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We interpret here the variability of levels of carbonaceous aerosols based on a 12 yr database from 78 monitoring stations across Spain specially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m−3 of non-mineral carbon (nmC), mostly made of organic carbon (OC) with very little elemental carbon (EC), around 0.1 μg m−3; OC / EC = 12–15), to the highly polluted major cities (8–10 μg m−3 of nmC; 3–4 μg m−3 of EC; 4–5 μg m−3 of OC; OC / EC = 1–2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning and of biogenic emissions. Correlations between yearly averaged OC / EC and EC concentrations adjust very well to a potential equation (OC = 3.37 EC0.326, R2 = 0.8). A similar equation is obtained when including average concentrations obtained at other European sites (OC = 3.60EC0.491, R2 = 0.7). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance from road, traffic volume and density, mixing-layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend for NO2 / (OC + EC) ratios as these standards have been much less effective for the abatement of NOx exhaust emissions in passenger diesel cars. This study concludes that EC, EBC, and especially nmC and OC + EC are very good candidates for new air quality standards since they cover both emission impact and health-related issues. ; This study was supported by the Ministry of Agriculture, Food and the Environment of Spain, the Ministry of Economy and Competitivity (MINECO) of Spain and FEDER funds under the projects VAMOS (CGL2010-19464/CLI), PRISMA (CGL2012-39623-C02-01), GRACCIE (CSD 2007-00067), POLLINDUST (CGL2011-26259) and UHU (CGL2011- 28025); and by AGAUR-Generalitat de Catalunya (2009 SGR 00008) and LIFE + AIRUSE (LIFE11-ENV/ES/000584). The Montseny site forms part of the ACTRIS network (European Union Seventh Framework Programme (FP7/2007-2013) project no. 262254), formerly EUSAAR (EUSAAR R113-CT-2006-026140). Funding was also received for the Andalucía sites from projects 2007-RNM027329 and 2011-RNM7800 (Department of Innovation Science and Enterprise, Andalusia Autonomous Government) M. C. Minguillón was funded by the JAE-Doc CSIC programme, co-funded by the European Social Fund (ESF).

The mass concentration, chemical composition and sources of quasi-ultrafine (quasi-UFP, PM 0.25 ), accumulation (PM 0.25–2.5 ) and coarse mode (PM 2.5–10 ) particles were determined in indoor and outdoor air at 39 schools in Barcelona (Spain). Quasi-UFP mass concentrations measured (25.6 μg m −3 outdoors, 23.4 μg m −3 indoors) are significantly higher than those reported in other studies, and characterised by higher carbonaceous and mineral matter contents and a lower proportion of secondary inorganic ions. Results suggest that quasi-UFPs in Barcelona are affected by local sources in the schools, mainly human activity (e.g. organic material from textiles, etc., contributing 23–46% to total quasi-UFP mass) and playgrounds (in the form of mineral matter, contributing about 9% to the quasi-UFP mass). The particle size distribution patterns of toxicologically relevant metals and major aerosol components was characterised, displaying two modes for most elements and components, and one mode for inorganic salts (ammonium nitrate and sulfate) and elemental carbon (EC). Regarding metals, Ni and Cr were partitioned mainly in quasi-UFPs and could thus be of interest for epidemiological studies, given their high redox properties. Exposure of children to quasi-UFP mass and chemical species was assessed by comparing the concentrations measured at urban background and traffic areas schools. Finally, three main indoor sources across all size fractions were identified by assessing indoor / outdoor ratios (I / O) of PM species used as their tracers: human activity (organic material), cleaning products, paints and plastics (Cl − source), and a metallic mixed source (comprising combinations of Cu, Zn, Co, Cd, Pb, As, V and Cr). Our results support the need to enforce targeted legislation to determine a minimum "safe" distance between major roads and newly built schools to reduce exposure to traffic-derived metals in quasi-UFPs.

