Estimating the probability of occurrence of African dust outbreaks over regions of the western Mediterranean basin from thermodynamic atmospheric parameters.

Desert dust is currently recognized as a health risk factor. Therefore, the World Health Organization (WHO) is actively promoting the establishment of early warning systems for sand and dust storms. This study introduces a methodology to estimate the probability of African dust outbreaks occurring in eight different regions of the Iberian Peninsula and the Balearic Islands. In each region, a multilinear regression model was developed to calculate daily probabilities of dust events using three thermodynamic variables (geopotential thickness in the 1000-500 hPa layer, mean potential temperature between 925 and 700 hPa, and temperature anomalies at 850 hPa) as assessment parameters. All days with African dust transport over each study region were identified in the period 2001-2021 using a proven procedure. This information was then utilized to establish a functional relationship between the values of the thermodynamic parameters and the probability of African dust outbreaks occurring. The validation of this methodology involved comparing the daily probabilities of dust events generated by the models in 2001-2021 with the daily African dust contributions to PM10 regional background levels in each region. On average, daily dust contributions increased proportionally with the increase in daily probabilities, reaching zero for days with low probabilities. Furthermore, a well-defined seasonal evolution of probability values was observed in all regions, with the highest values in the summer months and the lowest in the winter period, ensuring the physical relevance of the models' results. Finally, upward trends were observed in all regions for the three thermodynamic parameters over 1940-2021. Thus, the probability of dust events development also increased in this period. It demonstrates that the aggravation of warm conditions in southern Europe in the last decades, have modified the frequency of North-African dust outbreaks over the western Mediterranean basin.

Reasons for the observed tropospheric ozone weakening over south-western Europe during COVID-19: Strict lockdown versus the new normal.

In this work we investigate the variation in tropospheric ozone concentrations in south-western Europe in March and April 2020 in the context of COVID-19 disease, and to what extent the former situation was recovered one year after the pandemic outbreak. To carry this study, data from 15 regional background sites in Spain, from 2010 onwards, are used. Historic (2010-2019) and most recent tropospheric ozone concentrations are compared. March and April 2020 ozone concentrations declined over 15% in most cases, rising to 23-28% at sites facing the Mediterranean. Most of the decay was related to the reduction of hemispheric background concentrations, but those sites downwind continental emissions from the Iberian Peninsula and neighbouring countries experienced an additional lessening. By exploring O3 concentrations one year after, March and April 2021, the general decline with respect to 2010-2019 persist but its magnitude was substantially lessened with respect to the strict lockdown period. The pandemic situation unveiled that air pollution is not an endemic matter but it should be tackle with adequate actions. Ozone abatement plans for Mediterranean countries should need a pan-regional covenant in order to drop precursor emissions.

Influence of hail suppression systems over silver content in the environment in Aragón (Spain). I: Rainfall and soils.

In several countries, hail is considered as the most harmful climatic phenomenon from an agricultural perspective. The surroundings of the Gallocanta Lake (North-East Spain), is one of the areas where the storms affecting the Ebro Valley are formed. For this reason, silver iodide from hail suppression systems has been emitted to the atmosphere for half a century. Nowadays, there is an increasing social concern about the potential environmental consequences of this activity, which has promoted the analysis of the influence of hail suppression systems regarding the amount of silver concentration in the ecosystem. This study focuses on silver atmospheric deposition and its accumulation in soils. To this end, silver concentrations in rainfall (5 gauges, 16 samples per site, from April 2017 to March 2019) and soils (72 samples) distributed across the hail suppression network managed by the Anti-hail Consortium of Aragón, were analysed. The results show that the amount of silver is much higher in rainfall gauges and soils close to ground-based silver iodide generators (85 µg/m2·day and 10 mg/kg soil, respectively), but concentrations considerably decrease when samples are collected far from them (downing to 0.3 µg/m2·day and 0.1 mg/kg soil). Apart from the samples obtained nearby silver iodide generators, most of the other soil samples display silver concentrations below the legal threshold established for the most vulnerable activities (1 mg/kg soil in agricultural and forestry land uses). Nevertheless, silver content, both in precipitation and in soils, is higher in regions where hail suppression has been developed for decades when compared to nearby areas in which silver iodide emissions did not occur. Silver content observed in soils is not high, but their cumulative effect in sediments and biota should be analysed, which is the aim of the second part of the present study.

