Temporal and spatial variation of the chemical composition of PM10 at urban and rural sites in the Basel area,Switzerland

Particulate matter measurements of different size fractions (PM₄, PM₁₀, TSP) were performed in the Basel area (Switzerland) at seven urban sites throughout 1997 and at two urban and two rural sites during the following year (April 1998–May 1999). Based on a sample of filters which was chemically analyzed, we investigated the chemical composition of PM₁₀ both within the city of Basel and among urban and rural sites. The temporal and spatial variability of the chemical composition of PM₁₀ was evaluated taking into account additional data from meteorology and further air pollutants. The chemical analyses of PM₁₀ showed that carbonaceous substances (elemental carbon, organic matter) and inorganic substances of secondary origin such as sulfate, nitrate and ammonium were the most abundant component of PM₁₀ in the Basel area (approximately 60–70%). Difference in the PM₁₀ concentration between urban and rural sites was larger during the cold season than during the warm season. This was mainly due to the presence of an inversion layer between the city and the more elevated rural sites resulting in higher concentrations of nitrate, ammonium and organic matter in the city during the cold season. The higher PM₁₀ concentration on workdays compared to weekends was mostly a result of the temporal variation of the concentration of Ca, elemental carbon, Ti, Mn, and Fe, indicating that these compounds are for the most part caused by regional human activities. Although total PM₁₀ mass concentration was found to be in general uniformly distributed within the city of Basel, the chemical composition was more variable due to specific sources like road traffic and other anthropogenic emissions.     

An assessment of the impact of climate change on air quality at two UK sites

Possible effects of climate change on air quality are studied for two urban sites in the UK, London and Glasgow. Hourly meteorological data were obtained from climate simulations for two periods representing the current climate and a plausible late 21st century climate. Of the meteorological quantities relevant to air quality, significant changes were found in temperature, specific humidity, wind speed, wind direction, cloud cover, solar radiation, surface sensible heat flux and precipitation. Using these data, dispersion estimates were made for a variety of single sources and some significant changes in environmental impact were found in the future climate. In addition, estimates for future background concentrations of NO_x, NO₂, ozone and PM₁₀ upwind of London and Glasgow were made using the meteorological data in a statistical model. These showed falls in NO_x and increases in ozone for London, while a fall in NO₂ was the largest percentage change for Glasgow. Other changes were small. With these background estimates, annual-average concentrations of NO_x, NO₂, ozone and PM₁₀ were estimated within the two urban areas. For London, results averaged over a number of sites showed a fall in NO_x and a rise in ozone, but only small changes in NO₂ and PM₁₀. For Glasgow, the changes in all four chemical species were small. Large-scale background ozone values from a global chemical transport model are also presented. These show a decrease in background ozone due to climate change. To assess the net impact of both large scale and local processes will require models which treat all relevant scales.     

An empirical approach for the prediction of daily mean PM10 concentrations

An empirical model has been devised to predict concentrations of PM₁₀ at background and roadside locations in London. Factors to calculate primary PM₁₀ and PM_2.5 concentrations are derived from annual mean NO_X, PM_2.5 and PM₁₀ measurements across London and south east England. These factors are used to calculate daily means for the primary and non-primary PM₁₀ fractions for the London area. The model accurately predicts daily mean PM₁₀ and EU Directive Limit values across a range of sites from kerbside to rural. Predictions of future PM₁₀ can be made using the expected reductions in secondary PM₁₀ and site specific annual mean NO_X predicted from emission inventories and dispersion modelling. The model suggests that the EU Directive Limit values will be exceeded close to many of London's busiest roads, and perhaps at central background sites should there be a repeat of 1996 meteorological conditions during 2005. A repeat of 1997 meteorology conditions during 2005 would lead to the EU Limit Value being exceeded alongside the busiest central London roads only. The model is applicable for London and south east England but the methodology could be applied elsewhere at a city or regional level. The model relies on the currently observed ratio between NO_X and PM₁₀. This ratio has remained constant over the last 4 years but might change in the future. The NO_X:PM₁₀ ratio derived from measurements and used in this model, implies that emission inventories might over estimate primary PM₁₀ by more than 50%.     

