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Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter < 2.5 μm) resolved aerosol samples analysed by Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie European Union framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the approach used is the simultaneous sampling at two monitoring sites in Barcelona (Spain) during September-October 2010: an urban background site (UB) and a street canyon traffic road site (RS). Elements related to primary non-exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (regional sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non-exhaust brake dust (Fe-Cu) - 7%), and three types of industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%, percentages presented are average source contributions to the total elemental mass measured). The validity of the PMF solution of the PIXE data is supported by very good correlations with external single particle mass spectrometry measurements. Some important conclusions can be drawn about the PM2.5 mass fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial aerosol plumes associated with shipping oil combustion and smelters activities have a higher impact on the more ventilated UB site; (3) a unique source of Pb-Cl (associated with combustion emissions) is found to be the major (82%) source of fine Cl in the urban agglomerate; (4) the mean diurnal variation of PM2.5 primary traffic non-exhaust brake dust (Fe-Cu) suggests that this source is mainly emitted and not resuspended, whereas PM2.5 urban dust (Ca) is found mainly resuspended by both traffic vortex and sea breeze; (5) urban dust (Ca) is found the aerosol source most affected by land wetness, reduced by a factor of eight during rainy days and suggesting that wet roads may be a solution for reducing urban dust concentrations.

Measurements of aerosol chemical composition made on the island of Lampedusa, south of the Sicily channel, during years 2004–2008, are used to identify the influence of heavy fuel oil (HFO) combustion emissions on aerosol particles in the Central Mediterranean. Aerosol samples influenced by HFO are characterized by elevated Ni and V soluble fraction (about 80% for aerosol from HFO combustion, versus about 40% for crustal particles), high V and Ni to Si ratios, and values of Vsol>6 ng m−3. Evidence of HFO combustion influence is found in 17% of the daily samples. Back trajectories analysis on the selected events show that air masses prevalently come from the Sicily channel region, where an intense ship traffic occurs. This behavior suggests that single fixed sources like refineries are not the main responsible for the elevated V and Ni events, which are probably mainly due to ships emissions. Vsol, Nisol, and non-sea salt SO42− (nssSO42−) show a marked seasonal behaviour, with an evident summer maximum. Such a pattern can be explained by several processes: (i) increased photochemical activity in summer, leading to a faster production of secondary aerosols, mainly nssSO42−, from the oxidation of SO2 (ii) stronger marine boundary layer (MBL) stability in summer, leading to higher concentration of emitted compounds in the lowest atmospheric layers. A very intense event in spring 2008 was studied in detail, also using size segregated chemical measurements. These data show that elements arising from heavy oil combustion (V, Ni, Al, Fe) are distributed in the sub-micrometric fraction of the aerosol, and the metals are present as free metals, carbonates, oxides hydrates or labile complex with organic ligands, so that they are dissolved in mild condition (HNO3, pH1.5). Data suggest a characteristic nssSO42−/V ratio in the range 200–400 for HFO combustion aerosols in summer at Lampedusa. By using the value of 200 a lower limit for the HFO contribution to total sulphates is estimated. HFO combustion emissions account, as a summer average, at least for 1.2 μg m−3, representing about 30% of the total nssSO42−, 3.9% of PM10, 8% of PM2.5, and 11% of PM1. Within the used dataset, sulphate from HFO combustion emissions reached the peak value of 6.1 μg m−3 on 26 June 2008, when it contributed by 47% to nssSO42−, and by 15% to PM10.

The Mediterranean Basin atmosphere is influenced by both strong natural and anthropogenic aerosol emissions and is also subject to important climatic forcings. Several programs have addressed the study of the Mediterranean basin; nevertheless important pieces of information are still missing. In this framework, PM10 samples were collected on a daily basis on the island of Lampedusa (35.5 degree N, 12.6 degree E; 45 m a.s.l.), which is far from continental pollution sources (the nearest coast, in Tunisia, is more than 100 km away). After mass gravimetric measurements, different portions of the samples were analyzed to determine the ionic content by ion chromatography (IC), the soluble metals by inductively coupled plasma atomic emission spectrometry (ICP-AES), and the total (soluble + insoluble) elemental composition by particle-induced x-ray emission (PIXE). Data from 2007 and 2008 are used in this study. The Positive Matrix Factorization (PMF) model was applied to the 2-year long data set of PM10 mass concentration and chemical composition to assess the aerosol sources affecting the central Mediterranean basin. Seven sources were resolved: sea salt, mineral dust, biogenic emissions, primary particulate ship emissions, secondary sulfate, secondary nitrate, and combustion emissions. Source contributions to the total PM10 mass were estimated to be about 40 % for sea salt, around 25 % for mineral dust, 10 % each for secondary nitrate and secondary sulfate, and 5 % each for primary particulate ship emissions, biogenic emissions, and combustion emissions. Large variations in absolute and relative contributions are found and appear to depend on the season and on transport episodes. In addition, the secondary sulfate due to ship emissions was estimated and found to contribute by about one-third to the total sulfate mass. Results for the sea-salt and mineral dust sources were compared with estimates of the same contributions obtained from independent approaches, leading to an estimate of the water content bound to the sea salt in the marine source.

