Seasonal and spatial trends in the sources of fine particle organic carbon in Israel,Jordan, and Palestine

A study of carbonaceous particulate matter (PM) was conducted in the Middle East at sites in Israel, Jordan, and Palestine. The sources and seasonal variation of organic carbon, as well as the contribution to fine aerosol (PM_2.5) mass, were determined. Of the 11 sites studied, Nablus had the highest contribution of organic carbon (OC), 29%, and elemental carbon (EC), 19%, to total PM_2.5 mass. The lowest concentrations of PM_2.5 mass, OC, and EC were measured at southern desert sites, located in Aqaba, Eilat, and Rachma. The OC contribution to PM_2.5 mass at these sites ranged between 9.4% and 16%, with mean annual PM_2.5 mass concentrations ranging from 21 to 25 ug m^?3. These sites were also observed to have the highest OC to EC ratios (4.1–5.0), indicative of smaller contributions from primary combustion sources and/or a higher contribution of secondary organic aerosol. Biomass burning and vehicular emissions were found to be important sources of carbonaceous PM in this region at the non-southern desert sites, which together accounted for 30%–55% of the fine particle organic carbon at these sites. The fraction of measured OC unapportioned to primary sources (1.4 μgC m^?3 to 4.9 μgC m^?3; 30%–74%), which has been shown to be largely from secondary organic aerosol, is relatively constant at the sites examined in this study. This suggests that secondary organic aerosol is important in the Middle East during all seasons of the year.     

Chemical characteristics of principal PM2.5 species in Chongju,South Korea

Fine particles were collected over four seasons from October 1995 to August 1996 to evaluate the chemical characteristics of principal PM_2.5 components in Chongju, South Korea. The annual mean concentrations of PM_2.5 (d_p⩽2.5 μm), sulfate, nitrate, ammonium, elemental carbon (EC) and organic carbon (OC) were 44.2, 8.22, 3.63, 2.84, 4.44 and 4.99 μg m⁻³, respectively. The sum of the species measured from this study accounted for 50–62% of the PM_2.5 mass. Sulfate was the most abundant species and constituted 13–23% of the PM_2.5 mass. The EC and OC accounted for 17–28% of PM_2.5. The correlation between OC and EC was strong, and the annual mean ratio of OC/EC was 1.12, suggesting that OC measured in the Chongju area may be emitted directly in particulate form as a primary aerosol.     

Long-term variation of PM2.5 levels and composition at rural, urban, and roadside sites in Hong Kong: Increasing impact of regional air pollution

Long-term study of air pollution plays a decisive role in formulating and refining pollution control strategies. In this study, two 12-month measurements of PM_2.5 mass and speciation were conducted in 00/01 and 04/05 to determine long-term trend and spatial variations of PM_2.5 mass and chemical composition in Hong Kong. This study covered three sites with different land-use characteristics, namely roadside, urban, and rural environments. The highest annual average PM_2.5 concentration was observed at the roadside site (58.0±2.0 μg m⁻³ (average±2σ) in 00/01 and 53.0±2.7 μg m⁻³ in 04/05), followed by the urban site (33.9±2.5 μg m⁻³ in 00/01 and 39.0±2.0 μg m⁻³ in 04/05), and the rural site (23.7±1.9 μg m⁻³ in 00/01 and 28.4±2.4 μg m⁻³ in 04/05). The lowest PM_2.5 level measured at the rural site was still higher than the United States’ annual average National Ambient Air Quality Standard of 15 μg m⁻³. As expected, seasonal variations of PM_2.5 mass concentration at the three sites were similar: higher in autumn/winter and lower in summer. Comparing PM_2.5 data in 04/05 with those collected in 00/01, a reduction in PM_2.5 mass concentration at the roadside (8.7%) but an increase at the urban (15%) and rural (20%) sites were observed. The reduction of PM_2.5 at the roadside was attributed to the decrease of carbonaceous aerosols (organic carbon and elemental carbon) (>30%), indicating the effective control of motor vehicle emissions over the period. On the other hand, the sulfate concentration at the three sites was consistent regardless of different land-use characteristics in both studies. The lack of spatial variation of sulfate concentrations in PM_2.5 implied its origin of regional contribution. Moreover, over 36% growth in sulfate concentration was found from 00/01 to 04/05, suggesting a significant increase in regional sulfate pollution over the years. More quantitative techniques such as receptor models and chemical transport models are required to assess the temporal variations of source contributions to ambient PM_2.5 mass and chemical speciation in Hong Kong.     

