Abstract. The AIRUSE-LIFE+ project aims at characterizing similarities and heterogeneities in particulate matter (PM) sources and contributions in urban areas from southern Europe. Once the main PMx sources are identified, AIRUSE aims at developing and testing the efficiency of specific and non-specific measures to improve urban air quality. This article reports the results of the source apportionment of PM10 and PM2.5 conducted at three urban background sites (Barcelona, Florence and Milan, BCN-UB, FI-UB and MLN-UB), one suburban background site (Athens, ATH-SUB) and one traffic site (Porto, POR-TR). After collecting 1047 PM10 and 1116 PM2.5 24 h samples during 12 months (from January 2013 on) simultaneously at the five cities, these were analysed for the contents of OC, EC, anions, cations, major and trace elements and levoglucosan. The USEPA PMF5 receptor model was applied to these data sets in a harmonized way for each city. The sum of vehicle exhaust (VEX) and non-exhaust (NEX) contributes between 3.9 and 10.8 µg m−3 (16–32 %) to PM10 and 2.3 and 9.4 µg m−3 (15–36 %) to PM2.5, although a fraction of secondary nitrate is also traffic-related but could not be estimated. Important contributions arise from secondary particles (nitrate, sulfate and organics) in PM2.5 (37–82 %) but also in PM10 (40–71 %), mostly at background sites, revealing the importance of abating gaseous precursors in designing air quality plans. Biomass burning (BB) contributions vary widely, from 14–24 % of PM10 in POR-TR, MLN-UB and FI-UB, 7 % in ATH-SUB, to  <  2 % in BCN-UB. In PM2.5, BB is the second most important source in MLN-UB (21 %) and in POR-TR (18 %), the third one in FI-UB (21 %) and ATH-SUB (11 %), but is again negligible (< 2 %) in BCN-UB. This large variability among cities is mostly due to the degree of penetration of biomass for residential heating. In Barcelona natural gas is very well supplied across the city and is used as fuel in 96 % of homes, while in other cities, PM levels increase on an annual basis by 1–9 µg m−3 due to biomass burning influence. Other significant sources are the following. – Local dust, 7–12 % of PM10 at SUB and UB sites and 19 % at the TR site, revealing a contribution from road dust resuspension. In PM2.5 percentages decrease to 2–7 % at SUB-UB sites and 15 % at the TR site. – Industry, mainly metallurgy, contributing 4–11 % of PM10 (5–12 % in PM2.5), but only at BCN-UB, POR-TR and MLN-UB. No clear impact of industrial emissions was found in FI-UB and ATH-SUB. – Natural contributions from sea salt (13 % of PM10 in POR-TR, but only 2–7 % in the other cities) and Saharan dust (14 % in ATH-SUB, but less than 4 % in the other cities). During high pollution days, the largest sources (i.e. excluding secondary aerosol factors) of PM10 and PM2.5 are VEX + NEX in BCN-UB (27–22 %) and POR-TR (31–33 %), BB in FI-UB (30–33 %) and MLN-UB (35–26 %) and Saharan dust in ATH-SUB (52–45 %). During those days, there are also quite important industrial contributions in BCN-UB (17–18 %) and local dust in POR-TR (28–20 %).

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Saharan dust that is transported over the Atlantic Ocean provides an important input of phosphorus (P) to the oligotrophic waters of ocean and the P-depleted rain forests of America. To establish more firmly the role of Saharan dust events as P suppliers, the dust P sources needs to be identified. From analysis of phosphate oxygen isotopes of all the major Saharan dust events of 2011 over the Cape Verde islands in the northeastern Atlantic, supported by remote-sensing imagery, we infer that the dust P originates from widespread sedimentary sources and magmatic P "hot spots", in which the latter enrich the dust in bioavailable P. The fraction contributed from each source varied markedly between dust events. We also found that phosphate from the Bodeĺed epression is not evident in Cape Verde. Our results provide new information for global biogeochemical studies and suggest that identification of Saharan dust P sources is required to improve their accuracy.