Effects of Wind Direction on Coarse and Fine Particulate Matter Concentrations in Southeast Kansas

Abstract

Field data for coarse particulate matter ([PM] PM₁₀) and fine particulate matter (PM_2.5) were collected at selected sites in Southeast Kansas from March 1999 to October 2000, using portable MiniVol particulate samplers. The purpose was to assess the influence on air quality of four industrial facilities that burn hazardous waste in the area located in the communities of Chanute, Independence, Fredonia, and Coffeyville. Both spatial and temporal variation were observed in the data. Variation because of sampling site was found to be statistically significant for PM₁₀ but not for PM_2.5. PM₁₀ concentrations were typically slightly higher at sites located within the four study communities than at background sites. Sampling sites were located north and south of the four targeted sources to provide upwind and downwind monitoring pairs. No statistically significant differences were found between upwind and downwind samples for either PM₁₀ or PM_2.5, indicating that the targeted sources did not contribute significantly to PM concentrations. Wind direction can frequently contribute to temporal variation in air pollutant concentrations and was investigated in this study. Sampling days were divided into four classifications: predominantly south winds, predominantly north winds, calm/variable winds, and winds from other directions. The effect of wind direction was found to be statistically significant for both PM₁₀ and PM_2.5. For both size ranges, PM concentrations were typically highest on days with predominantly south winds; days with calm/variable winds generally produced higher concentrations than did those with predominantly north winds or those with winds from “other” directions. The significant effect of wind direction suggests that regional sources may exert a large influence on PM concentrations in the area.     

Source apportionment of urban fine and ultra-fine particle number concentration in a Western Mediterranean city

Extensive measurements on particle number concentration and size distribution (13–800 nm), together with detailed chemical composition of PM_2.5 have constituted the main inputs of the database used for a source apportionment analysis. Data were collected at an urban background site in Barcelona, Western Mediterranean.The source identification analysis helped us to distinguish five emission sources (vehicle exhausts, mineral dust, sea spray, industrial source and fuel-oil combustion) and two atmospheric processes (photochemical induced nucleation and regional/urban background particles derived from coagulation and condensation processes). After that, a multilinear regression analysis was applied in order to quantify the contribution of each factor.This study reveals that vehicle exhausts contribute dominantly to the number concentration in all the particle sizes (52–86%), but especially in the range 30–200 nm. This work also points out the importance of the regional and/or urban formed aerosols (secondary inorganic particles) on the total number concentration (around 25% of the total number), with a higher impact on the accumulation mode. The photo-chemically induced nucleation of aerosols only represents a small proportion of the total number as an annual mean (3%), but is very relevant when considering only the nucleation mode (13–20 nm) fraction (23%). The other sources recognized registered sporadic contributions to the total number, coinciding with specific meteorological scenarios.This study discloses the main sources and features affecting and controlling the fine and ultra-fine aerosols in a typical city in the Western Mediterranean coast. Whereas the road traffic appears to be the most important source of sub-micrometric aerosols, other sources may not be negligible under specific meteorological conditions.     

Regional Transport and Urban Contributions to Fine Particle Concentrations in Southeastern Canada

Abstract

The impact of various atmospheric transport directions on ambient fine particle (PM_2.5) concentrations at several sites in southeastern Canada was estimated (for May-September) using back-trajectory analysis. Three-day back trajectories (four per day) were paired with 6-hr average PM_2.5 mass concentrations measured using tapered element oscillating microbalances (TEOM). PM_2.5 concentrations at rural locations in the region were affected by nonlocal sources originating in both Canada and the United States. Comparison of sites revealed that, on average, the local contribution to total PM_2.5 in the greater Toronto area (GTA) is approximately 30–35%. At each location, average PM_2.5 concentrations under south/southwesterly flow conditions were 2–4 times higher than under the corresponding northerly flow conditions. The chemical composition of both urban and rural PM_2.5 was determined during two separate 2-week spring/summer measurement campaigns. Components identified included SO₄ ^2?, NO₃ ^?, NH₄+, black carbon and organic carbon (OC), and trace elements. Higher particle mass at the urban Toronto site was composed of a higher proportion of all components. However, black carbon, NO₃ ^?, NaCl, and trace elements were found to be the most enriched over the rural/regional background levels.     

