrocarbons – a review. Chem Soc Rev 42:9333–9391
Kiss G, Varga-Puchovny Z, Rohrbacher G, Hlavay J (1998) Distribution of polycyclic aromatic hydrocarbons on atmospheric aerosol particles of different sizes. Atmos Res 46:253–261.
Klánová J, Kohoutek J, Čupr P, Holoubek I (2007) Are the residents of former Yugoslavia still exposed to elevated PCB levels due to the Balkan wars?: Part 2. Passive air sampling network. Environ Int 33:727–735
Kroll JH, Seinfeld JH (2008) Chemistry of secondary organic aerosol: formation and evolution of low-volatility organics in the atmosphere. Atmos Environ 42:3592–3624
Lammel G, Leip A (2005) Formation of nitrate and sulfate in the plume of Berlin. Environ Sci Pollut Res 12:213–220
Lammel G, Brüggemann E, Gnauk T, Müller K, Neusüss C, Röhrl A (2003) A new method to study aerosol source contributions along the tracts of air parcels and its application to the near-ground level aerosol chemical composition in central Europe. J Aerosol Sci 34:1–25
Lammel G, Sehili AM, Bond TC, Feichter J, Grassl H (2009) Gas/particle partitioning and global distribution of polycyclic aromatic hydrocarbons – a modelling approach. Chemosphere 76:98–106
Lammel G, Klánová J, Ilić P, Kohoutek J, Gasić B, Kovacić I, Lakić N, Radić R (2010a) Polycyclic aromatic hydrocarbons on small spatial and temporal scales – I. Levels and variabilities. Atmos Environ 44:5015–5021
Lammel G, Klánová J, Ilić P, Kohoutek J, Gasić B, Kovacić I, Škrdlíková L (2010b) Polycyclic aromatic hydrocarbons on small spatial and temporal scales – II. Mass size distributions and gas-particle partitioning. Atmos Environ 44:5022–5027
Lammel G, Novák J, Landlová L, Dvorská A, Klánová J, Čupr P, Kohoutek J, Reimer E, Škrdlíková L (2010c) Sources and distributions of polycyclic aromatic hydrocarbons and toxicity of polluted atmosphere aerosols. In: Zereini F, Wiseman CLS (eds) Urban airborne particulate matter: origins, chemistry, fate and health impacts. Springer, Berlin, pp 39–62
Lammel G, Klánová J, Erić L, Ilić P, Kohoutek J, Kovacić I (2011) Sources of organochlorine pesticides in an urban Mediterranean environment: volatilisation from soil. J Environ Monit 13:3358–3364
Lohmann R, Lammel G (2004) Adsorptive and absorptive contributions to the gas particle partitioning of polycyclic aromatic hydrocarbons: state of knowledge and recommended parameterisation for modelling. Environ Sci Technol 38:3793–3803
Meunier A (2005) Clays. Springer, Berlin, 472 pp
Mikhailov E, Vlasenko S, Martin ST, Koop T, Pöschl U (2009) Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations. Atmos Chem Phys 9:9491–9522
Monarca S, Crebelli R, Feretti D, Zanardini A, Fuselli S, Filini L, Resola S, Bonardelli PG, Nardi G (1997) Mutagens and carcinogens in size-classified air particulates of a northern Italian town. Sci Total Environ 205:137–144
Nenes A, Pilinis C, Seinfeld JH (1998) ISORROPIA — a new thermodynamic model for multiphase multicomponent inorganic aerosols. Aquat Geochem 4:123–152
Novák J, Hilscherová K, Landlová L, Čupr P, Kohút L, Giesy JP, Klánová J (2013) Composition and effects of inhalable size fractions of atmospheric aerosols in the polluted atmosphere: Part II. In vitro biological potencies. Environ Int 63:64–70
Pankow JF (1987) Review and comparative analysis of the theory of partitioning between the gas and aerosol particulate phases in the atmosphere. Atmos Environ 21:2275–2283
Pankow JF (1994) An absorption model of gas-particle partitioning of organic compounds in the atmosphere. Atmos Environ 28:185–188
Pankow JF, Bidleman TF (1992) Interdependence of the slopes and intercepts from log–log correlations of measured gas particle partitioning and vapor-pressure: 1. Theory and analysis of available data. Atmos Environ 26:1071–1080
Putaud JP, van Dingenen R, Alastuey A, Bauer H, Birmili W, Cyrys J, Flentje H, Fuzzi S, Gehrig R, Hansson HC, Harrison RM, Herrmann H, Hitzenberger R, Hüglin C, Jones AM, Kasper-Giebl A, Kiss G, Kousa A, Kuhlbusch TAJ, Löschau G, Maenhaut W, Molnar A, Moreno T, Pekkanen J, Perrino C, Pitz M, Puxbaum H, Querol X, Rodriguez S, Salma I, Schwarz J, Smolik J, Schneider J, Spindler G, ten Brink H, Tursic J, Viana M, Wiedensohler A, Raes F (2010) A European aerosol phenomenology – 3. Physical and chemical characteristics of particulate matter from 60 rural, urban, and kerbside sites across Europe. Atmos Environ 44:1308–1320