Abstract. São Paulo in Brazil has relatively relaxed regulations for ambient air pollution standards and often experiences high air pollution levels due to emissions of particulate pollutants from local sources and long-range transport of air masses impacted by biomass burning. In order to evaluate the sources of particulate air pollution and related health risks, a year-round sampling was done at the University of São Paulo campus (20 m a.g.l.), a green area near an important expressway. The sampling was performed for PM 2.5 (≤ 2.5 µm) and PM 10 (≤ 10 µm) in 2014 through intensive (everyday sampling in wintertime) and extensive campaigns (once a week for the whole year) with 24 h of sampling. This year was characterized by having lower average precipitation compared to meteorological data, and high-pollution episodes were observed all year round, with a significant increase in pollution level in the intensive campaign, which was performed during wintertime. Different chemical constituents, such as carbonaceous species, polycyclic aromatic hydrocarbons (PAHs) and derivatives, water-soluble ions, and biomass burning tracers were identified in order to evaluate health risks and to apportion sources. The species such as PAHs, inorganic and organic ions, and monosaccharides were determined using chromatographic techniques and carbonaceous species using thermal-optical analysis. Trace elements were determined using inductively coupled plasma mass spectrometry. The risks associated with particulate matter exposure based on PAH concentrations were also assessed, along with indexes such as the benzo[a]pyrene equivalent (BaPE) and lung cancer risk (LCR). High BaPE and LCR were observed in most of the samples, rising to critical values in the wintertime. Also, biomass burning tracers and PAHs were higher in this season, while secondarily formed ions presented low variation throughout the year. Meanwhile, vehicular tracer species were also higher in the intensive campaign, suggesting the influence of lower dispersion conditions in that period. Source apportionment was performed using positive matrix factorization (PMF), which indicated five different factors: road dust, industrial emissions, vehicuPublished by Copernicus Publications on behalf of the European Geosciences Union. 11944 G. M. Pereira et al.: Particulate pollutants in the Brazilian city of São Paulo lar exhaust, biomass burning and secondary processes. The results highlighted the contribution of vehicular emissions and the significant input from biomass combustion in wintertime, suggesting that most of the particulate matter is due to local sources, in addition to the influence of pre-harvest sugarcane burning.

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Abstract. The contribution of natural sources to ambient air particulate matter (PM) concentrations is often not considered; however, it may be significant for certain areas and during specific periods of the year. In the framework of the AIRUSE-LIFE+ project, state-of-the-art methods have been employed for assessing the contribution of major natural sources (African dust, sea salt and forest fires) to PM concentrations, in southern European urban areas. 24 h measurements of PM 10 and PM 2.5 mass and chemical composition were performed over the course of a year in five cities: Porto, Barcelona, Milan, Florence and Athens. Net African dust and sea-salt concentrations were calculated based on the methodologies proposed by the EC (SEC 2011/208). The contribution of uncontrolled forest fires was calculated through receptor modelling. Sensitivity analysis with respect to the calculation of African dust was also performed, in order to identify major parameters affecting the estimated net dust concentrations. African dust contribution to PM concentrations was more pronounced in the eastern Mediterranean, with the mean annual relative contribution to PM 10 decreasing from 21 % in Athens, to 5 % in Florence, and around 2 % in Milan, Barcelona and Porto. The respective contribution to PM 2.5 was calculated equal to 14 % in Athens and from 1.3 to 2.4 % in all other cities. High seasonal variability of contributions was observed, with dust transport events occurring at different periods in the western and eastern Mediterranean basin. Sea salt was mostly related to the coarse mode and also exhibited significant seasonal variability. Sea-salt concentrations were highest in Porto, with average relative contributions equal to 12.3 % for PM 10 . Contributions from uncontrolled forest fires were quantified only for Porto and were low on an annual basis (1.4 and 1.9 % to PM 10 and PM 2.5 , respectively); nevertheless, contributions were greatly increased during events, reaching 20 and 22 % of 24 h PM 10 and PM 2.5 concentrations, respectively.

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