Size and time-resolved roadside enrichments of atmospheric particulate pollutants in PM10 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 PM10 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 hourly-resolved 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 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.

This study aims to determine the mineral contribution to PM10 in the central Mediterranean Sea, based on 7 yr of daily PM10 samplings made on the island of Lampedusa (35.5° N, 12.6° E). The chemical composition of the PM10 samples was determined by ion chromatography for the main ions, and, on selected samples, by particle-induced X-ray emission (PIXE) for the total content of crustal markers. Aerosol optical depth measurements were carried out in parallel to the PM10 sampling. The average PM10 concentration at Lampedusa over the period June 2004–December 2010 is 31.5 μg m−3, with low interannual variability. The annual means are below the EU annual standard for PM10, but 9.9% of the total number of daily data exceeds the daily threshold value established by the European Commission for PM (50 μg m−3, European Community, EC/30/1999). The Saharan dust contribution to PM10 was derived by calculating the contribution of Al, Si, Fe, Ti, non-sea-salt (nss) Ca, nssNa, and nssK oxides in samples in which PIXE data were available. Cases in which crustal content exceeded the 75th percentile of the crustal oxide content distribution were identified as elevated dust events. Using this threshold, we obtained 175 events. Fifty-five elevated dust events (31.6%) displayed PM10 higher than 50 μg m−3, with dust contributing by 33% on average. The crustal contribution to PM10 has an annual average value of 5.42 μg m−3, and reaches a value as high as 67.9 μg m−3 (corresponding to 49% of PM10) during an intense Saharan dust event. The crustal content estimated from a single tracer, such as Al or Ca, is in good agreement with the one calculated as the sum of the metal oxides. Conversely, larger crustal contents are derived by applying the EU guidelines for demonstration and subtraction of exceedances in PM10 levels due to high background of natural aerosol. The crustal aerosol amount and contribution to PM10 showed a very small seasonal dependence; conversely, the dust columnar burden displays an evident annual cycle, with a strong summer maximum (monthly average aerosol optical depth at 500 nm up to 0.28 in June–August). We found that 71.3% of the dust events identified from optical properties over the atmospheric column display a high dust content at the ground level. Conversely, the remaining 28.7% of cases present a negligible or small impact on the surface aerosol composition due to the transport processes over the Mediterranean Sea, where dust frequently travels above the marine boundary layer, especially in summer. Based on backward trajectories, two regions, one in Algeria–Tunisia, and one in Libya, are identified as main source areas for intense dust episodes occurring mainly in autumn and winter. Data on the bulk composition of mineral aerosol arising from these two source areas are scarce; results on characteristic ratios between elements show somewhat higher values of Ca / Al and (Ca + Mg) / Fe (2.5 ± 1.0, and 4.7 ± 2.0, respectively) for Algeria–Tunisia than for Libyan origin (Ca / Al = 1.9 ± 0.7 and (Ca + Mg) / Fe = 3.3 ± 1.1).

The LABEC laboratory, the INFN ion beam laboratory of nuclear techniques for environment and cultural heritage, located in the Scientific and Technological Campus of the University of Florence in Sesto Fiorentino, started its operational activities in 2004, after INFN decided in 2001 to provide our applied nuclear physics group with a large laboratory dedicated to applications of accelerator-related analytical techniques, based on a new 3 MV Tandetron accelerator. The new accelerator greatly improved the performance of existing Ion Beam Analysis (IBA) applications (for which we were using since the 1980s an old single-ended Van de Graaff accelerator) and in addition allowed to start a novel activity of Accelerator Mass Spectrometry (AMS), in particular for 14 C dating. Switching between IBA and AMS operation became very easy and fast, which allowed us high flexibility in programming the activities, mainly focused on studies of cultural heritage and atmospheric aerosol composition, but including also applications to biology, geology, material science and forensics, ion implantation, tests of radiation damage to components, detector performance tests and low-energy nuclear physics. This paper describes the facilities presently available in the LABEC laboratory, their technical features and some success stories of recent applications.

