Air quality challenges in Central Asian urban areas: a PM2.5 source apportionment analysis in Dushanbe, Tajikistan.

This work presents the first comprehensive assessment of PM pollution sources in Dushanbe, Tajikistan. A total of 138 PM2.5 samples were collected during 2015-2016 and 2018-2019 and were analyzed through gravimetric, ED-XRF, and multi-wavelength absorption techniques. The results show that PM2.5 concentrations were substantially higher than the European annual limit value and WHO Air Quality Guidelines annual average value, with an average of 90.9 ± 68.5 µg m-3. The PMF application identified eight sources of pollution that influenced PM2.5 concentration levels in the area. Coal burning (21.3%) and biomass burning (22.3%) were the dominant sources during the winter, while vehicular traffic (7.7%) contributed more during the warm season. Power plant emissions (17.5%) showed enhanced contributions during the warm months, likely due to high energy demand. Cement industry emissions (6.9%) exhibited significant contribution during the cold period of 2018-2019, while soil dust (11.3%) and secondary sulphates (11.5%) displayed increased contribution during the warm and cold months, respectively. Finally, waste burning (1.5%) displayed the lowest contribution, with no significant temporal variation. Our results highlight the significant impact of anthropogenic activities, and especially the use of coal burning for energy production (both in power plants and for residential heating), and the significant contribution of biomass burning during both warm and cold seasons.

Widespread Pesticide Distribution in the European Atmosphere Questions their Degradability in Air.

Risk assessment of pesticide impacts on remote ecosystems makes use of model-estimated degradation in air. Recent studies suggest these degradation rates to be overestimated, questioning current pesticide regulation. Here, we investigated the concentrations of 76 pesticides in Europe at 29 rural, coastal, mountain, and polar sites during the agricultural application season. Overall, 58 pesticides were observed in the European atmosphere. Low spatial variation of 7 pesticides suggests continental-scale atmospheric dispersal. Based on concentrations in free tropospheric air and at Arctic sites, 22 pesticides were identified to be prone to long-range atmospheric transport, which included 15 substances approved for agricultural use in Europe and 7 banned ones. Comparison between concentrations at remote sites and those found at pesticide source areas suggests long atmospheric lifetimes of atrazine, cyprodinil, spiroxamine, tebuconazole, terbuthylazine, and thiacloprid. In general, our findings suggest that atmospheric transport and persistence of pesticides have been underestimated and that their risk assessment needs to be improved.

Aerosol characterization and peculiarities of source apportionment in Moscow, the largest and northernmost European megacity.

High population and a wide range of activities in a megacity lead to large-scale ecological consequences which require the assessment with respect to distinct characteristics of climate, location, fuel consumption, and emission sources. In-depth study of aerosol characteristics was carried out in Moscow, the largest megacity in Europe, during the cold period (autumn and winter) and in spring. PM10 chemical speciation based on carbonaceous matter, water-soluble ions, and elements was carried out to reconstruct the PM mass and evaluate the primary and secondary aerosol contribution. For the whole study period organic matter, mineral dust, and secondary inorganic/organic accounted for 34, 24, and 16 % of PM10 mass, respectively. PM10, OC, and EC approached a maximum in spring and decreased in winter. Mineral dust seasonal fraction increased from spring (17 %) to autumn (32 %), and then decreased in winter (22 %). Secondary inorganic aerosols (SIA) in opposite showed the maximum 27 % in winter. K+ marked the residential biomass burning in the region surrounding a megacity in spring and autumn, agriculture fires in spring. In winter primary aerosol contribution dropped down 56 % while secondary approached practically equal 44 %. Source factors with the relative contributions are quantified, namely city dust (26 %), traffic (23 %), industrial (20 %), biomass burning (12 %), secondary (12 %), and de-icing salt (7 %); they were significantly varying between the cold heating period and springtime. The relevance of sources to meteorological parameters and mass transportation is investigated by using both bivariate polar plots and Lagrangian integrated trajectory (HYSPLIT) model. Trajectory clustering demonstrates regional sources being crucial contributors to PM10 pollution. Aerosol speciation and source apportion factors identify the differences of the Moscow urban background among large European and Asian cities due to northern climate conditions, fast construction, long-range transport from industrial-developing area surrounding a city, regional biomass burning preferably in spring and autumn, and winter road management.

Wildfire and African dust aerosol oxidative potential, exposure and dose in the human respiratory tract.