Chemistry of dry and wet atmospheric deposition over the Balearic Islands, NW Mediterranean: Source apportionment and African dust areas.

Wet and dry aerosol deposition samples were collected from September 2010 to August 2012 at a remote background site in the Mallorca Isle (Western Mediterranean). Ions and major and trace elements were determined in soluble and insoluble fractions. Temporal variations of chemical components are discussed and interpreted. The overall pattern associated to long-range-transport air masses is studied: Dry/Wet deposition ratios, charges and composition depend clearly on the meteorological scenario. E.g. Dry/Wet ratio is 1:1 when air comes from North Africa, in contrast to a 1:9 ratio under the mainland Europe influence. Moreover, an innovating source apportionment study was conducted integrating both dry and wet deposition samples. Six sources were revealed, including marine aerosols (32%); two different mineral factors, African dust (15%) and regional dust (12%); two anthropogenic factors, one related to road traffic (8%) and another to regional sources (17%); and a mixed factor having biomass burning emissions and others sources (17%). Temporal variations and influence from long-range-transport air masses are also investigated. Fertilization deposition trends have also been explored, observing nutrients settling, as well as nitrate and sulphate, due to their agricultural interest. An important peak during January-February 2012 is studied in depth. Having in mind the strong impact of African dust on the global deposition budget, the analysis of elemental ratios between key dust components was investigated in order to identify major source areas affecting Western Mediterranean: Western Sahara, Algeria-Hoggar Massif and Tunisia-Libya. Differences among these regions are evident. E.g. the impact of industrial emissions is well-detected under outbreaks from Tunisia-Libya, with relatively high content of Ni and Pb.

Phenomenology and geographical gradients of atmospheric deposition in southwestern Europe: Results from a multi-site monitoring network.

This article presents the results of atmospheric deposition from a 15-sites network which cover remote, agricultural, urban and industrial areas in the Iberian Peninsula and the Balearic Islands, with the aim of exploring geographical, climatic and natural vs anthropogenic gradients. Annual average fluxes of global deposition, discriminating insoluble (3,5-20,7 g m-2 year-1) and soluble-inorganic (7,1-45,5 g m-2 year-1) aerosols are discussed, seasonal patterns are regarded, and an attempt to estimate the impact of the main sources is presented. The wide range of atmospheric deposition fluxes (DF) regarding soluble (DFSOL) and insoluble (DFINS) has been investigated taking into consideration the contribution from nearby to long-distance sources, such as African dust, or regional-to-nearby ones, which include agricultural dust in the Ebro Valley, industrial emissions at different parts, urban dust at all cities, or saline dust resuspension from a dissicated lake bed. DFSOL is made up of marine aerosols, prevailing in coastal areas, with few exceptions in the Ebro Valley; nitrogen-species, homogeneously distributed across the network, with few exceptions due to agricultural sources; mineral dust, enhanced in the Ebro Valley owing to regional and agricultural emissions; and phospathe, displaying comparable values to other studies in general, but three hotspots at regional background environments have been identified. DFINS particles followed the aridity pattern, especially where anthropogenic emissions take place. Our estimates indicate that the regional dust to DFINS in the Ebro Valley represented 23-30%, overpassing 50% at intensive agricultural areas. Similarly, urban-metropolitan contributions accounted for 37-45% at the four cities, and 55% at the industrial one. African dust deposition was enhanced in the Central Pyrenees (75-80%) as a result of the magnification of atmospheric washout processes, and in south-eastern Iberia (69%) owing to the higher frequency of dust outbreaks.

Variability of air pollutants, and PM composition and sources at a regional background site in the Balearic Islands: Review of western Mediterranean phenomenology from a 3-year study.

