ALBERT

Description: The time variability and long term trends of PM2.5 (particulate matter of diameter 〈 2.5 μm) at various regional background (RB) sites across Europe are studied and interpreted in this work. Data on mean annual levels of PM2.5 measured at Montseny (MSY, North East Spain) and various RB sites in Spain and Europe are evaluated and compared, and subsequently analysed for statistically significant trends. The MSY site registered higher average PM2.5 levels than those measured at a selection of other RB sites across Spain, Portugal, Germany and Scandinavia by percentage compared to the mean of all the stations in these countries, but lower than those measured in Switzerland, Italy and Austria. Reductions in PM2.5 were observed across all stations in Spain and Europe to varying degrees (7–49%). MSY underwent a statistically significant reduction since measurements began, indicating a year-on-year gradual decrease (−3.7 μg m−3, calculated from the final year of data compared to the mean). Similar trends were observed in other RB sites across Spain (−1.9 μg m−3). Reductions recorded in PM2.5 across Europe were varied, with many experiencing gradual, year-on-year decreases (−1.8 μg m−3). These reductions have been attributed to various causes: the introduction and implementation of pollution abatement strategies in EU member states, the effect of the current economic crisis on emissions of PM2.5 and the influence of meteorology observed during the winters of 2009 and 2010. In addition, the North Atlantic Oscillation (NAO), a large scale meteorological phenomenon most prevalent during winter, was observed to influence the frequency of Saharan dust intrusions across the Iberian Peninsula. Chemical composition of PM2.5 at MSY is characterised by high levels of organic matter (OM) and sulphate, followed by crustal material, nitrate and ammonia. Sea Spray and elemental carbon (EC) comprised a minor part of the total PM2.5 mass. Statistical trend analysis was performed on the various chemical components of PM2.5 recorded at MSY to determine which components were accountable for the decrease in PM2.5 concentration. It is shown that OM underwent the largest decrease over the time period with a statistically significant trend (−1.3 μg m−3 compared to the mean), followed by sulphate (−0.8 μg m−3), ammonium (−0.5 μg m−3) and nitrate (−0.4 μg m−3). Conversely, sea spray, EC and crustal material reductions were found to be negligible.

Description: The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.

Description: The chemical composition and sources of ambient fine particulate matter (PM1) over a period of 2.5 years for a regional background site in the western Mediterranean are presented in this work. Furthermore, sub-micron particle number concentrations and the sources of these particles are also presented. The mean PM1 concentration for the measurement period was 8.9 μg m−3, with organic matter (OM) and sulphate comprising most of the mass (3.2 and 1.5 μg m−3 respectively). Six sources were identified in PM1 by Positive Matrix Factorisation (PMF): secondary organic aerosol, secondary nitrate, industrial, traffic + biomass burning, fuel oil combustion and secondary sulphate. Typically anthropogenic sources displayed elevated concentrations during the week with reductions at weekends. Nitrate levels were elevated in winter and negligible in summer, whereas secondary sulphate levels underwent a contrasting seasonal evolution with highest concentrations in summer, similar to the fuel oil combustion source. The SOA source was influenced by episodes of sustained pollution as a result of anticyclonic conditions occurring during winter, giving rise to thermal inversions and the accumulation of pollutants in the mixing layer. Increased levels in summer were owing to higher biogenic emissions and regional recirculation of air masses. The industrial source decreased in August due to decreased emissions during the vacation period. Increases in the traffic + biomass burning source were recorded in January, April and October, which were attributed to the occurrence of the aforementioned pollution episodes and local biomass burning emission sources, which include agriculture and domestic heating systems. Average particle number concentrations (N9-825 nm) from 5/11/2010 to 01/06/2011 and from 15/10/2011 to 18/12/2011 reached 3097 cm−3. Five emission sources of particle of sub-micron particles were determined by Principal Component Analysis (PCA); industrial + traffic + biomass burning, new particle formation + growth, secondary sulphate + fuel oil combustion, crustal material and secondary nitrate. The new particle formation + growth source dominated the particle number concentration (56% of total particle number concentration), especially for particles 〈 100 nm, followed by industrial + traffic + biomass burning (13%). Secondary sulphate + fuel oil combustion (8%), nitrate (9%) and crustal material (2%) were dominant for particles of larger diameter (〉 100 nm) and thus did not influence the particle number concentration significantly.

