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Abstract. Size and time-resolved roadside enrichments of atmospheric particulate pollutants in PM 10 were detected and quantified in a Mediterranean urban environment (Barcelona, Spain). Simultaneous data from one urban background (UB), one traffic (T) and one heavy traffic (HT) location were analysed, and roadside PM 10 enrichments (RE) in a number of elements arising from vehicular emissions were calculated. Tracers of primary traffic emissions (EC, Fe, Ba, Cu, Sb, Cr, Sn) showed the largest REs (>70%). Other traffic tracers (Zr, Cd) showed lower but still consistent REs (25-40%), similar to those obtained for mineral matter resulting from road dust resuspension (Ca, La, Ce, Ti, Ga, Sr, 30-40%). The sum of primary and secondary organic carbon showed a RE of 41%, with contributions of secondary OC (SOC) to total OC ranging from 46% at the HT site, 63% at the T site, and 78% in the UB. Finally, other trace elements (As, Co, Bi) showed unexpected but consistent roadside enrichments (23% up to 69%), suggesting a link to traffic emissions even though the emission process is unclear.Hourly-resolved PM speciation data proved to be a highly resourceful tool to determine the source origin of atmospheric pollutants in urban environments. At the HT site, up to 62% of fine Mn was attributable to industrial plumes, whereas coarse Mn levels were mainly attributed to traffic. Similarly, even though Zn showed on average no roadside enrichment and thus was classified as industrial, the hourlyresolved data proved that at least 15% of coarse Zn may be attributed to road traffic emissions. In addition, our results indicate that secondary nitrate formation occurs within the Correspondence to: F. Amato (fulvio.amato@idaea.csic.es) city-scale, even in the absence of long atmospheric residence times or long-range atmospheric transport processes. Characteristic tracer ratios of road traffic emissions were identified: Cu/Sb = 6.8-8.0, Cu/Sn = 4.7-5.4 and Sn/Sb = 1.5.

Hourly trace element measurements were performed in an urban street canyon and next to an interurban freeway in Switzerland during more than one month each, deploying a rotating drum impactor (RDI) and subsequent sample analysis by synchrotron radiation X-ray fluorescence spectrometry (SR-XRF). Antimony and other brake wear associated elements were detected in three particle size ranges (2.5-10, 1-2.5, and 0.1-1 microm). The hourly measurements revealed that the effect of resuspended road dust has to be taken into account for the calculation of vehicle emission factors. Individual values for light and heavy duty vehicles were obtained for stop-and-go traffic in the urban street canyon. Mass based brake wear emissions were predominantly found in the coarse particle fraction. For antimony, determined emission factors were 11 +/- 7 and 86 +/- 42 microg km(-1) vehicle(-1) for light and heavy duty vehicles, respectively. Antimony emissions along the interurban freeway with free-flowing traffic were significantly lower. Relative patterns for brake wear related elements were very similar for both considered locations. Beside vehicle type specific brake wear emissions, road dust resuspension was found to be a dominant contributor of antimony in the street canyon.

Abstract. Time and size resolved data of trace elements were obtained from measurements with a rotating drum impactor (RDI) and subsequent X-ray fluorescence spectrometry. Trace elements can act as indicators for the identification of sources of particulate matter <10 μm (PM10) in ambient air. Receptor modeling was performed with positive matrix factorization (PMF) for trace element data from an urban background site in Zürich, Switzerland. Eight different sources were identified for the three examined size ranges (PM1−0.1, PM2.5−1 and PM10−2.5): secondary sulfate, wood combustion, fire works, road traffic, mineral dust, de-icing salt, industrial and local anthropogenic activities. The major component was secondary sulfate for the smallest size range; the road traffic factor was found in all three size ranges. This trace element analysis is complemented with data from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS), assessing the PM1 fraction of organic aerosols. A separate PMF analysis revealed three factors related to three of the sources found with the RDI: oxygenated organic aerosol (OOA, related to inorganic secondary sulfate), hydrocarbon-like organic aerosol (HOA, related to road traffic) and biomass burning organic aerosol (BBOA), explaining 60 %, 22 % and 17 % of total measured organics, respectively. Since different compounds are used for the source classification, a higher percentage of the ambient PM10 mass concentration can be apportioned to sources by the combination of both methods.