Abstract. Levels of PM10, PM2.5 and PM1 and chemical speciation of PM10 and PM2.5 were measured during the MILAGRO campaign (1st to 31st March 2006, but extended in some cases until 6th April) at four urban, one suburban, two rural background and two rural sites, with different degree of industrial influence, in the Mexico City Metropolitan Area (MCMA) and adjacent regions. PM10 and PM2.5 daily levels varied between 50–56μg/m3 and 24–46μg/m3 at the urban sites, 22–35μg/m3 and 13–25μg/m3 at the rural sites, and 75μg/m3 and 31μg/m3 at the industrial hotspot, lower than those recorded at some Asian mega-cities and similar to those recorded at other Latin American cities. At the urban sites, hourly PM2.5 and PM1 concentrations showed a marked impact of road traffic emissions (at rush hours), with levels of coarse PM remaining elevated during daytime. At the suburban and rural sites different PM daily patterns were registered according to the influence of the pollution plume from MCMA, and also of local soil resuspension. The speciation studies showed that mineral matter accounted for 25–27% of bulk PM10 at the urban sites and a higher proportion (up to 43%) at the suburban and rural sites. This pattern is repeated in PM2.5, with 15% at urban and 28% at suburban and rural sites. Carbonaceous compounds accounted for a significant proportion at the urban and industrial sites (32–46% in PM10, and 51–55% in PM2.5), markedly reduced at the suburban and rural sites (16–23% in PM10, and 30% in PM2.5). The secondary inorganic aerosols accounted for 10–20% of bulk PM10 at urban, suburban, rural and industrial sites, with a higher proportion (40%) at the industrial background site. A relatively high proportion of nitrate in rural sites was present in the coarse fraction. Typically anthropogenic elements (As, Cr, Zn, Cu, Pb, Sn, Sb, Ba, among others) showed considerably high levels at the urban sites; however levels of particulate Hg and crustal trace elements (Rb, Ti, La, Sc, Ga) were generally higher at the suburban site. Principal component analysis identified three major common factors: crustal, regional background and road traffic. Moreover, some specific factors were obtained for each site.
Abstract. The main objective of this study is the identification of major factors controlling levels and chemical composition of aerosols in the regional background (RB) along the Mediterranean Basin (MB). To this end, data on PM levels and speciation from Montseny (MSY, NE Spain), Finokalia (FKL, Southern Greece) and Erdemli (ERL, Southern Turkey) for the period 2001 to 2008 are evaluated. Important differences on PM levels and composition are evident when comparing the Western and Eastern MBs. The results manifest W-E and N-S PM 10 and PM 2.5 gradients along the MB, attributed to the higher frequency and intensity of African dust outbreaks in the EMB, while for PM 1 very similar levels are encountered.PM in the EMB is characterized by higher levels of crustal material and sulphate as compared to WMB (and central European sites), however, RB nitrate and OC + EC levels are relatively constant across the Mediterranean and lower than other European sites. Marked seasonal trends are evidenced for PM levels, nitrate (WMB), ammonium and sulphate. Also relatively higher levels of V and Ni (WMB) are measured in the Mediterranean basin, probably as a consequence of high emissions from fuel-oil combustion (power generation, industrial and shipping emissions).Enhanced sulphate levels in EMB compared to WMB were measured. The high levels of sulphate in the EMB may deplete the available gas-phase NH 3 so that little ammonium nitrate can form due to the low NH 3 levels.Correspondence to: X. Querol (xavier.querol@idaea.csic.es) This study illustrates the existence of three very important features within the Mediterranean that need to be accounted for when modeling climate effects of aerosols in the area, namely: a) the increasing gradient of dust from WMB to EMB; b) the change of hygroscopic behavior of mineral aerosols (dust) via nitration and sulfation; and c) the abundance of highly hygroscopic aerosols during high insolation (low cloud formation) periods.
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.