Description: An analysis of chemical composition data of particulate matter samples (TSP, PM10 and PM2.5) collected from 2002 to 2008 in the North Atlantic free troposphere at the Izaña Global Atmospheric Watch (GAW) observatory (Tenerife, Canary Islands) shows that desert dust is very frequently mixed with particulate pollutants in the Saharan Air Layer (SAL). The study of this data set with Median Concentrations At Receptor (MCAR) plots allowed the identification of the potential source regions of the dust and particulate pollutants. Areas located at the south of the southern slope of the Atlas mountains emerge as the most frequent source of the soil desert dust advected to the northern edge of the SAL in summer. Industrial emissions occurring in Northern Algeria, Eastern Algeria, Tunisia and the Atlantic coast of Morocco appear as the most important source of the nitrate, ammonium and a fraction of sulphate (at least 60 % of the sulphate

Description: We interpret here the variability of levels of carbonaceous aerosols based on a 12 yr database from 78 monitoring stations across Spain specially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m−3 of non-mineral carbon (nmC), mostly made of organic carbon (OC) with very little elemental carbon (EC), around 0.1 μg m−3; OC / EC = 12–15), to the highly polluted major cities (8–10 μg m−3 of nmC; 3–4 μg m−3 of EC; 4–5 μg m−3 of OC; OC / EC = 1–2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning and of biogenic emissions. Correlations between yearly averaged OC / EC and EC concentrations adjust very well to a potential equation (OC = 3.37 EC0.326, R2 = 0.8). A similar equation is obtained when including average concentrations obtained at other European sites (OC = 3.60EC0.491, R2 = 0.7). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance from road, traffic volume and density, mixing-layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend for NO2 / (OC + EC) ratios as these standards have been much less effective for the abatement of NOx exhaust emissions in passenger diesel cars. This study concludes that EC, EBC, and especially nmC and OC + EC are very good candidates for new air quality standards since they cover both emission impact and health-related issues.

Description: The time variability and long term trends of PM2.5 (particulate matter of diameter

Description: Time variation of mass particulate matter (PM1 and PM1−10), black carbon (BC) and particle number (N) concentrations at the high altitude site of Montsec (MSC) in the southern Pyrenees was interpreted for the period 2010–2012. The MSC site registered higher PM10 (12 μg m−3) and N 〉 7 nm (2209 # cm−3) concentrations than those measured at other high altitude sites in central Europe (PM10: 3–9 μg m−3 and N: 634–2070 # cm−3). By contrast, BC concentrations at MSC (0.2 μg m−3) were equal or even lower than those measured at these European sites (0.2–0.4 μg m−3). These differences were attributed to the lower influence of anthropogenic emissions and to the higher relevance of Saharan dust transport and new particle formation (NPF) processes at MSC. The different time variation of PM and BC concentrations compared with that of N suggests that these aerosol parameters were governed by diverse factors at MSC. Both PM and BC concentrations showed marked differences for different meteorological scenarios, with enhanced concentrations under North African outbreaks (PM1−10: 13 μg m−3, PM1: 8 μg m−3 and BC: 0.3 μg m−3) and low concentrations when Atlantic advections occurred (PM1−10: 5 μg m−3, PM1: 4 μg m−3 and BC: 0.1 μg m−3). Because of the contrasting origin of the air masses in the warmer seasons (spring and summer) and in the colder seasons (autumn and winter), PM and BC concentrations showed a marked increase in summer, with a secondary maximum in early spring, and were at their lowest during winter. The maximum in the warmer seasons was attributed to long-range transport processes which mask the breezes and regional transport breaking the daily cycles of these pollutants. By contrast, PM and BC concentrations showed clear diurnal cycles with maxima at midday in the colder seasons. A statistically significant weekly variation was also obtained for the BC concentrations, displaying a progressive increase from Tuesday to Saturday, followed by a significant decrease on Sunday and Monday. N concentrations depended more on local meteorological variables such as solar radiation than on the air mass origin. Therefore, the highest concentrations of N were associated with summer regional episodes (N 〉 3 nm: 4461 # cm−3 and N 〉 7 nm: 3021 # cm−3) and the lowest concentrations were related to winter regional scenarios (N 〉 3 nm: 2496 # cm−3 and N 〉 7 nm: 1073 # cm−3). This dependence on solar radiation also accounted for the marked diurnal cycle of N concentrations throughout the year with a peak at midday and for the absence of a weekly pattern. Measurements carried out at MSC enabled us to characterize the tropospheric background aerosols in the Western Mediterranean Basin (WMB). Our results highlight the importance of the NPF processes in southern Europe, reveal much lower anthropogenic emissions than in central Europe, and underline the contribution of natural long-range transport such as Saharan dust.

Description: The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to slightly underestimate PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. In particular, the model description of formation of coarse nitrate on sea salt and dust particles requires further attention. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in good agreement with the measurements. As expected, the diurnal variability of ammonia is not very well captured, but this will probably improve if the EMEP model is coupled to a dynamic, mechanistic ammonia emission module. The largest underestimations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning source. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though presently measurement protocols have been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.