Exposure to wildfire smoke and dust can severely affect air quality and health. Although particulate matter (PM) levels and exposure are well-established metrics linking to health outcomes, they do not consider differences in particle toxicity or deposition location in the respiratory tract (RT). Usage of the oxidative potential (OP) exposure may further shape our understanding on how different pollution events impact health. Towards this goal, we estimate the aerosol deposition rates, OP and resulting OP deposition rates in the RT for a typical adult Caucasian male residing in Athens, Greece. We focus on a period when African dust (1-3 of August 2021) and severe wildfires at the northern part of the Attika peninsula and the Evia island, Greece (4-18 of August 2021) affected air quality in Athens. During these periods, the aerosol levels increased twofold leading to exceedances of the World Health Organization (WHO) [15(5) µg m-3] PM10 (PM2.5) air quality standard by almost 100 %. We show that the OP exposure is 1.5-times larger during the wildfire smoke events than during the dust intrusion, even if the latter was present in higher mass loads - because wildfire smoke has a higher specific OP than dust. This result carries two important implications: OP exposure should be synergistically used with other metrics - such as PM levels - to efficiently link aerosol exposure with the resulting health effects, and, certain sources of air pollution (in our case, exposure to biomass burning smoke) may need to be preferentially controlled, whenever possible, owing to their disproportionate contribution to OP exposure and ability to penetrate deeper into the human RT.

Integrated Human Exposure to Air Pollution: A Step Further.

Along with climate change, air pollution is one of the biggest environmental problems affecting everyone in the world today [...].

Ambient air particulate total lung deposited surface area (LDSA) levels in urban Europe.

This study aims to picture the phenomenology of urban ambient total lung deposited surface area (LDSA) (including head/throat (HA), tracheobronchial (TB), and alveolar (ALV) regions) based on multiple path particle dosimetry (MPPD) model during 2017-2019 period collected from urban background (UB, n = 15), traffic (TR, n = 6), suburban background (SUB, n = 4), and regional background (RB, n = 1) monitoring sites in Europe (25) and USA (1). Briefly, the spatial-temporal distribution characteristics of the deposition of LDSA, including diel, weekly, and seasonal patterns, were analyzed. Then, the relationship between LDSA and other air quality metrics at each monitoring site was investigated. The result showed that the peak concentrations of LDSA at UB and TR sites are commonly observed in the morning (06:00-8:00 UTC) and late evening (19:00-22:00 UTC), coinciding with traffic rush hours, biomass burning, and atmospheric stagnation periods. The only LDSA night-time peaks are observed on weekends. Due to the variability of emission sources and meteorology, the seasonal variability of the LDSA concentration revealed significant differences (p = 0.01) between the four seasons at all monitoring sites. Meanwhile, the correlations of LDSA with other pollutant metrics suggested that Aitken and accumulation mode particles play a significant role in the total LDSA concentration. The results also indicated that the main proportion of total LDSA is attributed to the ALV fraction (50 %), followed by the TB (34 %) and HA (16 %). Overall, this study provides valuable information of LDSA as a predictor in epidemiological studies and for the first time presenting total LDSA in a variety of European urban environments.

The oxidative potential of particulate matter (PM) in different regions around the world and its relation to air pollution sources.

In this study, we investigated the impact of urban emission sources on the chemical composition of ambient particulate matter (PM) as well as the associated oxidative potential. We collected six sets of PM samples in five urban location sites around the world over long time periods varying from weeks to months, intentionally selected for their PM to be dominated by unique emission sources: (1) PM2.5 produced mainly by traffic emissions in central Los Angeles, United States (US); (2) PM2.5 dominated by biomass burning in Milan, Italy; (3) PM2.5 formed by secondary photochemical reactions thus dominated by secondary aerosols in Athens, Greece; (4) PM10 emitted by refinery and dust resuspension in Riyadh, Saudi Arabia (SA); (5) PM10 generated by dust storms in Riyadh, SA, and (6) PM2.5 produced mainly by industrial and traffic emissions in Beirut, Lebanon. The PM samples were chemically analyzed and their oxidative potential were quantified by employing the dithiothreitol (DTT) assay. Our results revealed that the Milan samples were rich in water soluble organic carbon (WSOC) and PAHs, even exceeding the levels measured on Los Angeles (LA) freeways. The PM in Athens was characterized by high concentrations of inorganic ions, specifically sulfate which was the highest of all PM samples. The ambient PM in LA was impacted by the traffic-emitted primary organic and elemental carbon. Furthermore, the contribution of metals and elements per mass of PM in Riyadh and Beirut samples were more pronounced relative to other sampling areas. The highest intrinsic PM redox activity was observed for PM with the highest WSOC fraction, including Milan (biomass burning) and Athens (secondary organic aerosols, SOA). PM in areas characterized by high metal emissions including dust events, refinery and industry, such as Riyadh and Beirut, had the lowest oxidative potential as assessed by the DTT assay. The results of this study illustrate the impact of major emission sources in urban areas on the redox activity and oxidative potential of ambient PM, providing useful information for developing efficient air pollution control and mitigation policies in polluted areas around the globe.