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The occurrence of African dust outbreaks over the whole Mediterranean Basin has been identified on an 11-yr period (2001–2011). In order to evaluate the impact of such mineral dust outbreaks on ambient concentrations of particulate matter, PM10 data from regional and suburban background sites across the Mediterranean area were compiled. After identifying the daily influence of African dust, a methodology for estimating natural dust contributions on daily PM10 concentrations was applied. Our results reveal that African dust outbreaks occur with much higher frequency in southern areas of the Mediterranean, from 30 to 37% of the annual days, whereas they take place less than 20% of the annual days in northern sites. The central Mediterranean emerges as a transitional area, with slightly higher frequency of dust episodes in its lower extreme when compared to equivalent areas in western and eastern sides of the Basin. A decreasing south to north gradient of African dust contribution to PM10 is patent across the Mediterranean. Our study demonstrates that this gradient may be mainly explained by the latitudinal position. A longitudinal increasing trend of African dust contribution to PM10 is also observed from 25° E eastwards, and is due to the annual occurrence of intense dust episodes. Thus, the slightly higher frequency of African dust episodes over the lower part of Central Mediterranean is compensated by its moderately lower intensity. Concerning seasonality patterns and intensity characteristics, a clear summer prevalence is observed in the western part, with low occurrence of severe episodes (daily dust averages over 100 μg m−3 in PM10); no seasonal trend is detected in the central region, with moderate-intensity episodes; and significantly higher contributions are common in autumn-spring in the eastern side, with yearly occurrence of various severe episodes. Overall, African dust emerges as the largest PM10 source in regional background southern areas of the Mediterranean (35–50% of PM10), with seasonal peak contributions to PM10 up to 80% of the total mass.
The multi-year study of African dust episodes and their contributions to PM10 concentrations allowed us to identify a consistent decreasing trend in the period 2006/2007 to 2011 in 4 of the 17 studied regions, all of them located in the NW of the Mediterranean. The observed trend is almost parallel to the NAO (North Atlantic Oscillation) index for the summer period, progressively more negative since 2006 onwards. As a consequence, a sharp change in the atmospheric circulation over the last 5 yr (a similar negative NAO period occurred in the 1950 decade) have affected the number of African dust episodes and their mean contribution to PM10 in the NW part of the Mediterranean. The investigation of summer temperatures at 850 hPa suggest that warm air accomplishing African dust air masses moved anomalously through the central Mediterra...
We present results from the international field campaign DAURE (Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean), with the objective of apportioning the sources of fine carbonaceous aerosols. Submicron fine particulate matter (PM<sub>1</sub>) samples were collected during February-March 2009 and July 2009 at an urban background site in Barcelona (BCN) and at a forested regional background site in Montseny (MSY). We present radiocarbon (<sup>14</sup>C) analysis for elemental and organic carbon (EC and OC) and source apportionment for these data. We combine the results with those from component analysis of aerosol mass spectrometer (AMS) measurements, and compare to levoglucosan-based estimates of biomass burning OC, source apportionment of filter data with inorganic+EC+OC speciation, submicron bulk potassium (K) concentrations, and gaseous acetonitrile concentrations. <br></br> At BCN, 87 % and 91 % of the EC on average, in winter and summer, respectively, had a fossil origin, whereas at MSY these fractions were 66 % and 79 %. The contribution of fossil sources to organic carbon (OC) at BCN was 40 % and 48 %, in winter and summer, respectively, and 31 % and 25 % at MSY. The combination of results obtained using the <sup>14</sup>C technique, AMS data, and the correlations between fossil OC and fossil EC imply that the fossil OC at Barcelona is ~65 % primary whereas at MSY the fossil OC is mainly secondary (~85 %). Day-to-day variation in total carbonaceous aerosol loading and the relative contributions of different sources predominantly depended on the meteorological transport conditions. The estimated biogenic secondary OC at MSY only increased by ~40 % compared to the order-of-magnitude increase observed for biogenic volatile organic compounds (VOCs) between winter and summer, which highlights the uncertainties in the estimation of that component. Biomass burning contributions estimated using the <sup>14</sup>C technique ranged from similar to higher than when estimated using other techniques, and the different estimations were highly or moderately correlated. Differences can be explained by the contribution of secondary organic matter (not included in the primary biomass burning source estimates), and/or by an overestimation of the biomass burning OC contribution by the <sup>14</sup>C technique if the estimated biomass burning EC/OC ratio used for the calculations is too high for this region. Acetonitrile concentrations correlate well with the biomass burning EC determined by <sup>14</sup>C. K is a noisy tracer for biomass burning
