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The number of ultrafine particles may be a more health relevant characteristic of ambient particulate matter than the conventionally measured mass. Epidemiological time series studies typically use a central site to characterize human exposure to outdoor air pollution. There is currently very limited information how well measurements at a central site reflect temporal and spatial variation across an urban area for particle number concentrations (PNC). The main objective of the study was to assess the spatial variation of PNC compared to the mass concentration of particles with diameter less than 10 or 2.5 mm (PM 10 and PM 2.5). Continuous measurements of PM 10 , PM 2.5 , PNC and soot concentrations were conducted at a central site during October 2002-March 2004 in four cities spread over Europe (Amsterdam, Athens, Birmingham and Helsinki). The same measurements were conducted directly outside 152 homes spread over the metropolitan areas. Each home was monitored during 1 week. We assessed the temporal correlation and the variability of absolute concentrations. For all particle indices, including particle number, temporal correlation of 24-h average concentrations was high. The median correlation for PNC per city ranged between 0.67 and 0.76. For PM 2.5 median correlation ranged between 0.79 and

The objective of this study was to analyse environmental tobacco smoke (ETS) and PAH metabolites in urine samples of non-occupationally exposed non-smoker adult subjects and to establish relationships between airborne exposures and urinary concentrations in order to (a) assess the suitability of the studied metabolites as biomarkers of PAH and ETS, (b) study the use of 3-ethenypyridine as ETS tracer and (c) link ETS scenarios with exposures to carcinogenic PAH and VOC. Urine samples from 100 subjects were collected and concentrations of monophenolic metabolites of naphthalene, fluorene, phenanthrene, and pyrene and the nicotine metabolites cotinine and trans-3′-hydroxycotinine were measured using liquid chromatography–tandem mass spectrometry (LC-MS/MS) to assess PAH and ETS exposures. Airborne exposures were measured using personal exposure samplers and analysed using GC–MS. These included 1,3-butadiene (BUT), 3-ethenylpyridine (3-EP) (a tobacco-specific tracer derived from nicotine pyrolysis) and PAHs. ETS was reported by the subjects in 30-min time–activity questionnaires and specific comments were collected in an ETS questionnaire each time ETS exposure occurred. The values of 3-EP (>0.25 μg/m3 for ETS) were used to confirm the ETS exposure status of the subject. Concentrations as geometric mean, GM, and standard deviation (GSD) of personal exposures were 0.16 (5.50)μg/m3 for 3-EP, 0.22 (4.28)μg/m3 for BUT and 0.09 (3.03)ng/m3 for benzo(a)pyrene. Concentrations of urinary metabolites were 0.44 (1.70)ng/mL for 1-hydroxypyrene and 0.88 (5.28)ng/mL for cotinine. Concentrations of urinary metabolites of nicotine were lower than in most previous studies, suggesting very low exposures in the ETS-exposed group. Nonetheless, concentrations were higher in the ETS population for cotinine, trans-3′hydroxycotinine, 3-EP, BUT and most high molecular weight PAH, whilst 2-hydroxyphenanthrene, 3+ 4-hydroxyphenanthrene and 1-hydroxyphenanthrene were only higher in the high-ETS subpopulation. There were not many significant correlations between either personal exposures to PAH and their urinary metabolites, or of the latter with ETS markers. However, it was found that the urinary log cotinine concentration showed significant correlation with log concentrations of 3-EP (R =0.75), BUT (R =0.47), and high molecular weight PAHs (MW>200), especially chrysene (R = 0.55) at the p = 0.01 level. On the other hand, low correlation was observed between the PAH metabolite 2-naphthol and the parent PAH, gas-phase naphthalene. These results suggest that (1) ETS is a significant source of inhalation exposure to the carcinogen 1,3-butadiene and high molecular weight PAHs, many of which are carcinogenic, and (2) that for lower molecular weight PAHs such as naphthalene, exposure by routes other than inhalation predominate, since metabolite levels correlated poorly with personal exposure air sampling.

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The associations between residential outdoor and ambient particle mass, fine particle absorbance, particle number (PN) concentrations, and residential and traffic determinants were investigated in four European urban areas (Helsinki, Athens, Amsterdam, and Birmingham). A total of 152 nonsmoking participants with respiratory diseases, not exposed to occupational pollution, were included in the study, which comprised a 7-day intensive exposure monitoring period of both indoor and home outdoor particle mass and number concentrations. The same pollutants were also continuously measured at ambient fixed sites centrally located to the studied areas (fixed ambient sites). Relationships between concentrations measured directly outside the homes (residential outdoor) and at the IMPLICATIONS Uncertainties of health risk estimates associated with exposures to PM are mostly due to weak correlations between personal exposures and ambient concentrations, which vary for different fractions of PM. Among other factors, the variability of PM concentration within an urban area is accountable, especially for coarse and ultrafine particles. This study focused on the analysis of spatial variation of fine and coarse PM and ultrafine particles in urban areas. The outcomes of this investigation provide insights on the impact of sampling, home outdoor, and traffic characteristics on the variability of particle mass and number concentrations, which are also critical in developing policies to control atmospheric PM and its sources. fixed ambient sites were pollutant-specific, with substantial variations among the urban areas. Differences were more pronounced for coarse particles due to resuspension of road dust and PN, which is strongly related to traffic emissions. Less significant outdoor-to-fixed variation for particle mass was observed for Amsterdam and Birmingham, predominantly due to regional secondary aerosol. On the contrary, a strong spatial variation was observed for Athens and to a lesser extent for Helsinki. This was attributed to the overwhelming and time-varied inputs from traffic and other local sources. The location of the residence and traffic volume and distance to street and traffic light were important determinants of residential outdoor particle concentrations. On average, particle mass levels in suburban areas were less than 30% of those measured for residences located in the city center. Residences located less than 10 m from a street experienced 133% higher PN concentrations than residences located further away. Overall, the findings of this multi-city study, indicated that (1) spatial variation was larger for PN than for fine particulate matter (PM) mass and varied between the cities, (2) vehicular emissions in the residential street and location in the center of the city were significant predictors of spatial variation, and (3) the impact of traffic and location in the city was much larger for PN than for fine particle mass. TECHNICAL PAPER