Source apportionment analysis of atmospheric particulates in an industrialised urban site in southwestern Spain

A detailed physical and chemical characterisation of total suspended particles (TSP) in the highly industrialised city of Huelva (southwestern Spain) was carried out. The results evidenced a coarse grain-size prevalence (PM₁₀ accounting for only 40% of TSP mass, 37 and 91 μg/m³, respectively). PM₁₀ levels are in the usual range for urban background sites in Spain. The crustal, anthropogenic and marine components accounted for a mean of a 40%, 24% and 5% of bulk TSP, respectively. As expected from the industrial activities, relatively high PO₄³⁻ and As levels for an urban site were detected. In addition to the crustal and marine components, source apportionment analysis revealed three additional emission sources influencing the levels and composition of TSP: (a) a petrochemical source, (b) a mixed metallurgical-phosphate source, (c) and an unknown source (Sb and NO₃⁻).Due to the high local emissions, the mean TSP anthropogenic contribution (mostly PM₁₀) obtained for all possible air mass transport scenarios reached 18–29 μg/m³. The 2010 annual EU PM₁₀ limit value (20 μg/m³) would be exceeded by the anthropogenic load recorded for all the air mass transport scenarios, with the exception of the North Atlantic transport (only 15% of the sampling days). Under African air mass transport scenarios (20% of sampling days), the TSP crustal contribution reached near three times the local crustal contribution. It must be pointed out that this crustal input should diminish when sampling PM₁₀ due to the dominant coarse size distribution of this type of particles.     

Particulate matter sources on an hourly timescale in a rural community during the winter

Particulate matter (PM) sources at four different monitoring sites in Alexandra, New Zealand, were investigated on an hourly timescale. Three of the sites were located on a horizontal transect, upwind, central, and downwind of the general katabatic flow pathway. The fourth monitoring site was located at the central site, but at a height of 26 m, using a knuckleboom, when wind conditions permitted. Average hourly PM₁₀ (PM with an aerodynamic diameter <10 μm) concentrations in Alexandra showed slightly different diurnal profiles depending on the sampling site location. Each location did, however, feature a large evening peak and smaller morning peak in PM₁₀ concentrations. The central site in Alexandra experienced the highest PM₁₀ concentrations as a result of PM transport along a number of katabatic flow pathways. A significant difference in PM₁₀ concentrations between the central and elevated sites indicated that a shallow inversion layer formed below the elevated site, limiting the vertical dispersion of pollutants. Four PM₁₀ sources were identified at each of the sites: biomass combustion, vehicles, crustal matter, and marine aerosol. Biomass combustion was identified as the most significant source of PM₁₀, contributing up to 91% of the measured PM₁₀. Plots of the average hourly source contributions to each site revealed that biomass combustion was responsible for both the evening and morning peaks in PM₁₀ concentrations observed at each of the sites, suggesting that Alexandra residents were relighting their fires when they rose in the morning. The identification of PM sources on an hourly timescale can have significant implications for air quality management.

Implications: Monitoring the sources of PM₁₀ on an hourly timescale at multiple sites within an airshed provides extremely useful information for air quality management. Sources responsible for observed peaks in measured diurnal PM₁₀ concentration profiles can be easily identified and targeted for reduction. Also, hourly PM₁₀ sampling can provide crucial information on the role meteorology plays in the development of elevated PM₁₀ concentrations.     

Determination of PM2.5 sources using time-resolved integrated source and receptor models

Multivariate statistical techniques are applied to particulate matter (PM) and meteorological data to identify the sources responsible for evening PM spikes at Sunland Park, NM (USA). The statistical techniques applied are principal components analysis (PCA), redundancy analysis (RDA), and absolute principal components scores analysis (APCSA), and the data evaluated are 3-h average (6–9 p.m.) PM_2.5 mass and chemical composition and 1-h average PM_2.5 and PM₁₀ mass and environmental data collected in the winter of 2002. Although the interpretation of the data was complicated by the presence of sources which are likely changing in time (e.g. brick kilns), the multivariate analyses indicate that the evening high PM_2.5 is associated with burning-activities occurring to the south of Sunland Park, and these emissions are characterized by elevated Sb, Cl⁻, and elemental carbon; ∼68% of the PM_2.5 mass can be attributed to this source. The PM₁₀ evening peaks, on the other hand, are mainly caused by resuspended dust generated by vehicular movements south of the site and transported by the local terrain-induced drainage flow.     