Description: The chemical composition and sources of ambient fine particulate matter (PM1) over a period of 2.5 yr for a regional background site in the western Mediterranean are presented in this work. Major components (such as SO12−, NO3−, NH4+, organic and elemental carbon) and trace elements were analysed and the emission sources affecting PM1 were determined using Positive Matrix Factorisation (PMF). Furthermore, sub-micron particle number concentrations and the sources of these particles are also presented. Sources of sub-micron particles were determined by Principal Component Analysis (PCA). The mean PM1 concentration for the measurement period was 8.9 μg m−3, with organic matter (OM) and sulphate comprising most of the mass (3.2 and 1.5 μg m−3). A clear seasonal variation was recorded with higher PM1 concentrations in summer (11.2 μg m−3) compared to winter (6.6 μg m−3). This summer increase was due to elevated levels of sulphate and OM. Six sources were identified by PMF: secondary organic aerosol, secondary nitrate, industrial, traffic + biomass burning, fuel oil combustion and secondary sulphate. The daily variations of these sources were also determined, whereby the typically anthropogenic sources displayed elevated concentrations during the week with reductions at weekends. Nitrate levels were elevated in winter and negligible in summer, whereas secondary sulphate levels underwent a contrasting seasonal evolution with highest concentrations in summer, similar to the fuel oil combustion source. The SOA source was influenced by episodes of sustained pollution as a result of anticyclonic conditions occurring during winter, giving rise to thermal inversions and the accumulation of pollutants in the mixing layer. Increased levels in summer were owing to higher biogenic emissions and regional recirculation of air masses. The industrial source decreased in August due to decreased emissions during the vacation period. Increases in the traffic + biomass burning source were recorded in January, April and October, which were attributed to the occurrence of the aforementioned pollution episodes and local biomass burning emission sources, which include agriculture and domestic heating systems. Average particle number concentrations (N9–825 nm) from 5 November 2010 to 1 June 2011 and from 15 October 2011 to 18 December 2011 reached 3097 cm−3. Five emission sources of particles were identified by PCA; industrial + traffic + biomass burning, new particle formation + growth, secondary sulphate + fuel oil combustion, crustal material and secondary nitrate. Multilinear regression analysis was applied to the dataset to quantify the contribution of each source to the sub-micron particle number concentration. The new particle formation + growth source dominated the particle number concentration (56% of total particle number concentration), especially for particles 100 nm) and thus did not influence the particle number concentration significantly.

Description: We interpret here the variability of levels of carbonaceous aerosols based on a 12-yr database from 78 monitoring stations across Spain especially compiled for this article. Data did not evidence any spatial trends of carbonaceous aerosols across the country. Conversely, results show marked differences in average concentrations from the cleanest, most remote sites (around 1 μg m−3 of non-mineral carbon (nmC), mostly made of organic carbon (OC), with very little elemental carbon (EC) 0.1 μg m−3; OC/EC = 12–15), to the highly polluted major cities (8–10 μg m−3 of nmC; 3–4 μg m−3 of EC; 4–5 μg m−3 of OC; OC/EC = 1–2). Thus, urban (and very specific industrial) pollution was found to markedly increase levels of carbonaceous aerosols in Spain, with much lower impact of biomass burning. Correlations between yearly averaged OC/EC and EC concentrations adjust very well to a potential equation (OC/EC = 3.37 EC−0.67 R2 = 0.94). A similar equation is obtained when including average concentrations obtained at other European sites (y = 3.61x−0.5, R2 = 0.78). A clear seasonal variability in OC and EC concentrations was detected. Both OC and EC concentrations were higher during winter at the traffic and urban sites, but OC increased during the warmer months at the rural sites. Hourly equivalent black carbon (EBC) concentrations at urban sites accurately depict road traffic contributions, varying with distance to road, traffic volume and density, mixing layer height and wind speed. Weekday urban rush-hour EBC peaks are mimicked by concentrations of primary gaseous emissions from road traffic, whereas a single midday peak is characteristic of remote and rural sites. Decreasing annual trends for carbonaceous aerosols were observed between 1999 and 2011 at a large number of stations, probably reflecting the impact of the EURO4 and EURO5 standards in reducing the diesel PM emissions. This has resulted in some cases in an increasing trend of NO2/OC+EC ratios, because these standards have been much less effective for the abatement of NOx exhaust emissions in passenger diesel cars. This study concludes that EC, EBC, and especially nmC and OC+EC are very good candidates for new air quality standards since they cover both emission impact and health related issues.