The present study discloses the results of a comprehensive 3-years campaign (2010-2012) of air pollution measurements over an regional island background area (Can Llompart-Balearic Islands, Spain), contextualized with other measurements in the western Mediterranean region. Gaseous pollutants and particulate matter fractions were measured in real time; and PM10 and PM1 daily samples were obtained regularly from which chemical analyses were performed. Furthermore, during three intensive observation periods, real-time concentrations of particle number, black carbon and ammonia were additionally measured. Our results display particular diurnal and seasonal patterns for certain pollutants such as O3 and particle number concentration. Our study reveals that concentrations of air pollutants and aerosol chemical composition are rather similar all over the central and western Mediterranean basin. The most abundant chemical components in PM10 were mineral dust, followed by organic matter, sea spray and SO42-; in PM1 organic matter and SO42- dominated, with significant contribution of mineral dust. Furthermore, a source apportionment Positive Matrix Factorization analysis was conducted. Natural sources exert most of the impact on the coarse-mode fraction, while most of fine-mode aerosols are linked to anthropogenic sources coming from local, regional or long range transport emissions. Prevalence of Atlantic air masses in 2010 had a positive effect in air quality, lowering mineral dust, SO42- and EC concentrations. On the contrary, the high incidence of African dust and regional recirculation situations during the 2012 warm season favoured an overall PM load increase governed by mineral dust, SO42- and trace elements associated to dust aerosols. The continuous increase in tourists in the Balearic Islands, and in general all around the Mediterranean, is clearly changing air quality patterns: while urban air pollution has strongly decreased since 2010, such downward trend is less pronounced at the regional scale, thus related to crescent sources such as maritime and air transport.

Impact of harbour emissions on ambient PM10 and PM2.5 in Barcelona (Spain): Evidences of secondary aerosol formation within the urban area.

With the objective of estimating the impact of harbour activities on ambient PM10 and PM2.5 levels at the urban area of Barcelona, a one year long monitoring campaign was carried out in the context of the European APICE project (MED-FEDER-EC). This campaign was simultaneously conducted at the port and a central urban background site. A detailed PM10 and PM2.5 chemical speciation analysis was carried out with samples from both sites. Subsequently, a source apportionment analysis by means of the PMF receptor model was performed. Six common factors were identified, explaining local to regional emission sources (fuel oil combustion, industrial emissions, mineral-road dust resuspension, and road traffic emissions) and aerosol formation/transformation processes (secondary aerosols including ammonium sulphate and organic aerosols, and a mixed source accounting for aged sea spray and secondary nitrate). Around 50-55% PM10 and PM2.5 measured at the port was attributed to harbour activities: mineral matter from road dust and construction works of a new port area, vehicle traffic and fuel oil combustion. The estimated contribution of harbour emissions to the urban background reached 9-12% for PM10 and 11-15% for PM2.5 and is linked to primary emissions from fuel oil combustion but also to the formation of secondary aerosols. It becomes relevant to highlight the significantly higher contribution of secondary aerosols at the urban background when compared with the harbour site. Our hypothesis points to the fast formation of secondary ammonium sulphate within the city, after the reaction of SO2/H2SO4 transported by sea breezes with NH3, which is emitted in large amounts in Barcelona; and also to the enhanced formation of secondary organic aerosols within the city. This study broadens our knowledge on atmospheric phenomenology in urban Mediterranean cities and claims for effective abatement strategies focused on maritime practises, in agreement with the driving axis of the APICE project.

Desert Dust Outbreaks in Southern Europe: Contribution to Daily PM10 Concentrations and Short-Term Associations with Mortality and Hospital Admissions.

