PM Emissions Emanating from Limited-Access Highways

ABSTRACT

Motor vehicle contributions to primary particulate matter (PM) emissions include exhaust, tire wear, brake and clutch wear, and resuspended road dust. Relatively few field studies have been conducted to quantify fleetaverage exhaust emissions for actual on-road conditions. Therefore, direct measurements of motor vehicle-related PM emissions are warranted. In this study, PM₁₀ and PM_2.5 mass concentrations were measured near two major highways in the St. Louis area over the period from February–April 1997. Samplers were deployed both upwind and downwind of the roadways to capture the transport and dispersion of PM with distance from the roadway. The observed microscale concentration fields were compared to estimates using the PART5 emission factor model together with the CALINE4 highway dispersion model. Traffic- induced PM mass concentrations observed downwind of the roadway were always less than PART5/CALINE4 predictions; average percent differences for observed traffic-induced mass concentrations compared to predicted values were ?34% for PM_2.5 and -70% for PM₁₀. In most cases, the observed PM concentration decay with increasing distance from the roadway was steeper than predicted by dispersion modeling. Motor vehicle-induced emission factors were reconstructed by fitting CALINE4 to the observed concentration data with the emission factor as the sole adjustable parameter. Reconstructed fleet-average motor vehicle emission factors for the urban interstate highway were 0.03–0.04 g/VMT for both PM_2.5 and PM₁₀, while the fleet-average emission factors for the rural interstate highway were 0.2 and 0.3 g/VMT for PM_2.5 and PM₁₀, respectively.     

Spatial and temporal variations in traffic-related particulate matter at New York City high schools

Relatively little is known about exposures to traffic-related particulate matter at schools located in dense urban areas. The purpose of this study was to examine the influences of diesel traffic proximity and intensity on ambient concentrations of fine particulate matter (PM_2.5) and black carbon (BC), an indicator of diesel exhaust particles, at New York City (NYC) high schools. Outdoor PM_2.5 and BC were monitored continuously for 4–6 weeks at each of 3 NYC schools and 1 suburban school located 40 km upwind of the city. Traffic count data were obtained using an automated traffic counter or video camera. BC concentrations were 2–3 fold higher at urban schools compared with the suburban school, and among the 3 urban schools, BC concentrations were higher at schools located adjacent to highways. PM_2.5 concentrations were significantly higher at urban schools than at the suburban school, but concentrations did not vary significantly among urban schools. Both hourly average counts of trucks and buses and meteorological factors such as wind direction, wind speed, and humidity were significantly associated with hourly average ambient BC and PM_2.5 concentrations in multivariate regression models. An increase of 443 trucks/buses per hour was associated with a 0.62 μg/m³ increase in hourly average BC at an NYC school located adjacent to a major interstate highway. Car traffic counts were not associated with BC. The results suggest that local diesel vehicle traffic may be important sources of airborne fine particles in dense urban areas and consequently may contribute to local variations in PM_2.5 concentrations. In urban areas with higher levels of diesel traffic, local, neighborhood-scale monitoring of pollutants such as BC, which compared to PM_2.5, is a more specific indicator of diesel exhaust particles, may more accurately represent population exposures.     

Characteristics of water-soluble inorganic ions in PM2.5 and PM2.5–10 in the coastal urban agglomeration along the Western Taiwan Strait Region,China

PM_2.5 and PM_2.5–10 aerosol samples were collected in four seasons during November 2010, January, April, and August 2011 at 13 urban/suburban sites and one background site in Western Taiwan Straits Region (WTSR), which is the coastal area with rapid urbanization, high population density, and deteriorating air quality. The 10 days average PM_2.5 concentrations were 92.92, 51.96, 74.48, and 89.69 μg/m³ in spring, summer, autumn, and winter, respectively, exceeding the Chinese ambient air quality standard for annual average value of PM_2.5 (grade II, 35 μg/m³). Temporal distribution of water-soluble inorganic ions (WSIIs) in PM_2.5 was coincident with PM_2.5 mass concentrations, showing highest in spring, lowest in summer, and middle in autumn and winter. WSIIs took considerable proportion (42.2～50.1 %) in PM_2.5 and PM_2.5–10. Generally, urban/suburban sites had obviously suffered severer pollution of fine particles compared with the background site. The WSIIs concentrations and characteristics were closely related to the local anthropogenic activities and natural environment, urban sites in cities with higher urbanization level, or sites with weaker diffuse condition suffered severer WSIIs pollution. Fossil fuel combustion, traffic emissions, crustal/soil dust, municipal constructions, and sea salt and biomass burnings were the major potential sources of WSIIs in PM_2.5 in WTSR according to the result of principal component analysis.     