Source apportionment of children daily exposure to particulate matter.

The present study aims to investigate the sources of particulate pollution in indoor and outdoor environments, with focus on determining their contribution to the exposure of children to airborne particulate matter (PM). To this end, parallel indoor and outdoor measurements were carried out for a selection of 40 homes and 5 schools between September 2017 and October 2018. PM2.5 and PM2.5-10 samples were collected during five days in each microenvironment (ME) and analysed by X-Ray Fluorescence (XRF), for the determination of elements, and by a thermal-optical technique, for the measurement of organic and elemental carbon. The source apportionment analysis of the PM composition data, by means of the receptor model SoFi (Source Finder) 8 Pro, resulted in the identification of nine sources: exhaust and non-exhaust emissions from traffic, secondary particles, heavy oil combustion, industry, sea salt, soil, city dust, and an indoor source characterized by high levels of organic carbon. Integrated daily exposure to PM2.5 was on average 21 µg/m3. The organic matter, resulting from cleaning, cooking, smoking and biological material, was the major source contributing by 31% to the PM2.5 exposure. The source city dust, which was highly influenced by the resuspension of dust in classrooms, was the second main source (26%), followed by traffic (24%). The major sources affecting the integrated exposure to PM10, which was on average 33 µg/m3, were the city dust (39%), indoor organics (24%) and traffic (16%). This study provides important information for the design of measures to reduce the exposure of children to PM.

A new on-line SPE LC-HRMS method for the analysis of Perfluoroalkyl and Polyfluoroalkyl Substances (PFAS) in PM2.5 and its application for screening atmospheric particulates from Dublin and Enniscorthy, Ireland.

A sensitive analytical method has been developed and validated for the determination of 16 polyfluorinated alkyl substances (PFAS) in fine airborne particulate matter (PM2.5) using on-line solid phase extraction (SPE) coupled with liquid chromatography (LC) - negative electrospray ionisation high resolution mass spectrometry (-) ESI-HRMS. On-line SPE allows simultaneous sample clean-up from interfering matrices and lower limits of detection (LODs) by injecting a large volume of sample into the LC system without compromising chromatographic efficiency and resolution. The method provides LODs in the range 0.08-0.5 pg/mL of sample extract allowing detection of selected PFAS in aerosol particles at low fg/m3 level and showed good tolerance to the considered PM matrix. The validated method was applied for analysis of PFAS in ambient PM2.5 samples collected at two urban locations in Ireland, i.e., Enniscorthy and Dublin. Several PFAS were observed above the detection limit, including perfluorobutyrate (PFBA), perfluorooctanoic acid (PFOA), perfluorooctanesulfonic acid (PFOS), perfluorobutanesulfonic acid (L-PFBS) and perfluorononanoic acid (PFNA), as well as fluorotelomer sulfonates: 4:2 FTS, 6:2 FTS and 8:2 FTS. The results indicate that some toxic PFAS, such as PFOS and PFOA, are still detected in the environment despite being phased out from production and subject to restricted use in the EU and USA for more than two decades. Observation of fluorotelomer sulfonates (4:2 FTS, 6:2 FTS and 8:2 FTS, which are used as alternatives for legacy PFOA and PFOS) in ambient PM2.5 samples raises a concern about their persistence in the atmosphere and impact on human health considering emerging evidence that they could have similar health endpoints as PFOA and PFOS. To our knowledge, this is the first study to identify PFAS in ambient PM2.5 at urban locations in Ireland and also the first study to detect 4:2 and 8:2 fluorotelomer sulfonates in atmospheric aerosol particles.

Aerosol microphysics and chemistry reveal the COVID19 lockdown impact on urban air quality.