BACKGROUND: Evidence on the association between short-term exposure to desert dust and health outcomes is controversial. OBJECTIVES: We aimed to estimate the short-term effects of particulate matter ≤ 10 µm (PM10) on mortality and hospital admissions in 13 Southern European cities, distinguishing between PM10 originating from the desert and from other sources. METHODS: We identified desert dust advection days in multiple Mediterranean areas for 2001-2010 by combining modeling tools, back-trajectories, and satellite data. For each advection day, we estimated PM10 concentrations originating from desert, and computed PM10 from other sources by difference. We fitted city-specific Poisson regression models to estimate the association between PM from different sources (desert and non-desert) and daily mortality and emergency hospitalizations. Finally, we pooled city-specific results in a random-effects meta-analysis. RESULTS: On average, 15% of days were affected by desert dust at ground level (desert PM10 > 0 µg/m3). Most episodes occurred in spring-summer, with increasing gradient of both frequency and intensity north-south and west-east of the Mediterranean basin. We found significant associations of both PM10 concentrations with mortality. Increases of 10 µg/m3 in non-desert and desert PM10 (lag 0-1 days) were associated with increases in natural mortality of 0.55% (95% CI: 0.24, 0.87%) and 0.65% (95% CI: 0.24, 1.06%), respectively. Similar associations were estimated for cardio-respiratory mortality and hospital admissions. CONCLUSIONS: PM10 originating from the desert was positively associated with mortality and hospitalizations in Southern Europe. Policy measures should aim at reducing population exposure to anthropogenic airborne particles even in areas with large contribution from desert dust advections. CITATION: Stafoggia M, Zauli-Sajani S, Pey J, Samoli E, Alessandrini E, Basagaña X, Cernigliaro A, Chiusolo M, Demaria M, Díaz J, Faustini A, Katsouyanni K, Kelessis AG, Linares C, Marchesi S, Medina S, Pandolfi P, Pérez N, Querol X, Randi G, Ranzi A, Tobias A, Forastiere F, MED-PARTICLES Study Group. 2016. Desert dust outbreaks in Southern Europe: contribution to daily PM10 concentrations and short-term associations with mortality and hospital admissions. Environ Health Perspect 124:413-419; http://dx.doi.org/10.1289/ehp.1409164.

Short-term effects of particulate matter on mortality during forest fires in Southern Europe: results of the MED-PARTICLES Project.

BACKGROUND: An association between occurrence of wildfires and mortality in the exposed population has been observed in several studies with controversial results for cause-specific mortality. In the Mediterranean area, forest fires usually occur during spring-summer, they overlap with Saharan outbreaks, are associated with increased temperature and their health effects are probably due to an increase in particulate matter. AIM AND METHODS: We analysed the effects of wildfires and particulate matter (PM10) on mortality in 10 southern European cities in Spain, France, Italy and Greece (2003-2010), using satellite data for exposure assessment and Poisson regression models, simulating a case-crossover approach. RESULTS: We found that smoky days were associated with increased cardiovascular mortality (lag 0-5, 6.29%, 95% CIs 1.00 to 11.85). When the effect of PM10 (per 10 µg/m(3)) was evaluated, there was an increase in natural mortality (0.49%), cardiovascular mortality (0.65%) and respiratory mortality (2.13%) on smoke-free days, but PM10-related mortality was higher on smoky days (natural mortality up to 1.10% and respiratory mortality up to 3.90%) with a suggestion of effect modification for cardiovascular mortality (3.42%, p value for effect modification 0.055), controlling for Saharan dust advections. CONCLUSIONS: Smoke is associated with increased cardiovascular mortality in urban residents, and PM10 on smoky days has a larger effect on cardiovascular and respiratory mortality than on other days.

Particulate matter and gaseous pollutants in the Mediterranean Basin: results from the MED-PARTICLES project.