Study on ambient concentrations of PM10, PM10–2.5, PM2.5 and gaseous pollutants. Trace elements and chemical speciation of atmospheric particulates

This study provides the first comprehensive report on mass concentrations of particulate matter of various sizes, inorganic and organic gas concentrations monitored at three sampling sites in the city of Palermo (Sicily, Italy). It also provides information on the water-soluble species and trace elements. A total of 2054 PM₁₀ (1333) and PM_2.5 (721) daily measurements were collected from November 2006 to February 2008. The highest mass concentrations were observed at the urban stations, average values being about two times higher than those at the suburban (control) site. Time variations in PM₁₀ and also PM_10–2.5 were observed at the urban stations, the highest concentrations being measured in autumn and winter. CO, NOx, NO₂, benzene, toluene and o-xylene concentrations peaked in autumn and winter, a pattern similar to those recorded for PM₁₀ and PM_10–2.5 mass levels, indicating the importance of traffic emissions in urban air pollution. 91% and 51% of the benzene measurements exceeded the limit of 5 μg m^?3 at the two urban monitoring sites. Trace elements (As, Ba, Cr, Cu, Mo, Pb, Sb) suspected of being introduced into the atmosphere mainly by anthropogenic activities, were highly enriched with respect to local soil. Results indicate that a large fraction of PM₁₀ (31–47% in weight) and PM_2.5 (29% in weight) is made up of water-soluble ions. Ammonium sulphate and nitrate particles accounted for 14–29 wt% of particulate matter mass concentrations. Crustal and marine components, combined, account for 41% and 49% in PM_2.5 and PM₁₀, respectively. The calculated deficits in Cl^- and NH₄⁺ ions suggest that a proportion of these ions are lost, via the formation of gaseous NH₄Cl or HCl and NH₃.     

PM2.5 concentrations in London for 2008–A modeling analysis of contributions from road traffic

We report on the analysis of contributions from road traffic emissions to fine particulate matter (PM_2.5) concentrations within London for 2008 with the OSCAR Air Quality Assessment System. A spatiotemporal evaluation of the OSCAR system has been conducted with measurements from the London air quality network (LAQN). For the predicted and measured hourly time series of concentrations at 18 sites in London, the medians of correlation, mean absolute error, index of agreement, and factor of two (FAC2) of all stations were 0.80, 4.1 μg/m³, 0.86, and 74%, respectively. Spatial evaluation of modeled and observed annual mean concentrations also showed a fairly good agreement, with all the values falling within the FAC2 range. According to model predictions, the urban increment (including the contributions from urban traffic and other urban sources) was evaluated to be on the average 18%, 33%, 39%, and 43% of the total PM_2.5 in suburban environments, in the urban background, near roads, and near busy roads, respectively. However, the highest values of the urban traffic increment can be around 50% of the total PM_2.5 concentrations near motorways and major roads. The total concentrations (including regional background, and the contributions from urban traffic and other urban sources) can therefore be almost three times the regional background. The total urban increment close to busy roads was around 7–8 μg/m³, in which the estimated traffic contribution is more than 2 μg/m³. On the average, urban traffic contributes approximately 1 μg/m³ of PM_2.5 to the urban background across London. According to modeling, approximately two-thirds of the traffic increment originated from exhaust emissions and most of the rest was due to brake and tire wear.

Implications: The urban increment and traffic contribution to the total PM_2.5 are significant and spatially heterogeneous across London. The highly heterogeneous distribution of PM_2.5 hence requires detailed modeling studies to be carried out at high spatial resolution, which can be particularly important for exposure and health impact assessment. This type of information can be used to quantify health impacts resulting from specific sources of PM_2.5 such as traffic emissions, to aid city and national decision makers when formulating pollution control strategies.     