Source Apportionment of Ambient Total Suspended Particulates and Coarse Particulate Matter in Urban Areas of Jiaozuo,China

Abstract

Approximately 750 total suspended particulates (TSPs) and coarse particulate matter (PM₁₀) filter samples from six urban sites and a background site and >210 source samples were collected in Jiaozuo City during January 2002 to April 2003. They were analyzed for mass and abundances of 25 chemical components. Seven contributive sources were identified, and their contributions to ambient TSP/PM₁₀ levels at the seven sites in three seasons (spring, summer, and winter days) and a “whole” year were estimated by a chemical mass balance (CMB) receptor model. The spatial TSP average was high in spring and winter days at a level of approximately 530 ～g/m³ and low in summer days at 456 ～g/m³; however, the spatial PM₁₀ average exhibited little variation at a level of approximately 325 ～g/m³, and PM_10-to-TSP ratios ranged from 0.58 to 0.81, which suggested heavy particulate matter pollution existing in the urban areas. Apportionment results indicated that geological material was the largest contributor to ambient TSP/PM₁₀ concentrations, followed by dust emissions from construction activities, coal combustion, secondary aerosols, vehicle movement, and other industrial sources. In addition, paved road dust and re-entrained dust were also apportioned to the seven source types and found soil, coal combustion, and construction dust to be the major contributors.     

Determination and analysis of PM10 source apportionment during episodes of air pollution in Central Eastern European urban areas: The case of wintertime 2006

Source apportionment of air pollution due to particulate matter with an aerodynamic diameter <10 μm (PM₁₀) was investigated in Central Eastern European urban areas. A combination of four methods was developed to distinguish long-range transport (LRT) and regional transport (RT) from local pollution (LP) sources as well as to discern the involvement of traffic or residential sources in LP. Sources of PM₁₀ events of pollution were determined in January 2006 in representative Polish cities using monitored air quality and meteorological data, backward air mass trajectories, correlation and principal component analysis (PCA). Daily patterns of PM₁₀ levels show that several peak episodes were registered in Poland; January 21–30th being the most polluted days. Air mass back-trajectory analysis shows that all cities were under the influence of LRT from North-eastern origins (Russia–Belarus–Ukraine), most were also under LRT from Southern origin (Slovakia, Czech Republic), and northern cities were under national RT influence. PCA analysis shows that ion-sums of secondary inorganic aerosols account for LRT pollution while arsenic and chromium represents markers of RT (industrial) and LP (residential) sources of PM₁₀, respectively. Determination of several ratios (REG/UB, REG/TRAF, TRAF/UB) calculated between PM₁₀ levels measured at regional background (REG); urban background (UB) and traffic (TRAF) monitoring sites shows that, with ratios REG/UB ≥ 0.57, PM₁₀ episodes in both Szczecin and Warsaw bore a marked RT origin. The lower REG/UB ≤ 0.35 in the Southern cities of Cracow and Zabrze indicates that LP was the main contributor to the observed episodes. Only PM₁₀ episodes in Southern-western Poland (Jelenia Góra) were clearly of LP origin as characterized, by the lowest REG/UB ratio (<0.2). The high TRAF/UB ratios obtained for all cities (close to 1) indicate that there was a great uniformity of PM levels on an urban scale owing to the meteorologically stagnant conditions. A high correlation between PM₁₀, NO₂ and CO confirms that traffic emission represented a common and an important LP source of urban pollution in most Polish cities during January 2006. On the other hand PM₁₀ which is also highly correlated with SO₂ in 4 cities out of 6, indicates that coal combustion through domestic heating or industrial activities was also an important LP source of PM₁₀. Finally, extremely unfavourable meteorological conditions caused by the influence of a Siberian high-pressure system were found to be associated with the occurrence of severe PM₁₀ episodes of pollution.     