Previous studies reported significant variability of air pollutants across Europe with the lowest concentrations generally found in Northern Europe and the highest in Southern European countries. Within the MED-PARTICLES project the spatial and temporal variations of long-term PM and gaseous pollutants data were investigated in traffic and urban background sites across Southern Europe. The highest PM levels were observed in Greece and Italy (Athens, Thessaloniki, Turin and Rome) while all traffic sites showed high NO2 levels, frequently exceeding the established limit value. High PM2.5/PM10 ratios were calculated indicating that fine particles comprise a large fraction of PM10, with the highest values found in the urban background sites. It seems that although in traffic sites the concentrations of both PM2.5 and PM10 are significantly higher than those registered in urban background sites, the coarse fraction PM2.5-10 is more important at the traffic sites. This fact is probably due to the high levels of resuspended road dust in sites highly affected by traffic, a phenomenon particularly relevant for Mediterranean countries. The long-term trends of air pollutants revealed a significant decrease of the concentration levels for PM, SO2 and CO while for NO2 no clear trend or slightly increasing trends were observed. This reduction could be attributed to the effectiveness of abatement measures and strategies and also to meteorological conditions and to the economic crisis that affected Southern Europe.

Partitioning of magnetic particles in PM10, PM2.5 and PM1 aerosols in the urban atmosphere of Barcelona (Spain).

A combined magnetic-chemical study of 15 daily, simultaneous PM10-PM2.5-PM1 urban background aerosol samples has been carried out. The magnetic properties are dominated by non-stoichiometric magnetite, with highest concentrations seen in PM10. Low temperature magnetic analyses showed that the superparamagnetic fraction is more abundant when coarse, multidomain particles are present, confirming that they may occur as an oxidized outer shell around coarser grains. A strong association of the magnetic parameters with a vehicular PM10 source has been identified. Strong correlations found with Cu and Sb suggests that this association is related to brake abrasion emissions rather than exhaust emissions. For PM1 the magnetic remanence parameters are more strongly associated with crustal sources. Two crustal sources are identified in PM1, one of which is of North African origin. The magnetic particles are related to this source and so may be used to distinguish North African dust from other sources in PM1.

Neural network model for the prediction of PM10 daily concentrations in two sites in the Western Mediterranean.

An artificial neural network (ANN) was developed and tested to forecast PM10 daily concentration in two contrasted environments in NE Spain, a regional background site (Montseny), and an urban background site (Barcelona-CSIC), which was highly influenced by vehicular emissions. In order to predict 24-h average PM10 concentrations, the artificial neural network previously developed by Caselli et al. (2009) was improved by using hourly PM concentrations and deterministic factors such as a Saharan dust alert. In particular, the model input data for prediction were the hourly PM10 concentrations 1-day in advance, local meteorological data and information about air masses origin. The forecasted performance indexes for both sites were calculated and they showed better results for the regional background site in Montseny (R(2)=0.86, SI=0.75) than for urban site in Barcelona (R(2)=0.73, SI=0.58), influenced by local and sometimes unexpected sources. Moreover, a sensitivity analysis conducted to understand the importance of the different variables included among the input data, showed that local meteorology and air masses origin are key factors in the model forecasts. This result explains the reason for the improvement of ANN's forecasting performance at the Montseny site with respect to the Barcelona site. Moreover, the artificial neural network developed in this work could prove useful to predict PM10 concentrations, especially, at regional background sites such as those on the Mediterranean Basin which are primarily affected by long-range transports. Hence, the artificial neural network presented here could be a powerful tool for obtaining real time information on air quality status and could aid stakeholders in their development of cost-effective control strategies.

Chemical fingerprint and impact of shipping emissions over a western Mediterranean metropolis: primary and aged contributions.

An intensive monitoring campaign was carried out in the harbor of Barcelona (Spain) to quantify the contribution of primary shipping emissions (PSE) on PM10. Chemical composition of inorganic species, as well as OC and EC, was completed, and a source apportionment analysis by Positive Matrix Factorization was conducted. Among the 6 sources extracted, two were linked to harbor emissions: dusty materials released in different areas along the harbor and fuel-oil combustion. On average, harbor emissions accounted for 31% of the PM10 mass. Since the chemical signature of PSE was not determined neither their contribution was obtained, additional approaches were followed and mainly consisted in: 1) the evaluation of V/Ni and V/Cu ratios to identify those days affected by PSE; 2) the identification of the chemical components increasing under the influence of PSE; 3) the calculation of the daily and average PSE from their experimentally-determined chemical signature and the experimental concentrations of vanadium. As a result, the contribution of PSE was estimated in 0.84 µg m(-3) (2.7% of PM10) and the residual fuel-oil combustion factor (3.6 µg m(-3), 12% of PM10) was interpreted as aged shipping emissions. The present study splits the contribution of shipping emissions into primary and aged, and highlights the importance of atmospheric mixing and aging processes in western Mediterranean atmospheres. In the case of shipping emissions, the aged products were found to be dominant with respect to the primary ones even in the vicinity of the source.