Characterization of PM2.5-bound polycyclic aromatic hydrocarbons in Atlanta—Seasonal variations at urban,suburban, and rural ambient air monitoring sites

Twenty-eight polycyclic aromatic hydrocarbons (PAH) and methylated PAHs (Me-PAH) were measured in daily PM_2.5 samples collected at an urban site, a suburban site, and a rural site in and near Atlanta during 2004 (5 samples/month/site). The suburban site, located near a major highway, had higher PM_2.5-bound PAH concentrations than did the urban site, and the rural site had the lowest PAH levels. Monthly variations are described for concentrations of total PAHs (∑PAHs) and individual PAHs. PAH concentrations were much higher in cold months than in warm months, with average monthly ∑PAH concentrations at the urban and suburban-highway monitoring sites ranging from 2.12 to 6.85 ng m^?3 during January–February and November–December 2004, compared to 0.38–0.98 ng m^?3 during May–September 2004. ∑PAH concentrations were found to be well correlated with PM_2.5 and organic carbon (OC) within seasons, and the fractions of PAHs in PM_2.5 and OC were higher in winter than in summer. Methyl phenanthrenes were present at higher levels than their un-substituted homologue (phenanthrene), suggesting a petrogenic (unburned petroleum products) input. Retene, a proposed tracer for biomass burning, peaked in March, the month with the highest acreage and frequency of prescribed burning and unplanned fires, and in December, during the high residential wood-burning season, indicating that retene might be a good marker for burning of all biomass materials. In contrast, potassium peaked only in December, indicating that it might be a more specific tracer for wood-burning.     

Characterization of PM2.5-bound polycyclic aromatic hydrocarbons in Atlanta

Twenty-four hour PM_2.5 samples from a rural site, an urban site, and a suburban site (next to a major highway) in the metropolitan Atlanta area in December 2003 and June 2004 were analyzed for 19 polycyclic aromatic hydrocarbons (PAH). Extraction of the air samples was conducted using an accelerated solvent extraction method followed by isotope dilution gas chromatography/mass spectrometry determination. Distinct seasonal variations were observed in total PAH concentration (i.e. significantly higher concentrations in December than in June). Mean concentrations for total particulate PAHs in December were 3.16, 4.13, and 3.40 ng m^?3 for the urban, suburban and rural sites, respectively, compared with 0.60, 0.74, and 0.24 ng m^?3 in June. Overall, the suburban site, which is impacted by a nearby major highway, had higher PAH concentration than did the urban site. Total PAH concentrations were found to be well correlated with PM_2.5, organic carbon (OC), and elemental carbon (EC) in both months (r² = 0.36–0.78, p < 0.05), although the slopes from the two months were different. PAHs represented on average 0.006% of total PM_2.5 mass and 0.017% of OC in June, compared with 0.033% of total PM_2.5 and 0.14% of OC in December. Total PAH concentrations were also correlated with potassium ion (r² = 0.39, p = 0.014) in December, but not in June, suggesting that in winter biomass burning can potentially be an important source for particulate PAH. Retene was found at a higher median air concentration at the rural site than at the urban and suburban sites—unlike the rest of the PAHs, which were found at lower levels at the rural site. Retene also had a larger seasonal difference and had the weakest correlation with the rest of the PAHs measured, suggesting that retene, in particular, might be associated with biomass burning.     

Characteristic study of particulates and metallic elements at an urban sampling site in Taichung, central Taiwan

Atmospheric total suspended particulate concentrations and metallic element concentrations were measured at three locations, characteristic of urban, suburban and rural sites. The sampling period was from July 2000 to August 2000. The results indicated that the urban sampling site had the highest total suspended particulate concentrations (average 108.61μ1m3), followed by the suburban site (average 60.11μ1m3) and the rural site (average 53.31μ1m3). The average PM_2.5 concentrations (24.11μ1m3) were higher than the PM_2.5-10 concentrations (12.81μ1m3) at the urban site. The average distributed ratios for PM_2.5/PM_2.5-10 were about 1.29, 1.53, 0.12, 1.12 and 2.31 for Pb, Zn, Fe, Ni and Cr, respectively. The average total suspended particulate mass ratios for daytime and nighttime were about 1.72. As for the elements Cu, Pb, Zn, Fe, Ni and Cr, these ratios were about 0.63, 0.97, 0.54, 1.66, 0.53 and 1.12, respectively. The total suspended particulate daytime concentrations of Pb and Zn were positively correlated (R = 0.925) at the urban sampling site. The elements Ni and Cr were positively correlated both during the daytime (R = 0.648) and the nighttime (R = 0.511), revealing that they came from the same emission source during daytime and nighttime, at the urban sampling site.     