Chemical composition and mass closure of ambient coarse particles at traffic and urban-background sites in Thessaloniki,Greece

Concentrations and chemical composition of the coarse particle fraction (PM_c) were investigated at two urban sites in the city of Thessaloniki, Greece, through concurrent sampling of PM₁₀ and PM_2.5 during the warm and the cold months of the year. PM_c levels at the urban-traffic site (UT) were among the highest found in literature worldwide exhibiting higher values in the cold period. PM_c levels at the urban-background site (UB) were significantly lower exhibiting a reverse seasonal trend. Concentration levels of minerals and most trace metals were also higher at the UT site suggesting a stronger impact from traffic-related sources (road dust resuspension, brake and tire abrasion, road wear). According to the chemical mass closure obtained, minerals (oxides of Si, Al, Ca, Mg, Fe, Ti, and K) dominated the PM_c profile, regardless of the site and the period, with organic matter and secondary inorganic aerosols (mainly nitrate) also contributing considerably to the PM_c mass, particularly in the warm period. The influence of wind speed to dilution and/or resuspension of coarse particles was investigated. The source of origin of coarse particles was also investigated using surface wind data and atmospheric back-trajectory modeling. Finally, the contribution of resuspension to PM_c levels was estimated for air quality management perspectives.     

Reduction of atmospheric fine particle level by restricting the idling vehicles around a sensitive area

Atmospheric particles are a major problem that could lead to harmful effects on human health, especially in densely populated urban areas. Chiayi is a typical city with very high population and traffic density, as well as being located at the downwind side of several pollution sources. Multiple contributors for PM_2.5 (particulate matter with an aerodynamic diameter ≥2.5 μm) and ultrafine particles cause complicated air quality problems. This study focused on the inhibition of local emission sources by restricting the idling vehicles around a school area and evaluating the changes in surrounding atmospheric PM conditions. Two stationary sites were monitored, including a background site on the upwind side of the school and a campus site inside the school, to monitor the exposure level, before and after the idling prohibition. In the base condition, the PM_2.5 mass concentrations were found to increase 15% from the background, whereas the nitrate (NO₃^?) content had a significant increase at the campus site. The anthropogenic metal contents in PM_2.5 were higher at the campus site than the background site. Mobile emissions were found to be the most likely contributor to the school hot spot area by chemical mass balance modeling (CMB8.2). On the other hand, the PM_2.5 in the school campus fell to only 2% after idling vehicle control, when the mobile source contribution reduced from 42.8% to 36.7%. The mobile monitoring also showed significant reductions in atmospheric PM_2.5, PM_0.1, polycyclic aromatic hydrocarbons (PAHs), and black carbon (BC) levels by 16.5%, 33.3%, 48.0%, and 11.5%, respectively. Consequently, the restriction of local idling emission was proven to significantly reduce PM and harmful pollutants in the hot spots around the school environment.

Implications: The emission of idling vehicles strongly affects the levels of particles and relative pollutants in near-ground air around a school area. The PM_2.5 mass concentration at a campus site increased from the background site by 15%, whereas NO₃^? and anthropogenic metals also significantly increased. Meanwhile, the PM_2.5 contribution from mobile source in the campus increased 6.6% from the upwind site. An idling prohibition took place and showed impressive results. Reductions of PM_2.5, ionic component, and non-natural metal contents were found after the idling prohibition. The mobile monitoring also pointed out a significant improvement with the spatial analysis of PM_2.5, PM_0.1, PAH, and black carbon concentrations. These findings are very useful to effectively improve the local air quality of a densely city during the rush hour.     