Air quality in urban areas and megacities is dependent on emissions, physicochemical process and atmospheric conditions in a complex manner. The impact on air quality metrics of the COVID-19 lockdown measures was evaluated during two periods in Athens, Greece. The first period involved stoppage of educational and recreational activities and the second severe restrictions to all but necessary transport and workplace activities. Fresh traffic emissions and their aerosol products in terms of ultrafine nuclei particles and nitrates showed the most significant reduction especially during the 2nd period (40-50%). Carbonaceous aerosol both from fossil fuel emissions and biomass burning, as well as aging ultrafine and accumulation mode particles showed an increase of 10-20% of average before showing a decline (5 to 30%). It is found that removal of small nuclei and Aitken modes increased growth rates and migration of condensable species to larger particles maintaining aerosol volume.

Analysis of spatial factors, time-activity and infiltration on outdoor generated PM2.5 exposures of school children in five European cities.

Atmospheric particles are a major environmental health risk. Assessments of air pollution related health burden are often based on outdoor concentrations estimated at residential locations, ignoring spatial mobility, time-activity patterns, and indoor exposures. The aim of this work is to quantify impacts of these factors on outdoor-originated fine particle exposures of school children. We apply nested WRF-CAMx modelling of PM2.5 concentrations, gridded population, and school location data. Infiltration and enrichment factors were collected and applied to Athens, Kuopio, Lisbon, Porto, and Treviso. Exposures of school children were calculated for residential and school outdoor and indoor, other indoor, and traffic microenvironments. Combined with time-activity patterns six exposure models were created. Model complexity was increased incrementally starting from residential and school outdoor exposures. Even though levels in traffic and outdoors were considerably higher, 80-84% of the exposure to outdoor particles occurred in indoor environments. The simplest and also commonly used approach of using residential outdoor concentrations as population exposure descriptor (model 1), led on average to 26% higher estimates (15.7 µg/m3) compared with the most complex model (# 6) including home and school outdoor and indoor, other indoor and traffic microenvironments (12.5 µg/m3). These results emphasize the importance of including spatial mobility, time-activity and infiltration to reduce bias in exposure estimates.

Integrated Human Exposure to Air Pollution.

Air pollution is one of the major environmental health problems that people face nowadays, affecting everyone in the world [...].

Chemical characterisation of particulate matter in urban transport modes.

Traffic is a main source of air pollutants in urban areas and consequently daily peak exposures tend to occur during commuting. Personal exposure to particulate matter (PM) was monitored while cycling and travelling by bus, car and metro along an assigned route in Lisbon (Portugal), focusing on PM2.5 and PM10 (PM with aerodynamic diameter <2.5 and 10 µm, respectively) mass concentrations and their chemical composition. In vehicles, the indoor-outdoor interplay was also evaluated. The PM2.5 mean concentrations were 28 ± 5, 31 ± 9, 34 ± 9 and 38 ± 21 µg/m3 for bus, bicycle, car and metro modes, respectively. Black carbon concentrations when travelling by car were 1.4 to 2.0 times higher than in the other transport modes due to the closer proximity to exhaust emissions. There are marked differences in PM chemical composition depending on transport mode. In particular, Fe was the most abundant component of metro PM, derived from abrasion of rail-wheel-brake interfaces. Enhanced concentrations of Zn and Cu in cars and buses were related with brake and tyre wear particles, which can penetrate into the vehicles. In the motorised transport modes, Fe, Zn, Cu, Ni and K were correlated, evidencing their common traffic-related source. On average, the highest inhaled dose of PM2.5 was observed while cycling (55 µg), and the lowest in car travels (17 µg). Cyclists inhaled higher doses of PM2.5 due to both higher inhalation rates and longer journey times, with a clear enrichment in mineral elements. The presented results evidence the importance of considering the transport mode in exposure assessment studies.

Relationship between indoor and outdoor size-fractionated particulate matter in urban microenvironments: Levels, chemical composition and sources.

Exposure to particulate matter (PM) has been associated with adverse health outcomes, particularly in susceptible population groups such as children. This study aims to characterise children's exposure to PM and its chemical constituents. Size-segregated aerosol samples (PM0.25, PM0.25-0.5, PM0.5-1.0, PM1.0-2.5 and PM2.5-10) were collected in the indoor and outdoor of homes and schools located in Lisbon (Portugal). Organic and elemental carbon (OC and EC) were determined by a thermo-optical method, whereas major and trace elements were analysed by X-Ray Fluorescence. In school, the children were exposed to higher PM concentrations than in home, which might be associated not only to the elevated human occupancy but also to outdoor infiltration. The pattern of PM mass size distribution was dependent on the location (home vs. school and indoor vs. outdoor). The presence of EC in PM0.25 and OC in PM0.25-0.5 was linked to traffic exhaust emissions. OC and EC in PM2.5-10 may be explained by their adhesion to the surface of coarser particles. Generally, the concentrations of mineral and marine elements increased with increasing PM size, while for anthropogenic elements happened the opposite. In schools, the concentrations of mineral matter, anthropogenic elements and marine aerosol were higher than in homes. High mineral matter concentrations found in schools were related to the close proximity to busy roads and elevated human occupancy. Overall, the results suggest that exposure to PM is relevant and highlights the need for strategies that provide healthier indoor environments, principally in schools.