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.     

Spatial Variability of PM2.5 in Urban Areas in the United States

Abstract

Data from the U.S. Environmental Protection Agency's Aerometric Information Retrieval System (now known as the Air Quality System) database for 1999 and 2000 have been used to characterize the spatial variability of concentrations of particulate matter with aerodynamic diameter ≤2.5 μg (PM_2.5) in 27 urban areas across the United States. Different measures were used to quantify the degree of uniformity of PM_2.5 concentrations in the urban areas characterized. It was observed that PM_2.5 concentrations varied to differing degrees in the urban areas examined. Analyses of several urban areas in the Southeast indicated high correlations between site pairs and spatial uniformity in concentration fields. Considerable spatial variation was found in other regions, especially in the West. Even within urban areas in which all site pairs were highly correlated, a variable degree of heterogeneity in PM_2.5 concentrations was found. Thus, even though concentrations at pairs of sites were highly correlated, their concentrations were not necessarily the same. These findings indicate that the potential for exposure misclassification errors in time-series epidemiologic studies exists.     

Spatial and temporal variability of outdoor coarse particulate matter mass concentrations measured with a new coarse particle sampler during the Detroit Exposure and Aerosol Research Study

The Detroit Exposure and Aerosol Research Study (DEARS) provided data to compare outdoor residential coarse particulate matter (PM_10–2.5) concentrations in six different areas of Detroit with data from a central monitoring site. Daily and seasonal influences on the spatial distribution of PM_10–2.5 during Summer 2006 and Winter 2007 were investigated using data collected with the newly developed coarse particle exposure monitor (CPEM). These data allowed the representativeness of the community monitoring site to be assessed for the greater Detroit metro area. Multiple CPEMs collocated with a dichotomous sampler determined the precision and accuracy of the CPEM PM_10–2.5 and PM_2.5 data.CPEM PM_2.5 concentrations agreed well with the dichotomous sampler data. The slope was 0.97 and the R² was 0.91. CPEM concentrations had an average 23% negative bias and R² of 0.81. The directional nature of the CPEM sampling efficiency due to bluff body effects probably caused the negative CPEM concentration bias.PM_10–2.5 was observed to vary spatially and temporally across Detroit, reflecting the seasonal impact of local sources. Summer PM_10–2.5 was 5 μg m^?3 higher in the two industrial areas near downtown than the average concentrations in other areas of Detroit. An area impacted by vehicular traffic had concentrations 8 μg m^?3 higher than the average concentrations in other parts of Detroit in the winter due to the suspected suspension of road salt. PM_10–2.5 Pearson Correlation Coefficients between monitoring locations varied from 0.03 to 0.76. All summer PM_10–2.5 correlations were greater than 0.28 and statistically significant (p-value < 0.05). Winter PM_10–2.5 correlations greater than 0.33 were statistically significant (p-value < 0.05). The PM_10–2.5 correlations found to be insignificant were associated with the area impacted by mobile sources during the winter. The suspected suspension of road salt from the Southfield Freeway, combined with a very stable atmosphere, caused concentrations to be greater in this area compared to other areas of Detroit. These findings indicated that PM_10–2.5, although correlated in some instances, varies sufficiently across a complex urban airshed that that a central monitoring site may not adequately represent the population's exposure to PM_10–2.5.     