PM10 and PM2.5 sources at an insular location in the western Mediterranean by using source apportionment techniques.

PM10 and PM2.5 chemical composition has been determined at a suburban insular site in the Balearic Islands (Spain) during almost one and a half year. As a result, 200 samples with more than 50 chemical parameters analyzed have been obtained. The whole database has been analyzed by two receptor modelling techniques (Principal Component Analysis and Positive Matrix Factorisation) in order to identify the main PM sources. After that, regression analyses with respect to the PM mass concentrations were conducted to quantify the daily contributions of each source. Four common sources were identified by both receptor models: secondary nitrate coupled with vehicular emissions, secondary sulphate influenced by fuel-oil combustion, aged marine aerosols and mineral dust. In addition, PCA isolated harbour emissions and a mixed anthropogenic factor containing industrial emissions; whereas PMF isolated an additional mineral factor interpreted as road dust+harbour emissions, and a vehicular abrasion products factor. The use of both methodologies appeared complementary. Nevertheless, PMF sources by themselves were better differentiated. Besides these receptor models, a specific methodology to quantify African dust was also applied. The combination of these three source apportionment tools allowed the identification of 8 sources, being 4 of them mineral (African, regional, urban and harbour dusts). As a summary, 29% of PM10 was attributed to natural sources (African dust, regional dust and sea spray), whereas the proportion diminished to 11% in PM2.5. Furthermore, the secondary sulphate source, which accounted for about 22 and 32% of PM10 and PM2.5, is strongly linked to the aged polluted air masses residing over the western Mediterranean in the warm period.

Saharan dust, particulate matter and cause-specific mortality: a case-crossover study in Barcelona (Spain).

BACKGROUND: Studies measuring health effects of Saharan dust based on large particulate matter (PM) fraction groups may be masking some effects. Long distant transport reduces the amount of heavier and larger particles in the Saharan air masses increasing the relative contribution of smaller particles that may be more innocuous. This study investigates the association between different PM fractions and daily mortality during Saharan and non-Saharan days in Barcelona, Spain. METHODS: We collected daily PM(1), PM(2.5-1) and PM(10-2.5) fractions, and cause-specific mortality (cardiovascular, respiratory and cerebrovascular) between March 2003 and December 2007. Changes of effects between Saharan and non-Saharan dust days were assessed using a time-stratified case-crossover design. RESULTS: During non-Saharan dust days we found statistically significant (p<0.05) effects of PM(10-2.5) for cardiovascular (odds ratio for increase of an interquartile range, OR=1.033, 95% confidence interval: 1.006-1.060) and respiratory mortality (OR=1.044, 95% CI: 1.001-1.089). During Saharan dust days strongest cardiovascular effects were found for the same fraction (OR=1.085, 95% CI: 1.017-1.158) with an indication of effect modification (p=0.111). Effects of PM(2.5-1) during Saharan dust days were about the double than in non-dust days for cardiovascular and respiratory mortality, but these differences were not statistically significant. CONCLUSION: Our results using independent fractions of PMs provide further evidence that the effects of short-term exposure to PM during Saharan dust days are associated with both cardiovascular and respiratory mortality. A better understanding of which of the different PM size fractions brought by Saharan dust is more likely to accelerate adverse effects may help better understand mechanisms of toxicity.

Short-term effects of particulate matter on total mortality during Saharan dust outbreaks: a case-crossover analysis in Madrid (Spain).