Temporal characteristics from continuous measurements of PM2.5 and speciation at the Taipei Aerosol Supersite from 2002 to 2008

This study uses monitoring data collected at the Taipei Aerosol Supersite from March 2002 to February 2008 to analyze characteristics such as seasonal fluctuations, diurnal variations, and photochemical-related variations of PM_2.5 chemical compositions. The results indicate that the average of PM_2.5 mass concentration in Taipei during this period is 30.3 ± 16.0 μg m^?3. The highest average concentration of PM_2.5 components is that of sulfate, which accounts for 21.1% of the PM_2.5 mass, followed by organic carbon (OC) at 15.9%, nitrate at 5.8%, and elemental carbon (EC) at 5.4%. Concentrations of EC, OC, and nitrate have distinctive but similar seasonal fluctuations, which is highest in spring and lowest in fall. Sulfate concentration has less seasonal fluctuations, and the highest value appears during the fall. Similarly, concentrations of EC, OC, and nitrate have notable diurnal variations; however, the diurnal variation of sulfate concentration is not very apparent. These observation data show that EC, OC, and nitrate in PM_2.5 in the Taipei metropolis come mainly from local emissions, while sulfate comes mainly from the regional transport of pollutants. This is likely because Taiwan is located on the lee zone of the Asian prevailing winds from fall to spring; its air quality is frequently affected by the transport of air pollutants from Mainland China. In addition, the extent of increase in aerosols is much higher than that of CO, indicating the formation of secondary aerosol when photochemical activity is strong. Based on six years of observation data, this study explores three potential scenarios to set up Taiwan's PM_2.5 air quality standard (AQS). The analysis indicates that the optimum standard for 24-h air quality of PM_2.5 should be around 50 μg m^?3.     

Characteristics of vertical profiles and sources of PM2.5, PM10 and carbonaceous species in Beijing

In August 2003 during the anticipated month of the 2008 Beijing Summer Olympic Games, we simultaneously collected PM₁₀ and PM_2.5 samples at 8, 100, 200 and 325 m heights up a meteorological tower and in an urban and a suburban site in Beijing. The samples were analysed for organic carbon (OC) and elemental carbon (EC) contents. Particulate matter (PM) and carbonaceous species pollution in the Beijing region were serious and widespread with 86% of PM_2.5 samples exceeding the daily National Ambient Air Quality Standard of the USA (65 μg m⁻³) and the overall daily average PM₁₀ concentrations of the three surface sites exceeding the Class II National Air Quality Standard of China (150 μg m⁻³). The maximum daily PM_2.5 and PM₁₀ concentrations reached 178.7 and 368.1 μg m⁻³, respectively, while those of OC and EC reached 22.2 and 9.1 μg m⁻³ in PM_2.5 and 30.0 and 13.0 μg m⁻³ in PM₁₀, respectively. PM, especially PM_2.5, OC and EC showed complex vertical distributions and distinct layered structures up the meteorological tower with elevated levels extending to the 100, 200 and 300 m heights. Meteorological evidence suggested that there exist fine atmospheric layers over urban Beijing. These layers were featured by strong temperature inversions close to the surface (<50 m) and more stable conditions aloft. They enhanced the accumulation of pollutants and probably caused the complex vertical distributions of PM and carbonaceous species over urban Beijing. The built-up of PM was accompanied by transport of industrial emissions from the southwest direction of the city. Emissions from road traffic and construction activities as well as secondary organic carbon (SOC) are important sources of PM. High OC/EC ratios (range of 1.8–5.1 for PM_2.5 and 2.0–4.3 for PM₁₀) were found, especially in the higher levels of the meteorological tower suggesting there were substantial productions of SOC in summer Beijing. SOC is estimated to account for at least 33.8% and 28.1% of OC in PM_2.5 and PM₁₀, respectively, with higher percentages at the higher levels of the tower.     