Studies of the coarse particle (2.5–10 μm) component in UK urban atmospheres

An analysis is presented of continuous simultaneous measurement data for PM₁₀ and PM_2.5 using TEOM instruments from five sites in the United Kingdom. The results are analysed specifically in relation to the sources and processes influencing the coarse particle fraction (2.5–10 μm). The data show a generally strong correlation between fine and coarse particle concentrations at all sites, with a generally higher proportion of coarse particles in the dryer months of the year. The one rural site shows a notably lower proportion of coarse particles than the urban and suburban sites. Whilst it is possible to disaggregate the coarse particle concentrations into a component which is diluted by increasing windspeed and a component which increases with windspeed and is hence possibly attributable to wind-induced resuspension processes, the latter is only a minor proportion of the total coarse particle concentration. There are appreciable weekday-to-weekend and day-to-night differences between coarse particle concentrations which are most marked at the urban sites indicative of anthropogenic activities being a source of coarse particles. The clearest indication of the likely predominant source of coarse particles arises from an analysis of a data set derived from an urban street canyon site after subtraction of measurements from a nearby urban background location. The data indicate strong relationships of both fine and coarse incremental particle concentrations in the street canyon with incremental NO_x. If incremental fine particles and coarse particles are attributed to exhaust emissions and vehicle-induced resuspension, respectively, then it may be concluded that vehicle-induced resuspension provides a source strength approximately equal to that of exhaust emissions. An analysis of the coarse particle concentration data suggest that episodes of elevated coarse particle concentrations alone very rarely lead to exceedence of the UK air quality standard for PM₁₀ of 50 μg m⁻³ measured as a 24-h running mean.     

Determination of sources of fine particles in different ambient atmospheres in South Korea using a chemical mass balance model

Abstract

To determine the sources of particulate matter less than 2.5?μm (PM_2.5 in different ambient atmospheres (urban, roadside, industrial, and rural sites), the chemical components of PM_2.5 such as ions (Cl^-, NO₃^-, SO₄^2-, NH₄⁺, Na⁺, K⁺, Ca²⁺, and Mg²⁺), carbonaceous species, and elements (Al, As, Ba, Cd, Cu, Fe, Mn, Ni, Pb, Se, V, and Zn) were measured. The average mass concentrations of PM_2.5 at the urban, roadside, industrial, and rural sites were 31.5?±?14.8, 31.6?±?22.3, 31.4?±?16.0, and 25.8?±?12.4?μg/m³, respectively. Except for secondary ammonium sulfate and ammonium nitrate, the model results showed that the traffic source (i.e., the sum of gasoline and diesel vehicle sources) was the most dominant source of PM_2.5 (17.1%) followed by biomass burning (13.8%) at the urban site. The major primary sources of PM_2.5 were consistent with the site characteristics (diesel vehicle source at the roadside site, coal-fired plants at the industrial site, and biomass burning at the rural site). Seasonal data from the urban site suggested that ammonium sulfate and ammonium nitrate were the most dominant sources of PM_2.5 during all seasons. Further, the contribution of road dust source to PM_2.5 increased during spring and fall seasons. We conclude that the determination of the major PM_2.5 sources is useful for establishing efficient control strategies for PM_2.5 in different regions and seasons.     

Spatial variation of particle number and mass over four European cities

The number of ultrafine particles may be a more health relevant characteristic of ambient particulate matter than the conventionally measured mass. Epidemiological time series studies typically use a central site to characterize human exposure to outdoor air pollution. There is currently very limited information how well measurements at a central site reflect temporal and spatial variation across an urban area for particle number concentrations (PNC).The main objective of the study was to assess the spatial variation of PNC compared to the mass concentration of particles with diameter less than 10 or 2.5 μm (PM₁₀ and PM_2.5).Continuous measurements of PM₁₀, PM_2.5, PNC and soot concentrations were conducted at a central site during October 2002–March 2004 in four cities spread over Europe (Amsterdam, Athens, Birmingham and Helsinki). The same measurements were conducted directly outside 152 homes spread over the metropolitan areas. Each home was monitored during 1 week. We assessed the temporal correlation and the variability of absolute concentrations.For all particle indices, including particle number, temporal correlation of 24-h average concentrations was high. The median correlation for PNC per city ranged between 0.67 and 0.76. For PM_2.5 median correlation ranged between 0.79 and 0.98. The median correlation for hourly average PNC was lower (range 0.56–0.66). Absolute concentration levels varied substantially more within cities for PNC and coarse particles than for PM_2.5. Measurements at the central site reflected the temporal variation of 24-h average concentrations for all particle indices at the selected homes across the urban area. A central site could not assess absolute concentrations across the urban areas for particle number.     