We offer an overview of the COVID-19 -driven air quality changes across 11 metropolises in Spain with the focus on lessons learned on how continuing abating pollution. Traffic flow decreased by up to 80% during the lockdown and remained relatively low during the full relaxation (June and July). After the lockdown a significant shift from public transport to private vehicles (+21% in Barcelona) persisted due to the pervasive fear that using public transport might increase the risk of SARS-CoV-2 infection, which need to be reverted as soon as possible. NO 2 levels fell below 50% of the WHO annual air quality guidelines (WHOAQGs), but those of PM 2.5 were reduced less than expected due to the lower contributions from traffic, increased contributions from agricultural and domestic biomass burning, or meteorological conditions favoring high secondary aerosol formation yields. Even during the lockdown, the annual PM 2.5 WHOAQG was exceeded in cities within the NE and E regions with high NH 3 emissions from farming and agriculture. Decreases in PM 10 levels were greater than in PM 2.5 due to reduced emissions from road dust, vehicle wear, and construction/demolition. Averaged O 3 daily maximum 8-h (8hDM) experienced a generalized decrease in the rural receptor sites in the relaxation (June–July) with −20% reduced mobility. For urban areas O 3 8hDM responses were heterogeneous, with increases or decreases depending on the period and location. Thus, after canceling out the effect of meteorology, 5 out of 11 cities experienced O 3 decreases during the lockdown, while the remaining 6 either did not experience relevant reductions or increased. During the relaxation period and coinciding with the growing O 3 season (June–July), most cities experienced decreases. However, the O 3 WHOAQG was still exceeded during the lockdown and full relaxation periods in several cities. For secondary pollutants, such as O 3 and PM 2.5 , further chemical and dispersion modeling along with source apportionment techniques to identify major precursor reduction targets are required to evaluate their abatement potential.
Abstract.A physicochemical characterization, including aerosol number size distribution, chemical composition and mass concentrations, of the urban fine aerosol captured in MILAN, BARCELONA and LONDON is presented in this article. The objective is to obtain a comprehensive picture of the microphysical processes involved in aerosol dynamics during the: 1) regular evolution of the urban aerosol (daily, weekly and seasonal basis) and in the day-to-day variations (from clean-air to pollution-events), and 2) the link between "aerosol chemistry and mass concentrations" with the "number size distribution".The mass concentrations of the fine PM 2.5 aerosol exhibit a high correlation with the number concentration of >100 nm particles N>100 (nm) ("accumulation mode particles") which only account for <20% of the total number concentration N of fine aerosols; but do not correlate with the number of <100 nm particles ("ultrafine particles"), which accounts for >80% of fine particles number concentration. Organic matter and black-carbon are the only aerosol components showing a significant correlation with the ultrafine particles, attributed to vehicles exhausts emissions; whereas ammonium-nitrate, ammonium-sulphate and also organic matter and black-carbon correlate with N>100 (nm) and attributed to condensation mechanisms, other parCorrespondence to: S. Rodríguez (srodriguez@inm.es) ticle growth processes and some primary emissions. Time series of the aerosol DpN diameter (dN/dlogD mode), mass PM 2.5 concentrations and number N>100 (nm) concentrations exhibit correlated day-to-day variations, which point to a significant involvement of condensation of semi-volatile compounds during urban pollution events. This agrees with the observation that ammonium-nitrate is the component exhibiting the highest increases from mid-to-high pollution episodes, when the highest DpN increases are observed. The results indicates that "fine PM 2.5 particles urban pollution events" tend to occur when condensation processes have made particles grow large enough to produce significant number concentrations of N>100 (nm) ("accumulation mode particles"). In contrast, because the low contribution of ultrafine particles to the fine aerosol mass concentrations, high "ultrafine particles N<100(nm) events" frequently occurs under low PM 2.5 conditions. The results of this study demonstrate that vehicles exhausts emissions are strongly involved in this ultrafine particles aerosol pollution.
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