Particulate matter emissions from on-road vehicles in a freeway tunnel study

Particulate matter, including coarse particles (PM_2.5–10, aerodynamic diameter of particle between 2.5 and 10 μm) and fine particles (PM_2.5, aerodynamic diameter of particle lower than 2.5 μm) and their compositions, including elemental carbon, organic carbon, and 11 water-soluble ionic species, and elements, were measured in a tunnel study. A comparison of the six-hour average of light-duty vehicle (LDV) flow of the two sampling periods showed that the peak hours over the weekend were higher than those on weekdays. However, the flow of heavy-duty vehicles (HDVs) on the weekdays was significant higher than that during the weekend in this study. EC and OC content were 49% for PM_2.5–10 and 47% for PM_2.5 in the tunnel center. EC content was higher than OC content in PM_2.5–10, but EC was about 2.3 times OC for PM_2.5. Sulfate, nitrate, ammonium were the main species for PM_2.5–10 and PM_2.5. The element contents of Na, Al, Ca, Fe and K were over 0.8 μg m^?3 in PM_2.5–10 and PM_2.5. In addition, the concentrations of S, Ba, Pb, and Zn were higher than 0.1 μg m^?3 for PM_2.5–10 and PM_2.5. The emission factors of PM_2.5–10 and PM_2.5 were 18 ± 6.5 and 39 ± 11 mg km^?1-vehicle, respectively. The emission factors of EC/OC were 3.6/2.7 mg km^?1-vehicle for PM_2.5–10 and 15/4.7 mg km^?1-vehicle for PM_2.5 Furthermore, the emission factors of water-soluble ions were 0.028(Mg²⁺)–0.81(SO₄^2?) and 0.027(NO₂^?)–0.97(SO₄^2?) mg km^?1-vehicle for PM_2.5–10 and PM_2.5, respectively. Elemental emission factors were 0.003(V)–1.6(Fe) and 0.001(Cd)–1.05(Na) mg km^?1-vehicle for PM_2.5–10 and PM_2.5, respectively.     

The characteristics of PM2.5 in Beijing,China

Weekly PM_2.5 samples were simultaneously collected at a residential (Tsinghua University) and a downtown (Chegongzhuang) site in Beijing from July 1999 through September 2000. The ambient mass concentration and chemical composition of the PM_2.5 were determined. Analyses included elemental composition, water-soluble ions, and organic and elemental carbon. Weekly PM_2.5 mass concentrations ranged from 37 to 357 μg/m³, with little difference found between the two sites. Seasonal variation of PM_2.5 concentrations was significant, with the highest concentration in the winter and the lowest in the summer. Spring dust storms had a strong impact on the PM_2.5. Overall, organic carbon was the most abundant species, constituting no less than 30% of the total PM_2.5 mass at both sites. Concentrations of organic and elemental carbon were 35% and 16% higher at Tsinghua University than at Chegongzhuang. Ammonium, nitrate and sulfate were comparable at the sites, accounting for 25–30% of the PM_2.5 mass.     