Attainment Flip-Flops and the Achievability of the Ozone Air Quality Standard

Abstract

This paper presents the results of the first reported study on fine particulate matter (PM) chemical composition at Salamanca, a highly industrialized urban area of Central Mexico. Samples were collected at six sites within the urban area during February and March 2003. Several trace elements, organic carbon (OC), elemental carbon (EC), and six ions were analyzed to characterize aerosols. Average concentrations of PM with aerodynamic diameter of less than 10 μm (PM₁₀) and fine PM with aerodynamic diameter of less than 2.5 μm (PM_2.5) ranged from 32.2 to 76.6 μg m^-3 and 11.1 to 23.7 μg m^-3, respectively. OC (34%), SO₄ ⁼ (25.1%), EC (12.9%), and geological material (12.5%) were the major components of PM_2.5. For PM₁₀, geological material (57.9%), OC (17.3%), and SO₄ ⁼ (9.7%) were the major components. Coarse fraction (PM₁₀ –PM_2.5), geological material (81.7%), and OC (8.6%) were the dominant species, which amounted to 90.4%. Correlation analysis showed that sulfate in PM_2.5 was present as ammonium sulfate. Sulfate showed a significant spatial variation with higher concentrations to the north resulting from predominantly southwesterly winds above the surface layer and by major SO₂ sources that include a power plant and refinery. At the urban site of Cruz Roja it was observed that PM_2.5 mass concentrations were similar to the submicron fraction concentrations. Furthermore, the correlation between EC in PM_2.5 and EC measured from an aethalometer was r² = 0.710. Temporal variations of SO₂ and nitrogen oxide were observed during a day when the maximum concentration of PM_2.5 was measured, which was associated with emissions from the nearby refinery and power plant. From cascade impactor measurements, the three measured modes of airborne particles corresponded with diameters of 0.32, 1.8, and 5.6 μm.     

Comparison of Fine Particles and the Relationship between Particle Variations and Meteorology at an Urban Site and a Remote Site in the Eastern United States

Abstract

This study compared the variations in the mass of certain particles at an urban site, Washington, DC, and at a remote site, Shenandoah National Park, VA, in the eastern United States. Seven years (1991-1997) of Interagency Monitoring of Protected Visual Environments (IMPROVE) fine particulate matter (PM_2.5), PM₁₀, coarse fraction, SO₄ ^2?, and total sulfur data were used for this study together with available meteorology/climatology data. Various statistical modeling and analysis procedures, including time series analysis, factor analysis, and regression modeling, were employed. Time series of the constituents were divided into four terms: the long-term mean, the intra-annual perturbation, the interannual perturbation, and the synoptic perturbation. PM_2.5 at the two sites made up ~72% of the total mass for PM₁₀, and the coarse fraction made up the remaining 28%, on average. Thirty-one percent of the PM_2.5 at the DC site and 42% at the Shenandoah site was SO₄ ^2?, based on average data for the entire period. At the DC site, the two main contributors to the constituent mass were the long-term mean and the synoptic perturbation terms, and at the Shenandoah site, they were the long-term mean and the intra-annual perturbation terms. This suggested that the constituent mass at the two sites was affected by very different processes. The terms that provided the principal contribution to the constituent mass at the two sites were studied in detail.

At the DC site, dew point trends, a climate variable, were the primary driver of the 7-year trends for PM_2.5, PM₁₀, the coarse fraction, and total sulfur, and SO₂ emission trends were the primary driver of the trends for SO₄ ^2?. SO₂ emission trends influenced the trends for PM_2.5 and total sulfur, appearing as the second term in the model, but only parameters dealing with climate trends had significant effects on the trends for PM₁₀ and the coarse fraction. At the Shenandoah site, only parameters dealing with climate trends affected long-term particle trends.     

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.     

Observations and Interpretations from the Canadian Fine Particle Monitoring Program

ABSTRACT

Canadian particle monitoring programs examining PM10, PM2.5, and particle composition have been in operation for over 10 years. Until recently, the measurements were manual/filter-based with 24-hr sample collection varying in frequency from daily to every sixth day, using GrasebyAnderson dichotomous samplers. In the past few years, these monitoring activities have been expanded to include hourly measurements using tapered element oscillating microbalances (TEOMs). This continuous monitoring program started operation focusing on PM_10, but now emphasizes PM_2.5 through the addition of more TEOMs and switching of the inlets of some of the existing units. The data from all of these measurement activities show that there are broad geographical differences and also local- to regional-scale spatial differences in mass and composition of PM2.5. Due to variations in sources, significantly different PM2.5 concentrations are not uncommon within the same city. Comparison of nearby urban and rural sites indicates that 30 and 40% of the PM_2.5 is from local urban sources in Montreal and Toronto, respectively. Hourly PM_2.5 measurements in Toronto suggest that vehicular emissions are an important contributor to urban PM_2.5. There has been a decreasing trend in urban PM_2.5, with annual average concentrations between the 1987–1990 and 1993–1995 periods decreasing by 11 to 39%, depending upon the site. The largest declines were in Montreal and Halifax, and the smallest decline was in Toronto. Comparison of 24-hr TEOM and manual dichotomous sampler PM_2.5 measurements from a site in Toronto indicates that the TEOM results in lower concentrations. The magnitude of this difference is relatively small in the warmer months, averaging about 12%. During the colder months the difference averages about 23%, but can be as large as 50%.     