BACKGROUND: The role of Saharan dust outbreaks on the relationship between particulate matter and daily mortality has recently been addressed in studies conducted in Southern Europe, although they have not given consistent results. METHODS: We investigated the effects of coarse (PM(10-2.5)) and fine particulate matter (PM(2.5)) in Madrid on total mortality during Saharan dust and non-dust days using a case-crossover design. RESULTS: During Saharan dust days, an increase of 10mg/m(3) of PM(10-2.5) raised total mortality by 2.8% compared with 0.6% during non-dust days (P-value for interaction=0.0165). CONCLUSION: We found evidence of stronger adverse health effects of PM(10-2.5) during Saharan dust outbreaks effects for impacted European populations, but not for PM(2.5). Further research is needed to understand mechanisms by which Saharan dust increases risk of mortality.

The effects of particulate matter sources on daily mortality: a case-crossover study of Barcelona, Spain.

BACKGROUND: Dozens of studies link acute exposure to particulate matter (PM) air pollution with premature mortality and morbidity, but questions remain about which species and sources in the vast PM mixture are responsible for the observed health effects. Although a few studies exist on the effects of species and sources in U.S. cities, European cities-which have a higher proportion of diesel engines and denser urban populations-have not been well characterized. Information on the effects of specific sources could aid in targeting pollution control and in articulating the biological mechanisms of PM. OBJECTIVES: Our study examined the effects of various PM sources on daily mortality for 2003 through 2007 in Barcelona, a densely populated city in the northeast corner of Spain. METHODS: Source apportionment for PM ≤ 2.5 µm and ≤ 10 µm in aerodynamic diameter (PM2.5 and PM10) using positive matrix factorization identified eight different factors. Case-crossover regression analysis was used to estimate the effects of each factor. RESULTS: Several sources of PM2.5, including vehicle exhaust, fuel oil combustion, secondary nitrate/organics, minerals, secondary sulfate/organics, and road dust, had statistically significant associations (p < 0.05) with all-cause and cardiovascular mortality. Also, in some cases relative risks for a respective interquartile range increase in concentration were higher for specific sources than for total PM2.5 mass. CONCLUSIONS: These results along with those from our multisource models suggest that traffic, sulfate from shipping and long-range transport, and construction dust are important contributors to the adverse health effects linked to PM.

Source apportionment of PM(10) and PM(2.5) at multiple sites in the strait of Gibraltar by PMF: impact of shipping emissions.

BACKGROUND: The impact of shipping emissions on urban agglomerations close to major ports and vessel routes is probably one of the lesser understood aspects of anthropogenic air pollution. Little research has been done providing a satisfactory comprehension of the relationship between primary pollutant emissions, secondary aerosols formation and resulting air quality. MATERIALS AND METHODS: In this study, multi-year (2003-2007) ambient speciated PM(10) and PM(2.5) data collected at four strategic sampling locations around the Bay of Algeciras (southern Spain), and positive matrix factorisation model were used to identify major PM sources with particular attention paid to the quantification of total shipping emissions. The impact of the emissions from both the harbour of Algeciras and vessel traffic at the Western entrance of Mediterranean Sea (Strait of Gibraltar) were quantified. Ambient levels of V, Ni, La and Ce were used as markers to estimate PM emitted by shipping. RESULTS AND DISCUSSION: Shipping emissions were characterised by La/Ce ratios between 0.6 and 0.8 and V/Ni ratios around 3 for both PM(10) and PM(2.5). In contrast, elevated La/Ce values (1-5) are attributable to emissions from refinery zeolitic fluid catalytic converter plant, and low average V/Ni values (around 1) result mainly from contamination from stainless steel plant emissions. The direct contribution from shipping in the Bay of Algeciras was estimated at 1.4-2.6 µg PM(10)/m(3) (3-7%) and 1.2-2.3 µg PM(2.5)/m(3) (5-10%). The total contribution from shipping (primary emissions + secondary sulphate aerosol formation) reached 4.7 µg PM(10)/m(3) (13%) and 4.1 µg PM(2.5)/m(3) (17%).