Source apportionment of ambient PM2.5 at five spanish centres of the european community respiratory health survey (ECRHS II)

Fine particulate matter (PM_2.5) was sampled at 5 Spanish locations during the European Community Respiratory Health Survey II (ECRHS II). In an attempt to identify and quantify PM_2.5 sources, source contribution analysis by principal component analysis (PCA) was performed on five datasets containing elemental composition of PM_2.5 analysed by ED-XRF. A total of 4–5 factors were identified at each site, three of them being common to all sites (interpreted as traffic, mineral and secondary aerosols) whereas industrial sources were site-specific. Sea-salt was identified as independent source at all coastal locations except for Barcelona (where it was clustered with secondary aerosols). Despite their typically dominant coarse grain-size distribution, mineral and marine aerosols were clearly observed in PM_2.5. Multi-linear regression analysis (MLRA) was applied to the data, showing that traffic was the main source of PM_2.5 at the five sites (39–53% of PM_2.5, 5.1–12.0 μg m⁻³), while regional-scale secondary aerosols accounted for 14–34% of PM_2.5 (2.6–4.5 μg m⁻³), mineral matter for 13–31% (2.4–4.6 μg m⁻³) and sea-salt made up 3–7% of the PM_2.5 mass (0.4–1.3 μg m⁻³). Consequently, despite regional and climatic variability throughout Spain, the same four main PM_2.5 emission sources were identified at all the study sites and the differences between the relative contributions of each of these sources varied at most 20%. This would corroborate PM_2.5 as a useful parameter for health studies and environmental policy-making, owing to the fact that it is not as subject to the influence of micro-sitting as other parameters such as PM₁₀. African dust inputs were observed in the mineral source, adding on average 4–11 μg m⁻³ to the PM_2.5 daily mean during dust outbreaks. On average, levels of Al, Si, Ti and Fe during African episodes were higher by a factor of 2–8 with respect to non-African days, whereas levels of local pollutants (absorption coefficient, S, Pb, Cl) showed smaller variations (factor of 0.5–2).     

What are the sources and conditions responsible for exceedences of the 24 h PM10 limit value (50 μg m−3) at a heavily trafficked London site?

The European Union has set limit values for PM₁₀ to be met in 2005. At Marylebone Road, London, where the traffic is heavy, the daily limit value of 50 μg m⁻³ is exceeded more than 35 times a year. A total of 185 days with daily PM₁₀ concentrations exceeding the limit value of 50 μg m⁻³ measured between January 2002 and December 2004 (data capture of 89.5%) are discussed in this paper. These exceedences were more frequent in early spring and in autumn. Concentrations have been disaggregated into regional, urban (background) and local (street) contributions. Most of the episodes of gravimetric PM₁₀ above the limit value were associated with a high regional background and very often the regional contribution dominated the PM₁₀ mass. The secondary aerosol (especially the particulate nitrate) made a major contribution to the PM₁₀ load. These situations were frequently observed when air masses came from the European mainland (showing that both emissions from the UK and other EU countries contributed to the exceedences), and less frequently with maritime air masses that have stagnated over the UK (showing that emissions from the UK alone less frequently contributed to the high regional background). However, the higher frequency of episodes breaching the limit value at the roadside site than at the rural site and the higher frequency of PM₁₀ concentrations above the limit value on weekdays show that the high regional contributions are additional to local and urban emissions. Local emissions mainly due to traffic were the second important contributor to the exceedences, while the contribution of the urban background of London was less important than the local emissions and the regional background. Applying the pragmatic mass closure model of Harrison et al. [2003. A pragmatic mass closure model for airborne particulate matter at urban background and roadside sites. Atmospheric Environment 37, 4927–4933], revealed that the regional aerosol is comprised very largely of ammonium nitrate and sulphate and secondary organic aerosol. Findings suggest that international abatement of secondary aerosol precursors may be the most effective measure to fulfil the requirements of the European Directive 1999/30/CE by lowering the regional background.     

Sources and processes affecting concentrations of PM10 and PM2.5 particulate matter in Birmingham (U.K.)

Hourly average concentrations of PM₁₀ and PM_2.5 have been measured simultaneously at a site within Birmingham U.K. between October 1994 and October 1995. Comparison of PM₁₀ and NO_x data with two other sites in the same city shows comparable summer and winter mean concentrations and highly significant inter-site correlations for both hourly and daily mean data. Over a four-month period samples were also collected for chemical analysis of sulphate, nitrate, chloride, ammonium and elemental and organic carbon. Analysis of the data indicates a marked difference between summer and winter periods. In the winter months PM_2.5 comprises about 80% of PM₁₀ and is strongly correlated with NO_x indicating the importance of road traffic as a source. In the summer months, coarse particles (PM₁₀−PM_2.5) account for almost 50% of PM₁₀ and the influence of resuspended surface dusts and soils and of secondary particulate matter is evident. The chemical analysis data are also consistent with three sources dominating the PM₁₀ composition: vehicle exhaust emissions, secondary ammonium salts and resuspended surface dusts. Coarse particles from resuspension showed a positive dependence on windspeed, whilst elemental carbon derived from road traffic exhibited a negative dependence.     