Discriminating the regional and urban contributions in the North-Western Mediterranean: PM levels and composition

Simultaneous measurements of the PM concentration levels and chemical composition of atmospheric aerosols at a regional background (RB) and an urban background (UB) site, located in the same geographic region, allowed for the determination of their urban and regional contributions. In the specific case of the North-Western region of the Mediterranean the RB amount has been quantified in 18, 13 and 12 μg m^?3 for PM₁₀, PM_2.5 and PM₁, respectively, whereas the UB contribution reached 22, 13 and 8 μg m^?3, respectively. The UB contributions in the Western Mediterranean are much higher than those observed in other European regions; especially concerning the coarse fraction. The high loads of road dust in the urban areas across the Mediterranean may account for these large differences.The urban contributions are extremely enriched in Ca, Fe, Sb, Sn, Cu, Zn, being the main tracers of the road dust, with concentrations up to 6–8 times higher than those at the RB. Elemental carbon and nitrate are mainly derived from direct vehicular emissions. Some industrial tracers (Mn, Pb, Bi) are also enriched in the urban area. The evaluation of the Cu/Sb, Cu/Zn, Cu/Cd and Cu/Pb ratios and the high enrichment of these trace elements versus the Upper Crustal Composition average values corroborates the importance of the road-traffic emissions in the study area, also influencing the RB.The supplementary results from a suburban site in the Balearic Islands and the evaluation of the V/Ni ratios evidence the strong signature of fuel-oil combustion processes, which is a general characteristic of the Mediterranean aerosols.     

Characterizing and predicting coarse and fine particulates in classrooms located close to an urban roadway

The PM₁₀, PM_2.5, and PM₁ (particulate matter with aerodynamic diameters <10, <2.5, and <1 μm, respectively) concentrations were monitored over a 90-day period in a naturally ventilated school building located at roadside in Chennai City. The 24-hr average PM₁₀, PM_2.5, and PM₁ concentrations at indoor and outdoor environments were found to be 136 ± 60, 36 ± 15, and 20 ± 12 and 76 ± 42, 33 ± 16, and 23 ± 14 μg/m³, respectively. The size distribution of PM in the classroom indicated that coarse mode was dominant during working hours (08:00 a.m. to 04:00 p.m.), whereas fine mode was dominant during nonworking hours (04:00 p.m. to 08:00 a.m.). The increase in coarser particles coincided with occupant activities in the classrooms and finer particles were correlated with outdoor traffic. Analysis of indoor PM₁₀, PM_2.5, and PM₁ concentrations monitored at another school, which is located at urban reserved forest area (background site) indicated 3–4 times lower PM₁₀ concentration than the school located at roadside. Also, the indoor PM₁ and PM_2.5 concentrations were 1.3–1.5 times lower at background site. Further, a mass balance indoor air quality (IAQ) model was modified to predict the indoor PM concentration in the classroom. Results indicated good agreement between the predicted and measured indoor PM_2.5 (R² = 0.72–0.81) and PM₁ (R² = 0.81–0.87) concentrations. But, the measured and predicted PM₁₀ concentrations showed poor correlation (R² = 0.17–0.23), which may be because the IAQ model could not take into account the sudden increase in PM₁₀ concentration (resuspension of large size particles) due to human activities.

Implications:The present study discusses characteristics of the indoor coarse and fine PM concentrations of a naturally ventilated school building located close to an urban roadway and at a background site in Chennai City, India. The study results will be useful to engineers and policymakers to prepare strategies for improving the IAQ inside classrooms. Further, this study may help in the development of IAQ standards and guidelines in India.