PM2.5 particles and size-segregated ionic species measured during fall season in three urban sites in Korea

Twelve hours integrated fine particles (PM_2.5) and 24-h average size-segregated particles were collected to investigate the chemical characteristics and to determine the size distribution of ionic species during October–December 1999 in three cities of different urban scale; Chongju, Kwangju, and Seoul, Korea. Concentrations of 5-min PM_2.5 black carbon (BC) and hourly criteria air pollutants (PM₁₀, CO, NO_x, SO₂, and O₃) were also measured using the Aethalometer and ambient air monitoring system, respectively.Highest PM_2.5 mass concentrations at Chongju, Kwangju, and Seoul sites were 63.0, 77.9, and 143.7 μg m⁻³, respectively. For the time period when highest PM_2.5 mass occurred, BC level out of PM_2.5 chemical species was highest at both Chongju and Kwangju, and highest NO₃⁻ (23.6 μg m⁻³) followed by BC (23.1 μg m⁻³) were observed at Seoul site, indicating that highest PM_2.5 pollution is closely associated with the traffic emissions. Strong relationships of Fe with BC and Zn at both Kwangju and Seoul sites support that the Fe and Zn measured there are originated partly from same source as BC, i.e. diesel traffics. However, it is suggested that the Fe measured at Chongju is most likely derived from dispersion of soil dust.The size distributions of SO₄²⁻, NO₃⁻, and NH₄⁺ ionic species indicated similar unimodal distributions at all sampling sites. However, different unimodal patterns in the accumulation mode size range with a peak in the smaller size (0.28–0.53 μm, condensation mode) in both Kwangju and Seoul, and in the relatively larger size (0.53–1.0 μm, droplet mode) in Chongju, were found. The potassium ion under the study sites dominates in the fine mode, and its size distribution showed unimodal character with a maximum in the size range 0.56–1.0 μm.     

Effect of SME biodiesel blends on PM2.5 emission from a heavy-duty engine

To explore the effect of biodiesel and sulfur content on PM_2.5 emissions, engine dynamometer tests were performed on a Euro II engine to compare the PM_2.5 emissions from four fuels: two petroleum diesel fuels with sulfur contents of 50 and 100 ppm respectively, and two B20 fuels in which soy methyl ester (SME) biodiesel was added to each of the above mentioned petroleum diesel fuels (v/v: 80%/20% for petroleum diesel and SME respectively). Gaseous pollutants and PM_2.5 emissions were sampled with an AVL AMA4000 and Model 130 High-Flow Impactor (MSP Corp). Measurements were made of the PM_2.5 mass, organic carbon (OC), elemental carbon (EC) and the water-soluble ion distribution. The results showed that PM_2.5 emissions decreased with lower sulfur content or blending with SME biodiesel, and the decrease would be more by applying both two methods together. Particles of approximately 0.13 μm contributed 48–83% of PM_2.5 emissions. The impact of sulfur content on this percentage was different for low and high engine speed. The majority of PM_2.5 was comprised of OC and EC, and the carbon emission rate had the same trend as PM_2.5. Since the EC abatement of B20 was larger than OC, the OC/EC ratio of B20 was always larger than that of petroleum diesel. For petroleum diesel, the OC/EC increased with sulfur content, which was not the case for B20. The SO₄^2? had highest emission rate in the water-soluble ions of PM.     

Sources and characteristics of carbonaceous aerosol in two largest cities in Pearl River Delta Region,China

PM_2.5 samples were collected at five sites in Guangzhou and Hong Kong, Pearl River Delta Region (PRDR), China in both summer and winter during 2004–2005. Elemental carbon (EC) and organic carbon (OC) in these samples were measured. The OC and EC concentrations ranked in the order of urban Guangzhou > urban Hong Kong > background Hong Kong. Total carbonaceous aerosol (TCA) contributed less to PM_2.5 in urban Guangzhou (32–35%) than that in urban Hong Kong (43–57%). The reason may be that, as an major industrial city in South China, Guangzhou would receive large amount of inorganic aerosol from all kinds of industries, however, as a trade center and seaport, urban Hong Kong would mainly receive organic aerosol and EC from container vessels and heavy-duty diesel trucks. At Hong Kong background site Hok Tsui, relatively lower contribution of TCA to PM_2.5 may result from contributions of marine inorganic aerosol and inland China pollutant. Strong correlation (R²=0.76–0.83) between OC and EC indicates minor fluctuation of emission and the secondary organic aerosol (SOA) formation in urban Guangzhou. Weak correlation between OC and EC in Hong Kong can be related to the impact of the long-range transported aerosol from inland China. Averagely, secondary OC (SOC) concentrations were 3.8–5.9 and 10.2–12.8 μg m⁻³, respectively, accounting for 21–32% and 36–42% of OC in summer and winter in Guangzhou. The average values of 4.2–6.8% for SOA/ PM_2.5 indicate that SOA was minor component in PM_2.5 in Guangzhou.     