The mass concentration, chemical composition and sources of quasi-ultrafine (quasi-UFP, PM0.25), accumulation (PM0.25–2.5) and coarse mode (PM2.5–10) particles were determined in indoor and outdoor air at 39 schools in Barcelona (Spain). Quasi-UFP mass concentrations measured (25.6 μg m−3 outdoors, 23.4 μg m−3 indoors) are significantly higher than those reported in other studies, and characterised by higher carbonaceous and mineral matter contents and a lower proportion of secondary inorganic ions. Results suggest that quasi-UFPs in Barcelona are affected by local sources in the schools, mainly human activity (e.g. organic material from textiles, etc., contributing 23–46% to total quasi-UFP mass) and playgrounds (in the form of mineral matter, contributing about 9% to the quasi-UFP mass). The particle size distribution patterns of toxicologically relevant metals and major aerosol components was characterised, displaying two modes for most elements and components, and one mode for inorganic salts (ammonium nitrate and sulfate) and elemental carbon (EC). Regarding metals, Ni and Cr were partitioned mainly in quasi-UFPs and could thus be of interest for epidemiological studies, given their high redox properties. Exposure of children to quasi-UFP mass and chemical species was assessed by comparing the concentrations measured at urban background and traffic areas schools. Finally, three main indoor sources across all size fractions were identified by assessing indoor / outdoor ratios (I / O) of PM species used as their tracers: human activity (organic material), cleaning products, paints and plastics (Cl− source), and a metallic mixed source (comprising combinations of Cu, Zn, Co, Cd, Pb, As, V and Cr). Our results support the need to enforce targeted legislation to determine a minimum "safe" distance between major roads and newly built schools to reduce exposure to traffic-derived metals in quasi-UFPs.

We demonstrate that there is great variation in the size range and chemical composition of metalliferous particulate matter (PM) present within petrochemical complex chimney stacks. Cascade impactor PM samples from seven size ranges (17, 14, 5, 2.5, 1.3, 0.67, and 0.33 mu m) were collected from inside stacks within the San Roque complex which includes the largest oil refinery in Spain. SEM analysis demonstrates the PM to be mostly carbonaceous and aluminous fly ash and abundant fine metalliferous particles. The metals with the most extreme concentrations averaged over all size ranges were Ni (up to 3295 mu g m(-3)), Cr (962 mu g m(-3)), V (638 mu g m(-3)), Zn (225 mu g m(-3)), Mo (91 mu g m(-3)), La (865 mu g m(-3)), and Co (94 mu g m(-3)). Most metal PM are strongly concentrated into the finest fraction (200 mu g m(-3) in PM(0.67-1.3)). Cr and Ni in a relatively coarse PM size range (0.7-14 mu m). Our unique database, directly sampled from chimney stacks, confirms that oil refinery complexes such as San Roque are a potent source of a variety of fine, deeply inhalable metalliferous atmospheric PM emissions ; This study was supported by the Department of the Environment and the Department of Innovation, Science and Enterprise (project RNM2007-02729) of the Autonomous Government of Andalusia, and Projects GRACCIE-CSD2007 of the Spanish Ministry of Science and Innovation. The authors are indebted to Juan Contreras, Francisca Godoy and Antonio Lozano of the Department of Air Quality in the Environmental Office of Andalusia Government for their collaboration with this study. Thanks are due to Wes Gibbons for his revision of the manuscript.

An analysis of chemical composition data of particulate matter samples (TSP, PM10 and PM2.5) collected from 2002 to 2008 in the North Atlantic free troposphere at the Izana Global Atmospheric Watch (GAW) observatory (Tenerife, Canary Islands) shows that desert dust is very frequently mixed with particulate pollutants in the Saharan Air Layer (SAL). The study of this data set with Median Concentrations At Receptor (MCAR) plots allowed the identification of the potential source regions of the dust and particulate pollutants. Areas located at the south of the southern slope of the Atlas mountains emerge as the most frequent source of the soil desert dust advected to the northern edge of the SAL in summer. Industrial emissions occurring in Northern Algeria, Eastern Algeria, Tunisia and the Atlantic coast of Morocco appear as the most important source of the nitrate, ammonium and a fraction of sulphate (at least 60% of the sulphate <10 mu m transported from some regions) observed in the SAL. These emissions are mostly linked to crude oil refineries, phosphate-based fertilizer industry and power plants. Although desert dust emissions appear as the most frequent source of the phosphorous observed in the SAL, high P concentrations are observed when the SAL is affected by emissions from open mines of phosphate and phosphate based fertilizer industry. The results also show that a significant fraction of the sulphate (up to 90% of sulphate <10 mu m transported from some regions) observed in the SAL may be influenced by soil emissions of evaporite minerals in well defined regions where dry saline lakes (chotts) are present. These interpretations of the MCAR plots are consistent with the results obtained with the Positive Matrix Factorization PMF2) receptor modelling. The results of this study show that North African industrial pollutants may be mixed with desert dust and exported to the North Atlantic in the Saharan Air Layer. ; This study has been carried out within the Global Atmospheric Watch Program (financed by AEMET), and in the framework of the research projects GRACCIE (CSD2007-00067; Ministry of Science and Innovation of Spain), CARIATI (CGL2008-06294/CLI; Ministry of Science and Innovation of Spain), AER-REG (P07-RNM-03125; Department of Innovation, Science and Enterprise of the Government of Andalusia) and REDMAAS (CGL2010-11095-E; Ministry of Science and Innovation of Spain). We thank NOAA Air Resources Laboratory for the facilities (software and data) for determining back-trajectories, NOAA Earth System Research Laboratory for providing meteorological tools, NASA Goddard Earth Sciences Data and Information Service Centre (Giovanni service) for providing Aerosol Index data and Google Earth (TM), Google map (TM) and Panoramio (TM). We distinguish the excellent work performed by the staff in charge of the aerosol sampling: Fernando de Ory, Carlos Torres, Virgilio Varreno, Candida Hernandez, Julian Perez, Daniel Martin, Ruben Del Campo, Cesar Lopez, Marco Hernandez, Damian Exposito, Antonio Hernandez and Jose Hernandez.