Radonić J, Turk Sekulić M, Vojinović MM, Čupr P, Klánová J (2009) Gas–particle partitioning of persistent organic pollutants in the Western Balkan countries affected by war conflicts. Environ Sci Pollut Res 16:65–72
Raes F, van Dingenen R, Vignati E, Wilson J, Putaud JP, Seinfeld JH, Adams P (2000) Formation and cycling of aerosols in the global troposphere. Atmos Environ 34:4215–4240
Rancourt DG, Dang MZ (2005) Absolute quantification by powder X-ray diffraction of complex mixtures of crystalline and amorphous phases for applications in the Earth sciences. Am Mineral 90:1571–1586
Ringuet J, Leoz-Garciandia E, Budzinski H, Villenave E, Albinet A (2012) Particle size distribution of nitrated and oxygenated polycyclic aromatic hydrocarbons (NPAHs and OPAHs) o traffic and suburban sites of a European megacity: Paris (France). Atmos Chem Phys 12:8877–8887
Roth CM, Goss KU, Schwarzenbach RP (2005) Sorption of a diverse set of organic vapors to urban aerosols. Environ Sci Technol 39:6638–6643
Ruan HD, Gilkes RJ (1995) Dehydroxylation of aluminous goethite: unit cell dimensions, crystal size and surface area. Clays Clay Miner 43:196–211
Salmeen I, Pero AM, Zator R, Schuetzle D, Riley TL (1984) Ames assay chromatograms and the identification of mutagens in diesel particle extracts. Environ Sci Technol 18:375–382
Schauer JJ, Rogge WF, Hildemann LM, Mazurek MA, Cass GR, Simoneit BRT (1996) Source apportionment of airborne particulate matter using organic compounds as tracers. Atmos Environ 30:3837–3855
Schwarzenbach RP, Gschwend PM, Imboden DM (2003) Environmental organic chemistry, 2nd ed., Wiley, New York, p 1328
Schnelle J, Jänsch J, Wolf K, Gebefügi I, Kettrup A (1995) Particle size dependent concentrations of polycyclic aromatic hydrocarbons (PAH) in the outdoor air. Chemosphere 31:3119–3127
Seinfeld JH, Pandis SN (2006) Atmospheric chemistry and physics, 2nd edn. Wiley, Hoboken, 1203 pp
Škrdlíková L, Landlová L, Klánová J, Lammel G (2011) Wet deposition and scavenging efficiency of gaseous and particulate phase polycyclic aromatic compounds at a central European suburban site. Atmos Environ 45:4305–4312
Spindler G, Gnauk T, Grüner A, Iinuma Y, Müller K, Scheinhardt S, Herrmann H (2012) Site-segregated characterization of PM10 at the EMEP site Melpitz (Germany) using a five-stage impactor: a six year study. J Atmos Chem 69:127–157
Spurny KR (1998) On the physics, chemistry and toxicology of ultrafine anthropogenic atmospheric aerosols: new advances. Toxicol Lett 96–97:253–261
Stier P, Feichter J, Roeckner E, Kloster S, Esch M (2006) The evolution of the global aerosol system in a transient climate simulation, 1860–2100. Atmos Chem Phys 6:3059–3076
Taylor GH, Teichmüller M, Davis A, Diessel CFK, Littke R, Robert P (1998) Organic petrology. Gebrüder Borntraeger, Berlin, Germany, 704 pp
Topinka J, Milcova A, Schmuczerova J, Krouzek J, Hovorka J (2013) Ultrafine particles are not major carriers of carcinogenic PAHs and their genotoxicity in size-segregated aerosols. Mutat Res 754:1–6
USEPA (2006) National ambient air quality standards, Federal Register 61143-61233, US Environmental Protection Agency, Washington, URL http://epa.gov/pm/actions.html
Welton JE, Field CO (1984) SEM petrology atlas. American Association of Petroleum Geologists. Tulsa, USA
WHO (2003) Health risks of persistent organic pollutants from long-range transboundary air pollution. World Health Organization Regional Office for Europe, Copenhagen, 252 pp
Zuend A, Seinfeld JH (2012) Modeling the gas-particle partitioning of secondary organic aerosol: the importance of liquid–liquid phase separation. Atmos Chem Phys 12:3857–3882
Acknowledgments
This study was supported by the Ministry of Environment of the Czech Republic (SP1a3/29/07), the EC FP7 project ArcRisk (226534), and by the Granting Agency of the Czech Republic (P503/11/1230). The RECETOX research infrastructure was supported by the project of the Ministry of Education of the Czech Republic LM2011028 and the CETOCOEN project of the European Structural Funds (CZ.1.05/2.1.00/01.001). Special thanks are due to F. Laufek and J. Malec for the XRD and SEM analysis.
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Landlová, L., Čupr, P., Franců, J. et al. Composition and effects of inhalable size fractions of atmospheric aerosols in the polluted atmosphere: Part I. PAHs, PCBs and OCPs and the matrix chemical composition. Environ Sci Pollut Res 21, 6188–6204 (2014). https://doi.org/10.1007/s11356-014-2571-y
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DOI: https://doi.org/10.1007/s11356-014-2571-y