Organic and elemental carbon associated to PM10 and PM2.5 at urban sites of northern Greece

Organic carbon (OC) and elemental carbon (EC) concentrations, associated to PM₁₀ and PM_2.5 particle fractions, were concurrently determined during the warm and the cold months of the year (July–September 2011 and February–April 2012, respectively) at two urban sites in the city of Thessaloniki, northern Greece, an urban-traffic site (UT) and an urban-background site (UB). Concentrations at the UT site (11.3?±?5.0 and 8.44?±?4.08 14 μg m^?3 for OC₁₀ and OC_2.5 vs. 6.56?±?2.14 and 5.29?±?1.54 μg m^?3 for EC₁₀ and EC_2.5) were among the highest values reported for urban sites in European cities. Significantly lower concentrations were found at the UB site for both carbonaceous species, particularly for EC (6.62?±?4.59 and 5.72?±?4.36 μg m^?3 for OC₁₀ and OC_2.5 vs. 0.93?±?0.61 and 0.69?±?0.39 μg m^?3 for EC₁₀ and EC_2.5). Despite that, a negative UT-UB increment was frequently evidenced for OC_2.5 and PM_2.5 in the cold months possibly indicative of emissions from residential wood burning at the urban-background site. At both sites, cconcentrations of OC fractions were significantly higher in the cold months; on the contrary, EC fractions at the UT site were prominent in the warm season suggesting some influence from maritime emissions in the nearby harbor area. Secondary organic carbon, being estimated using the EC tracer method and seasonally minimum OC/EC ratios, was found to be an appreciable component of particle mass particularly in the cold season. The calculated secondary contributions to OC ranged between 35 and 59 % in the PM₁₀ fraction, with relatively higher values in the PM_2.5 fraction (39–61 %). The source origin of carbonaceous species was investigated by means of air parcel back trajectories, satellite fire maps, and concentration roses. A local origin was mainly concluded for OC and EC with limited possibility for long range transport of biomass (agricultural waste) burning aerosol.     

Determination of Source Contributions to Ambient PM2.5 in Kaohsiung,Taiwan, Using a Receptor Model

ABSTRACT

Ambient particulates of PM_2.5 were sampled at three sites in Kaohsiung, Taiwan, during February and March 1999. In addition, resuspended PM_2.5 collected from traffic tunnels, paved roads, fly ash of a municipal solid waste (MSW) incinerator, and seawater was obtained. All the samples were analyzed for twenty constituents, including water-soluble ions, organic carbon (OC), elemental carbon (EC), and metallic elements. In conjunction with local source profiles and the source profiles in the model library SPECIATE EPA, the receptor model based on chemical mass balance (CMB) was then applied to determine the source contributions to ambient PM_2.5.

The mean concentration of ambient PM_2.5 was 42.6953.68 μj.g/m³ for the sampling period. The abundant species in ambient PM_2.5 in the mass fraction for three sites were OC (12.7-14.2%), SO₄ ^2- (12.8-15.1%), NO₃ ^- (8.110.3%), NH₄+ (6.7-7.5%), and EC (5.3-8.5%). Results of CMB modeling show that major pollution sources for ambient PM_2.5 are traffic exhaust (18-54%), secondary aerosols (30-41% from SO₄ ^2- and NO₃ ^-), and outdoor burning of agriculture wastes (13-17%).     