Source apportionment of the oxidative potential of fine ambient particulate matter (PM2.5) in Athens, Greece.

The main objective of this study was chemical characterization and source apportionment of the oxidative potential of ambient PM2.5 samples collected in an urban background area in Athens, Greece. Ambient PM2.5 samples were collected during the summer (June-September) of 2017 and winter (February-March) of 2018 at a residential, urban background site in the outlying neighborhood of the Demokritos National Laboratory in Athens, Greece. The collected PM samples were analyzed for their chemical constituents including metals and trace elements, water-soluble organic carbon (WSOC), elemental and organic carbon (EC/OC), and marker of biomass burning (i.e., levoglucosan). In addition, the DCFH in vitro assay was performed to determine the oxidative potential of the PM2.5 samples. We performed a series of statistical analyses, including Spearman rank-order correlation analysis, principal component analysis (PCA), and multi linear regression (MLR) to determine the most significant species (as source tracers) contributing to the oxidative potential of PM2.5. Our findings revealed that the intrinsic (per PM mass) and extrinsic (per m3 of air volume) oxidative potentials of the collected ambient PM2.5 samples were significantly higher than those measured in many urban areas around the world. The results of the MLR analyses indicated that the major pollution sources contributing to the oxidative potential of ambient PM2.5 were vehicular emissions (characterized by EC) (44%), followed by secondary organic aerosol (SOA) formation (characterized by WSOC) (16%), and biomass burning (characterized by levoglucosan) (9%). The oxidative potential of the collected ambient PM2.5 samples was also higher in summer compared to the winter, mainly due to higher concentrations of EC and WSOC during this season. Results from this study corroborate the impact of traffic and SOA on the oxidative potential of ambient PM2.5 in greater Athens area, and can be helpful in adopting appropriate public health policies regarding detrimental outcomes of exposure to PM2.5.

Polycyclic aromatic hydrocarbons and their derivatives (nitro-PAHs, oxygenated PAHs, and azaarenes) in PM2.5 from Southern European cities.

Atmospheric particulate matter (PM2.5) samples were collected over two one month periods during winter and summer in three Southern European cities (Oporto - traffic site, Florence - urban background, Athens - suburban). Concentrations of 27 polycyclic aromatic hydrocarbons (PAHs), 15 nitro-PAHs (NPAHs), 15 oxygenated-PAHs (OPAHs) and 4 azaarenes (AZAs) were determined. On average, the winter-summer concentrations of ΣPAHs were 16.3-5.60, 7.75-3.02 and 3.44-0.658ngm-3 in Oporto, Florence and Athens, respectively. The corresponding concentrations of ΣNPAHs were 15.8-9.15, 10.9-3.36 and 15.9-2.73ngm-3, whilst ΣOPAHs varied in the ranges 41.8-19.0, 11.3-3.10 and 12.6-0.704ngm-3. Concentrations of ΣAZAs were always below 0.5ngm-3. Irrespective of the city, the dominant PAHs were benzo[b+j+k]fluoranthene, retene, benzo[ghi]perylene and indeno[1,2,3-cd]pyrene. The most abundant OPAH in all cities was 1,8-naphthalic anhydride, whereas 5-nitroacenaphthene was the prevailing NPAH. The ΣOPAHs/ΣPAHs and ΣNPAHs/ΣPAHs were higher in summer than in winter, suggesting increasing formation of derivatives by photochemical degradation of PAHs. Molecular diagnostic ratios suggested that, after traffic, biomass burning was the dominant emission source. Apart from being influenced by seasonal sources, the marked differences between winter and summer may indicate that these diagnostic ratios are particularly sensitive to photodegradation, and thus should be applied and interpreted cautiously. The lifetime excess cancer risk from inhalation was, in part, attributable to PAH derivatives, acclaiming the need to include these compounds in regular monitoring programmes. On average, 206, 88 and 26 cancer cases per million people were estimated, by the World Health Organisation method, for the traffic-impacted, urban background and suburban atmospheres of Oporto, Florence and Athens, respectively.