Airborne particulate matter is a serious threat to human health, especially in fast-growing cities. In this study, we carried out a magnetic and elemental study on tree leaves used as passive captors and urban dust from various sites in the city of Santiago, Chile, to assess the reliability of magnetic and elemental measurements to characterize particulate matter pollution from vehicular origin. We found that the magnetic susceptibility and saturation isothermal remanent magnetization measured on urban tree leaves is a good proxy for tracing anthropogenic metallic particles and allow controlling the exposure time for particulate matter collection, in agreement with other studies carried out in large cities. Similar measurements on urban soil can be influenced by particles of detritic (natural) origin, and therefore, magnetic measurements on tree leaves can help to identify hotspots where fine particles are more abundant. Elemental particle-induced X-ray emission analysis of tree leaves showed the presence of a number of elements associated with vehicular emissions, in particular Cu, Zn, Fe, K and S which are present at every site, and As, Se, V, Ni, Sr, Zr, Mo and Pb identified at some sites. We observed a correlation between magnetic parameters and the concentrations of S and Br as well as Cu to a smaller extent. Moreover, this study shows the importance of selecting carefully the tree species as well as the location of trees in order to optimize phytoremediation.

Seasonal changes in the levels of PM 1 and its main components (organic carbon (OC), elemental carbon (EC), SO 4 2− , NO 3 − and NH 4 + ) were studied in an urban street canyon in southeastern Spain. Although PM 1 levels did not show an evident seasonal cycle, strong variations in the concentrations of its major components were observed. Ammonium sulfate, the main secondary inorganic compound, was found to be of regional origin. Its formation was favored during summer due to increased photochemical activity. In contrast, the concentrations of particulate ammonium nitrate, which is thermally unstable, were highest in winter. Although traffic emissions are the dominant source of EC in the city, variations in traffic intensity could not explain the seasonal cycle of this component. The higher EC concentrations during the cold months were attributed to the lower dispersion conditions and the increase in EC emissions. Special attention has been given to variations in organic carbon levels since it accounted for about one third of the total PM 1 mass. The concentrations of both total OC and secondary OC (SOC) were maxima in winter. The observed seasonal variation in SOC levels is similar to that found in other southern European cities where the frequency of sunny days in winter is high enough to promote photochemical processes.

The regular eastward drift of transboundary aerosol intrusions from the Asian mainland into the NW Pacific region has a pervasive impact on air quality in Japan, especially during springtime. Analysis of 24-h filter samples with Inductively Coupled Plasma Atomic Emission Spectroscopy (ICP-AES) and Mass Spectrometry (ICP-MS), and hourly Streaker with Particle Induced X-ray Emission (PIXE) samples collected continuously for six weeks reveal the chemistry of successive waves of natural mineral desert dust (\"Kosa\") and metalliferous sulphatic pollutants arriving in western Japan during spring 2011. The main aerosol sources recognised by Positive Matrix Factorization (PMF) analysis of Streaker data are mineral dust and fresh sea salt (both mostly in the coarser fraction PM2.5–10), As-bearing sulphatic aerosol (PM0.1–2.5), metalliferous sodic particulate matter (PM) interpreted as aged, industrially contaminated marine aerosol, and ZnCu-bearing aerosols. Whereas mineral dust arrivals are typically highly transient, peaking over a few hours, sulphatic intrusions build up and decline more slowly, and are accompanied by notable rises in ambient concentrations of metallic trace elements such as Pb, As, Zn, Sn and Cd. The magnitude of the loss in regional air quality due to the spread and persistence of pollution from mainland Asia is especially clear when cleansing oceanic air advects westward across Japan, removing the continental influence and reducing concentrations of the undesirable metalliferous pollutants by over 90%. Our new chemical database, especially the Streaker data, demonstrates the rapidly changing complexity of ambient air inhaled during these transboundary events, and implicates Chinese coal combustion as the main source of the anthropogenic aerosol component.

The aim of the present study is to evaluate the possible influence of cement works on carbonaceous aerosol concentrations in the western Mediterranean. A PM 2.5 and PM 10 sampling campaign was performed between September 2005 and August 2006 in a suburban area close to two cement plants in southeastern Spain. All the samples were analyzed for elemental carbon (EC) and organic carbon (OC) using a thermal-optical method. The percentage contribution of total carbon to annual PM mass concentrations was 20 % for PM 2.5 and 10 % for PM 10 . These values were lower than those reported for other European urban and industrial locations because of a higher proportion of crustal matter and secondary inorganic aerosols in the study area. The seasonal cycle of OC concentrations, with higher values in winter than in summer, was influenced by the transport of cement plants’ emissions to the sampling site, as corroborated by the results obtained from the CPF analysis. In contrast, no clear effect of cement plants’ emissions on EC concentrations could be established. The concentrations of secondary organic carbon (SOC) in the PM 2.5 fraction were estimated using the EC tracer method. The contribution of SOC to the annual OC concentration was 50 %, varying between 30 % in July and 70 % in February. Contrary to expectations, SOC levels also exhibited a summer minimum, suggesting that photochemistry cannot be considered to be the leading factor in the formation of secondary organic aerosols in the research area.