Concentrations of ultrafine,fine and PM2.5 particles in three European cities

Total number concentrations, number concentrations of ultrafine (0.01–0.1 μm) and accumulation (0.1–0.5 μm) particles, as well as mass concentration of PM_2.5 particles and blackness of PM_2.5 filters, which is related to Black Smoke were simultaneously monitored in three European cities during the winter period for three and a half months. The purpose of the study was to describe the differences in concentration levels and daily and diurnal variations in particle number and mass concentrations between European cities. The results show statistically significant differences in the concentrations of PM_2.5 and the blackness of the PM_2.5 filters between the cities, but not in the concentrations of ultrafine particles. Daily PM_2.5 levels were found to be poorly correlated with the daily total and ultrafine number concentrations but better correlated with the number concentration of accumulation particles. According to the principal component analysis airborne particulate pollutants seem to be divided into two major source categories, one identified with particle number concentrations and the other related to mass-based information. The present results underline the importance of using both particle number and mass concentrations to evaluate urban air quality.     

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.     

Exposure of PM2.5 and EC from diesel and gasoline vehicles in communities near the Ports of Los Angeles and Long Beach,California

The Ports of Los Angeles and Long Beach are the entry point for almost half of all cargo containers entering the United States. The use of diesel trucks to move Port-related goods has raised significant public health concerns associated with black carbon and other air pollutants. It is difficult to reliably estimate people's exposure to vehicle-related pollutants due to the narrow impact zone of traffic, usually within 200–300 m downwind of major roadways. Previous studies suffer from the lack of traffic count data on surface streets and the lack of neighborhood-level population data. We examined seasonal and annual average exposures of particulate matter less than 2.5 μm (PM_2.5) and elemental carbon (EC) at a neighborhood scale for communities heavily impacted by diesel trucks near these ports. We assembled a traffic-activity database that distinguishes gasoline and diesel vehicles on both freeways and surface streets, by consolidating information from several sources, including our own field measurements. The CALINE4 model was used to estimate residential exposure of the study population to PM_2.5 and EC. Parcel property data were used to allocate Census block group (BG) population to increase spatial resolution. The annual average PM_2.5 and EC exposure due to local traffic was 3.8 and 0.4 μg m^?3, respectively. On average, surface streets contributed a little more than freeways (55% vs. 45% for EC and 57% and 43% for PM_2.5). Light-duty vehicles contributed significantly more than heavy-duty trucks for PM_2.5 (61% vs. 39%), but slightly less than heavy-duty trucks for EC (49% vs. 51%). Community mean population exposure was similar using parcel, census block, and BG population data, but extreme values and standard deviations varied significantly at different spatial resolutions. The intake fraction for the study population was in the range of 1.0–2.2 × 10^?5 by vehicle type, roadway type, and season.     

Spatial variation of mass concentration of roadside suspended particulate matter in metropolitan Hong Kong

This study conducted roadside particulate sampling to measure the total suspended particulate (TSP), PM₁₀ (particles <10 μm in aerodynamic diameter) and PM_2.5 (particles <2.5 μm in aerodynamic diameter) mass concentration in 11 urbanized and densely populated districts in Hong Kong. One hundred and thirty-three samples were obtained to measure the mass concentrations of TSP, PM₁₀ and PM_2.5. According to these results, the TSP, PM₁₀ and PM_2.5 mass concentrations varied from 94.85 to 301.63 μg m⁻³, 67.67 to 142.68 μg m⁻³ and 50.01 to 125.12 μg m⁻³, respectively. The PM_2.5/PM₁₀ ratio of all samples was 0.82 which ranged from 0.62 to 0.95. The PM levels and PM ratios in metropolitan Hong Kong significantly fluctuated from site-to-site and over time. The PM_2.5 mass concentration in different districts corresponding to urban industrial, new town, urban residential and urban commercial were 77.64, 87.50, 106.96 and 88.54 μg m⁻³, respectively. The PM_2.5 level is high in Hong Kong, and for individual sampling, more than 60% daily measurements exceeded the NAAQS. The mass fraction of PM_2.5 in PM₁₀ and TSP is relatively high when compared with overseas studies.     