Characterization of PM2.5 chemical composition at the Demokritos suburban station, in Athens Greece. The influence of Saharan dust.

The aim of this work is to study the atmospheric concentrations of selected major and trace elements and ions found in PM2.5, at a suburban site in Athens, Greece, and discuss on the impact of the different sources. Special focus is given to the influence of Saharan dust episodes. The seasonal variability in the metal and ion concentrations is also examined. The results show that PM2.5 mass concentrations are significantly influenced by Saharan dust events; it is observed that when the PM2.5 concentration is higher than 25 µg/m3, five out of six times, the air mass crossed North Africa at an altitude within the boundary layer. Fe is found to be the element with the more significant seasonal variability, displaying much higher concentrations during cold period. The frequent Saharan dust intrusions in the cold period of this dataset may explain this result. Mineral dust and secondary aerosol are the main PM2.5 components (29 and 34%, respectively). During Saharan dust events, the concentration of mineral dust is increased by 35% compared to the days without dust intrusions, while an increase of 68% of the sea salt is also observed. During event days, PM2.5 concentrations are also increased by 14%. Anthropogenic components do not decrease during those days, while sulfate displays even a slight increase, suggesting enrichment of mineral dust with secondary sulfates. The results indicate that African dust intrusions add a rather significant PM pollution load even in the PM2.5 fraction, with implication to population exposure and human health.

Factors controlling air quality in different European subway systems.

Sampling campaigns using the same equipment and methodology were conducted to assess and compare the air quality at three South European subway systems (Barcelona, Athens and Oporto), focusing on concentrations and chemical composition of PM2.5 on subway platforms, as well as PM2.5 concentrations inside trains. Experimental results showed that the mean PM2.5 concentrations widely varied among the European subway systems, and even among different platforms within the same underground system, which might be associated to distinct station and tunnel designs and ventilation systems. In all cases PM2.5 concentrations on the platforms were higher than those in the urban ambient air, evidencing that there is generation of PM2.5 associated with the subway systems operation. Subway PM2.5 consisted of elemental iron, total carbon, crustal matter, secondary inorganic compounds, insoluble sulphate, halite and trace elements. Of all metals, Fe was the most abundant, accounting for 29-43% of the total PM2.5 mass (41-61% if Fe2O3 is considered), indicating the existence of an Fe source in the subway system, which could have its origin in mechanical friction and wear processes between rails, wheels and brakes. The trace elements with the highest enrichment in the subway PM2.5 were Ba, Cu, Mn, Zn, Cr, Sb, Sr, Ni, Sn, Co, Zr and Mo. Similar PM2.5 diurnal trends were observed on platforms from different subway systems, with higher concentrations during subway operating hours than during the transport service interruption, and lower levels on weekends than on weekdays. PM2.5 concentrations depended largely on the operation and frequency of the trains and the ventilation system, and were lower inside the trains, when air conditioning system was operating properly, than on the platforms. However, the PM2.5 concentrations increased considerably when the train windows were open. The PM2.5 levels inside the trains decreased with the trains passage in aboveground sections.

The risks of acute exposure to black carbon in Southern Europe: results from the MED-PARTICLES project.

OBJECTIVES: While several studies have reported associations of daily exposures to PM2.5 (particles less than 2.5 µm) with mortality, few studies have examined the impact of its constituents such as black carbon (BC), which is also a significant contributor to global climate change. METHODS: We assessed the association between daily concentrations of BC and total, cardiovascular and respiratory mortality in two southern Mediterranean cities. Daily averages of BC were collected for 2 years in Barcelona, Spain and Athens, Greece. We used case-crossover analysis and examined single and cumulative lags up to 3 days. RESULTS: We observed associations between BC and all mortality measures. For a 3-day moving average, cardiovascular mortality increased by 4.5% (95% CI 0.7 to 8.5) and 2.0% (95% CI 0 to 4.0) for an interquartile change in BC in Athens and Barcelona, respectively. Considerably higher effects for respiratory mortality and for those above age 65 were observed. In addition, BC exhibited much greater toxicity per microgram than generic PM2.5. CONCLUSIONS: Our findings suggest that BC, derived in western industrialised nations primarily from diesel engines and biomass burning, poses a significant burden to public health, particularly in European cities with high-traffic density.