The Caliope project funded by the Spanish Ministry of the Environment establishes an air quality forecasting system for Spain to increase the knowledge on transport and dynamics of pollutants in Spain, to assure the accomplishment of legislation and to inform the population about the levels of pollutants, topics in which the European Commission has shown a great concern. The present contribution describes the first quantitative verification study performed so far with two chemistry transport models (CMAQ and CHIMERE) for a reference year (2004) at medium spatial resolution (around 20×20 km for the Iberian Peninsula). Both models perform similarly in the case of ground-level ozone. The mean normalised gross error MNGE remains below 15–20% during summertime, when ozone episodes occur, outlining the good skills of the system concerning the forecasting of air quality in Spain. Furthermore, the ongoing developments of the system towards high resolution modelling (4×4 km for Spain, 12×12 km for Europe, 1 h temporal resolution) and the integration with observations within the Caliope umbrella are described.

OBJECTIVE: Quantitative estimates of air pollution health impacts have become an increasingly critical input to policy decisions. The WHO project "Health risks of air pollution in Europe--HRAPIE" was implemented to provide the evidence-based concentration-response functions for quantifying air pollution health impacts to support the 2013 revision of the air quality policy for the European Union (EU). METHODS: A group of experts convened by WHO Regional Office for Europe reviewed the accumulated primary research evidence together with some commissioned reviews and recommended concentration-response functions for air pollutant-health outcome pairs for which there was sufficient evidence for a causal association. RESULTS: The concentration-response functions link several indicators of mortality and morbidity with short- and long-term exposure to particulate matter, ozone and nitrogen dioxide. The project also provides guidance on the use of these functions and associated baseline health information in the cost-benefit analysis. CONCLUSIONS: The project results provide the scientific basis for formulating policy actions to improve air quality and thereby reduce the burden of disease associated with air pollution in Europe.

The Caliope project funded by the Spanish Ministry of the Environment establishes an air quality forecasting system for Spain to increase the knowledge on transport and dynamics of pollutants in Spain, to assure the accomplishment of legislation and to inform the population about the levels of pollutants, topics in which the European Commission has shown a great concern. The present contribution describes the first quantitative verification study performed so far with two chemistry transport models (CMAQ and CHIMERE) for a reference year (2004) at medium spatial resolution (around 20×20 km for the Iberian Peninsula). Both models perform similarly in the case of ground-level ozone. The mean normalised gross error MNGE remains below 15–20% during summertime, when ozone episodes occur, outlining the good skills of the system concerning the forecasting of air quality in Spain. Furthermore, the ongoing developments of the system towards high resolution modelling (4×4 km for Spain, 12×12 km for Europe, 1 h temporal resolution) and the integration with observations within the Caliope umbrella are described.

International audience ; The Caliope project funded by the Spanish Ministry of the Environment establishes an air quality forecasting system for Spain to increase the knowledge on transport and dynamics of pollutants in Spain, to assure the accomplishment of legislation and to inform the population about the levels of pollutants, topics in which the European Commission has shown a great concern. The present contribution describes the first quantitative verification study performed so far with two chemistry transport models (CMAQ and CHIMERE) for a reference year (2004) at medium spatial resolution (around 20×20 km for the Iberian Peninsula). Both models perform similarly in the case of ground-level ozone. The mean normalised gross error MNGE remains below 15?20% during summertime, when ozone episodes occur, outlining the good skills of the system concerning the forecasting of air quality in Spain. Furthermore, the ongoing developments of the system towards high resolution modelling (4×4 km for Spain, 12×12 km for Europe, 1 h temporal resolution) and the integration with observations within the Caliope umbrella are described.