Monitoring and Source Apportionment of Particulate Matter near a Large Phosphorus Production Facility

ABSTRACT

A source apportionment study was conducted to identify sources within a large elemental phosphorus plant that contribute to exceedances of the National Ambient Air Quality Standards (NAAQS) for 24-hr PM₁₀. Ambient data were collected at three monitoring sites from October 1996 through July 1999, and included the following: 24-hr PM₁₀ mass, 24-hr PM_2.5 and PM_10–2.5 mass and chemistry, continuous PM₁₀and PM_2.5 mass, continuous meteorological data, and wind-direction-resolved PM_2.5 and PM₁₀ mass and chemistry. Ambient-based receptor modeling and wind-directional analysis were employed to help identify major sources or source locations and source contributions. Fine-fraction phosphate was the dominant species observed during PM₁₀ exceedances, though in general, re-suspended coarse dusts from raw and processed materials at the plant were also needed to create an exceedance. Major sources that were identified included the calciners, the CO flares, process-related dust, and electric-arc furnace operations.     

Assessment of natural components of PM10 at UK urban and rural sites

Proposals from the European Commission have raised the possibility that Member States may be able to subtract the concentrations of natural components of airborne particulate matter from measured concentrations when evaluating compliance with EU Limit Values. By applying the pragmatic mass closure model [Harrison et al., 2003. A pragmatic mass closure model for airborne particulate matter at urban background and roadside sites. Atmospheric Environment 37, 4927–4933] to chemical composition data for PM₁₀, it has been possible to estimate the concentrations of natural sea salt, strongly bound water and secondary organic carbon (which is assumed wholly biogenic) to the measured mass of PM₁₀. Because of the difficulty in distinguishing between natural and anthropogenic crustal dusts, the contribution of natural windblown dust and soil has not been accounted for. When the natural components are estimated for two urban and one rural site in the UK, the long-term mean PM₁₀ concentration is reduced by between 5.2 and 7.3 μg m⁻³. The number of exceedences of the 50 μg m⁻³ 24-h limit value falls dramatically from 54 to 21 (from a total of 291 days) at an urban street canyon site, 7 to 3 (n=292 days) at an urban background site and from 8 to 0 (n=241 days) at a rural site when using gravimetric PM₁₀ concentrations. The calculations have also been performed using PM₁₀ concentrations measured by TEOM increased by a factor of 1.3 as recommended by the European Commission as an interim means of estimating gravimetric equivalency, and the number of exceedences of the 24-h limit value fell from 92 to 47 (from a total of 291 days) at the urban street canyon site, from 11 to 3 (n=292 days) at the urban background site and from 6 to 3 (n=241) at the rural site. Clearly, therefore, application of this proposed measure would make a very major difference to the likelihood of compliance or otherwise with the 24-h limit value for PM₁₀.     

Concentrations and source apportionment of PM10 and associated elemental and ionic species in a lignite-burning power generation area of southern Greece