Correlations between fine particulate matter (PM2.5) and meteorological variables in the United States: Implications for the sensitivity of PM2.5 to climate change

We applied a multiple linear regression (MLR) model to study the correlations of total PM_2.5 and its components with meteorological variables using an 11-year (1998–2008) observational record over the contiguous US. The data were deseasonalized and detrended to focus on synoptic-scale correlations. We find that daily variation in meteorology as described by the MLR can explain up to 50% of PM_2.5 variability with temperature, relative humidity (RH), precipitation, and circulation all being important predictors. Temperature is positively correlated with sulfate, organic carbon (OC) and elemental carbon (EC) almost everywhere. The correlation of nitrate with temperature is negative in the Southeast but positive in California and the Great Plains. RH is positively correlated with sulfate and nitrate, but negatively with OC and EC. Precipitation is strongly negatively correlated with all PM_2.5 components. We find that PM_2.5 concentrations are on average 2.6 μg m^?3 higher on stagnant vs. non-stagnant days. Our observed correlations provide a test for chemical transport models used to simulate the sensitivity of PM_2.5 to climate change. They point to the importance of adequately representing the temperature dependence of agricultural, biogenic and wildfire emissions in these models.     

Errors in coarse particulate matter mass concentrations and spatiotemporal characteristics when using subtraction estimation methods

In studies of coarse particulate matter (PM_10-2.5), mass concentrations are often estimated through the subtraction of PM_2.5 from collocated PM₁₀ tapered element oscillating microbalance (TEOM) measurements. Though all field instruments have yet to be updated, the Filter Dynamic Measurement System (FDMS) was introduced to account for the loss of semivolatile material from heated TEOM filters. To assess errors in PM_10-2.5 estimation when using the possible combinations of PM₁₀ and PM_2.5 TEOM units with and without FDMS, data from three monitoring sites of the Colorado Coarse Rural–Urban Sources and Health (CCRUSH) study were used to simulate four possible subtraction methods for estimating PM_10-2.5 mass concentrations. Assuming all mass is accounted for using collocated TEOMs with FDMS, the three other subtraction methods were assessed for biases in absolute mass concentration, temporal variability, spatial correlation, and homogeneity. Results show collocated units without FDMS closely estimate actual PM_10-2.5 mass and spatial characteristics due to the very low semivolatile PM_10-2.5 concentrations in Colorado. Estimation using either a PM_2.5 or PM₁₀ monitor without FDMS introduced absolute biases of 2.4 µg/m³ (25%) to –2.3 µg/m³ (–24%), respectively. Such errors are directly related to the unmeasured semivolatile mass and alter measures of spatiotemporal variability and homogeneity, all of which have implications for the regulatory and epidemiology communities concerned about PM_10-2.5. Two monitoring sites operated by the state of Colorado were considered for inclusion in the CCRUSH acute health effects study, but concentrations were biased due to sampling with an FDMS-equipped PM_2.5 TEOM and PM₁₀ TEOM not corrected for semivolatile mass loss. A regression-based model was developed for removing the error in these measurements by estimating the semivolatile concentration of PM_2.5 from total PM_2.5 concentrations. By estimating nonvolatile PM_2.5 concentrations from this relationship, PM_10-2.5 was calculated as the difference between nonvolatile PM₁₀ and PM_2.5 concentrations.

Implications: Errors in the estimation of PM_10-2.5 concentrations using subtraction methods were shown to be related to the unmeasured semivolatile mass when using certain combinations of TEOM instruments. For the northeastern Colorado region, the absolute bias associated with this error significantly affects mean and 95th percentile values, which would affect assessment of compliance if PM_10-2.5 is regulated in the future. Estimating PM_10-2.5 mass concentrations using nonvolatile mass concentrations from collocated PM₁₀ and PM_2.5 TEOM monitors closely estimates the total PM_10-2.5 mass concentrations. A corrective model that removes the described error was developed and applied to data from two sites in Denver.

Supplemental Materials: Supplemental materials are available for this paper. Go to the publisher's online edition of the Journal of the Air & Waste Management Association.     

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).     

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.