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.     

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.     

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.     

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.     

Characterisation of fresh particulate vehicular exhausts near a Paris high flow road

Simultaneous continuous measurements of PM_2.5, PM₁₀, black carbon mass (BCae), Black smoke (BS) and particle number density (N) were conducted in the close vicinity of a high traffic road around Paris during a three-month period beginning in August 1997. In parallel some aerosol collection was performed on filters in order to assess the black carbon (BC), organic carbon (OC) and water soluble organic fractions (WSOC) of the freshly emitted traffic aerosols. The high hourly concentrations of PM_2.5 (39±20 μg m⁻³), BCae (14±7 μg m⁻³), and N (220,000±115,000 cm⁻³), were found to be well correlated with each other. On average PM_2.5 represented 66±13% of PM₁₀ and appears to be composed primarily of BC (43±20%). On the contrary no correlation was found between PM_2.5 and the coarse (PM₁₀–PM_2.5) mass fractions which was attributed to resuspension processes by vehicles. Black carbon mass concentrations obtained from both filter analyses (BC) and Aethalometre data (BCae) show a good agreement suggesting that the Aethalometre calibration based on a black carbon specific attenuation coefficient (σ) of 19 m² g⁻¹ is well adapted to nearby roadside measurements. Daily BC (used as a surrogate for fine particles) concentrations and wind speed were found to be anti-correlated. Average daily variations of BC could be related to traffic intensity and regime as well as to the boundary layer height. As expected for freshly emitted traffic aerosols, filter analyses indicated a high BC/TC ratio (29±5%) and a low mean WSOC/OC ratio (12.5±5%) for the bulk aerosol. For these two ratios no day/night differences were observed, the sampling station being probably too close to traffic to evidence photochemical modification of the aerosol phase. Finally, a linear relationship was found between BC and BS hourly concentrations (BC=0.10×BS+1.18; r²=0.93) which offers interesting perspectives to retrieve BC concentrations from existing BS archives.     

Spatial variability of carbonaceous aerosols and associated source tracers in two cites in the Midwestern United States

Semi-continuous and 24-h averaged measurements of fine carbonaceous aerosols were made concurrently at three sites within each of two U.S. Midwestern Cities; Detroit, Michigan and Cleveland, Ohio; during two, one-month intensive campaigns conducted in July of 2007 and January & February of 2008. A comparison of 24-h measurements revealed substantial intra-urban variability in carbonaceous aerosols consistent with the influence of local sources, and excesses in both PM_2.5 organic carbon (OC) and elemental carbon (EC) were identified at individual sites within each city. High time-resolved black carbon (BC) measurements indicated that elemental carbon concentrations were higher at sites adjacent to freeways and busy surface streets, and temporal patterns suggested that excess EC at sites adjacent to freeways was dominated by mobile source emissions while excesses in EC away from traffic corridors was dominated by point/area source emissions. The site-to-site variability in OC concentrations was approximately 7% within the neighborhood scale (0.5–4 km) and between 4 and 27% at the urban scale (4–100 km). In contrast, measurements of organic source tracers, in conjunction with a Chemical Mass Balance (CMB) source-apportionment model, indicated that the spatial variation in the contribution of both mobile and stationary sources to PM_2.5 OC often exceeded the variation in OC mass concentration by a factor of 3 or more. Markers for mobile sources, biomass smoke, natural gas, and coal combustion differed by as much as 60% within the neighborhood scale and by greater than 200% within the urban scale. The observations made during this study suggest that the urban excess of carbonaceous aerosols is much more complex than has been previously reported and that a more rigorous, source-oriented approach should be taken in order to assess the risk associated with exposure to carbonaceous aerosols within the industrialized environments of the Midwestern United States.     

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.     

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).     

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.     

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.     

Multi-year hourly PM2.5 carbon measurements in New York: Diurnal,day of week and seasonal patterns

Multi-year hourly measurements of PM_2.5 elemental carbon (EC) and organic carbon (OC) from a site in the South Bronx, New York were used to examine diurnal, day of week and seasonal patterns. The hourly carbon measurements also provided temporally resolved information on sporadic EC spikes observed predominantly in winter. Furthermore, hourly EC and OC data were used to provide information on secondary organic aerosol formation. Average monthly EC concentrations ranged from 0.5 to 1.4 μg m^?3 with peak hourly values of several μg m^?3 typically observed from November to March. Mean EC concentrations were lower on weekends (approximately 27% lower on Saturday and 38% lower on Sunday) than on weekdays (Monday to Friday). The weekday/weekend difference was more pronounced during summer months and less noticeable during winter. Throughout the year EC exhibited a similar diurnal pattern to NO_x showing a pronounced peak during the morning commute period (7–10 AM EST). These patterns suggest that EC was impacted by local mobile emissions and in addition by emissions from space heating sources during winter months. Although EC was highly correlated with black carbon (BC) there was a pronounced seasonal BC/EC gradient with summer BC concentrations approximately a factor of 2 higher than EC. Average monthly OC concentrations ranged from 1.0 to 4.1 μg m^?3 with maximum hourly concentrations of 7–11 μg m^?3 predominantly in summer or winter months. OC concentrations generally correlated with PM_2.5 total mass and aerosol sulfate and with NO_x during winter months. OC showed no particular day of week pattern. The OC diurnal pattern was typically different than EC except in winter when OC tracked EC and NO_x indicating local primary emissions contributed significantly to OC during winter at the urban location. On average secondary organic aerosol was estimated to account for 40–50% of OC during winter and up to 63–73% during summer months.     