Ambient concentrations of PM₁₀ and associated elemental and ionic species were measured over the cold and the warm months of 2010 at an urban and two rural sites located in the lignite-fired power generation area of Megalopolis in Peloponnese, southern Greece. The PM₁₀ concentrations at the urban site (44.2?±?33.6 μg m^?3) were significantly higher than those at the rural sites (23.7?±?20.4 and 22.7?±?26.9 μg m^?3). Source apportionment of PM₁₀ and associated components was accomplished by an advanced computational procedure, the robotic chemical mass balance model (RCMB), using chemical profiles for a variety of local fugitive dust sources (power plant fly ash, flue gas desulfurization wet ash, feeding lignite, infertile material from the opencast mines, paved and unpaved road dusts, soil), which were resuspended and sampled through a PM₁₀ inlet onto filters and then chemically analyzed, as well as of other common sources such as vehicular traffic, residential oil combustion, biomass burning, uncontrolled waste burning, marine aerosol, and secondary aerosol formation. Geological dusts (road/soil dust) were found to be major PM₁₀ contributors in both the cold and warm periods of the year, with average annual contribution of 32.6 % at the urban site vs. 22.0 and 29.0 % at the rural sites. Secondary aerosol also appeared to be a significant source, contributing 22.1 % at the urban site in comparison to 30.6 and 28.7 % at the rural sites. At all sites, the contribution of biomass burning was most significant in winter (28.2 % at the urban site vs. 14.6 and 24.6 % at the rural sites), whereas vehicular exhaust contribution appeared to be important mostly in the summer (21.9 % at the urban site vs. 11.5 and 10.5 % at the rural sites). The highest contribution of fly ash (33.2 %) was found at the rural site located to the north of the power plants during wintertime, when winds are favorable. In the warm period, the highest contribution of fly ash was found at the rural site located to the south of the power plants, although it was less important (7.2 %). Moderate contributions of fly ash were found at the urban site (5.4 and 2.7 % in the cold and the warm period, respectively). Finally, the mine field was identified as a minor PM₁₀ source, occasionally contributing with lignite dust and/or deposited wet ash dust under dry summer conditions, with the summertime contributions ranging between 3.1 and 11.0 % among the three sites. The non-parametric bootstrapped potential source contribution function analysis was further applied to localize the regions of sources apportioned by the RCMB. For the majority of sources, source regions appeared as being located within short distances from the sampling sites (within the Peloponnesse Peninsula). More distant Greek areas of the NNE sector also appeared to be source regions for traffic emissions and secondary calcium sulfate dust.     

The Southeastern Aerosol Research and Characterization Study: Part II. Filter-Based Measurements of Fine and Coarse Particulate Matter Mass and Composition

Abstract

The Southeastern Aerosol Research and Characterization Study (SEARCH) was implemented in 1998–1999 to provide data and analyses for the investigation of the sources, chemical speciation, and long-term trends of fine particulate matter (PM_2.5) and coarse particulate matter (PM_10–2.5) in the Southeastern United States. This work is an initial analysis of 5 years (1999–2003) of filter-based PM_2.5 and PM_10–2.5 data from SEARCH. We find that annual PM_2.5 design values were consistently above the National Ambient Air Quality Standards (NAAQS) 15 µg/m³ annual standard only at monitoring sites in the two largest urban areas (Atlanta, GA, and North Birmingham, AL). Other sites in the network had annual design values below the standard, and no site had daily design values above the NAAQS 65 µg/m³ daily standard. Using a particle composition monitor designed specifically for SEARCH, we found that volatilization losses of nitrate, ammonium, and organic carbon must be accounted for to accurately characterize atmospheric particulate matter. In particular, the federal reference method for PM_2.5 underestimates mass by 3–7% as a result of these volatilization losses. Organic matter (OM) and sulfate account for ≥60% of PM_2.5 mass at SEARCH sites, whereas major metal oxides (MMO) and unidentified components (“other”) account for ≥80% of PM_10–2.5 mass. Limited data suggest that much of the unidentified mass in PM_10–2.5 may be OM. For paired comparisons of urban-rural sites, differences in PM_2.5 mass are explained, in large part, by higher OM and black carbon at the urban site. For PM₁₀, higher urban concentrations are explained by higher MMO and “other.” Annual means for PM_2.5 and PM_10–2.5 mass and major components demonstrate substantial declines at all of the SEARCH sites over the 1999–2003 period (10–20% in the case of PM_2.5, dominated by 14–20% declines in sulfate and 11–26% declines in OM, and 14–25% in the case of PM_10–2.5, dominated by 17–30% declines in MMO and 14–31% declines in “ other”). Although declining national emissions of sulfur dioxide and anthropogenic carbon may account for a portion of the observed declines, additional investigation will be necessary to establish a quantitative assessment, especially regarding trends in local and regional emissions, primary carbon emissions, and meteorology.