Carbonaceous aerosol over a Pinus taeda forest in Central North Carolina,USA

Organic aerosol is the least understood component of ambient fine particulate matter (PM_2.5). In this study, organic and elemental carbon (OC and EC) within ambient PM_2.5 over a three-year period at a forested site in the North Carolina Piedmont are presented. EC exhibited significant weekday/weekend effects and less significant seasonal effects, in contrast to OC, which showed strong seasonal differences and smaller weekend/weekday effects. Summer OC concentrations are about twice as high as winter concentrations, while EC was somewhat higher in the winter. OC was highly correlated with EC during cool periods when both were controlled by primary combustion sources. This correlation decreased with increasing temperature, reflecting higher contributions from secondary organic aerosol, likely of biogenic origin. PM_2.5 radiocarbon data from the site confirms that a large fraction of the carbon in PM_2.5 is indeed of biogenic origin, since modern (non-fossil fuel derived) carbon accounted for 80% of the PM_2.5 carbon over the course of a year. OC and EC exhibited distinct diurnal profiles, with summertime OC peaking in late evening and declining until midday. During winter, OC peaked during the early morning hours and again declined until midday. Summertime EC peaked during late morning hours except on weekends. Wintertime EC often peaked in late PM or early AM hours due to local residential wood combustion emissions. The highest short term peaks in OC and EC were associated with wildfire events. These data corroborate recent source apportionment studies conducted within 20 km of our site, where oxidation products of isoprene, α-pinene, and β-caryophyllene were identified as important precursors to organic aerosols. A large fraction of the carbon in rural southeastern ambient PM_2.5 appears to be of biogenic origin, which is probably difficult to reduce by anthropogenic controls.     

Chemical characterization and source apportionment of fine and coarse particulate matter in Lahore,Pakistan

Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM_2.5 and PM₁₀) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (±one standard deviation) of PM_2.5 was 194 ± 94 μg m^?3 and PM₁₀ was 336 ± 135 μg m^?3. Coarse aerosol (PM_10?2.5) was dominated by crustal sources like dust (74 ± 16%, annual average ± one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 ± 17%). Organic tracer species were used to identify sources of PM_2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 ± 19%). Lesser sources included biomass burning (10 ± 5%) and the combined source of diesel engines and residual fuel oil combustion (6 ± 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 ± 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 ± 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity.     

Characteristics and sources of PM2.5 and carbonaceous species during winter in Taiyuan,China

Continuous observation of PM_2.5 was conducted in Taiyuan, a heavily polluted city in China, during high pollution season from December 2005 to February 2006. The results of this study showed that PM_2.5 and carbonaceous species pollution were serious during winter in Taiyuan. The organic carbon (OC) and element carbon (EC) were accounted for 18.6±11.2% and 2.9±1.6% of PM_2.5, respectively, which indicated that carbonaceous aerosols were key components for control fine particles pollution in Taiyuan. Coal combustion was a dominant source of OC and EC of PM_2.5 in the urban area of Taiyuan during winter. The impact of local and remote particle sources on urban air quality was assessed using PM_2.5 concentration rose and 3-day back trajectories of air masses arriving at Taiyuan. The meteorological conditions were found to affect the ambient concentrations of PM_2.5, OC, EC and OC/EC ratio.     

Evidence for a significant contribution of wood burning aerosols to PM2.5 during the winter season in Paris,France

Although particulate emissions from residential wood burning have become a subject of great scientific concern for a few years, data related to their impact on the air quality of large European urban centres are still missing. In the present study, we investigated the chemical and optical properties of fine (PM_2.5) carbonaceous aerosols in Paris during the 2005 winter season in order to track the presence of wood burning emissions in such a large city. The use of a seven wavelength Aethalometer allowed us to document shortwave light absorption by brown-carbon-containing organic aerosols of biomass burning origin. In particular, a well-marked diurnal pattern of the spectral dependence of light absorption, with maxima during the night, could be observed every day of the campaign and attributed to wood burning emissions. Relatively high absorption Ångstrom exponents and WSOC/OC ratios (respectively 1.25 and 0.35 on average for the period of study) also indicated the importance of biomass burning aerosols in the Paris atmosphere in winter. Finally, a rough estimate of the contribution of wood burning carbonaceous aerosols to PM_2.5 could be achieved. This contribution was found to be as high as 20 ± 10% on average at the Paris background site investigated here.     

Carbon content of atmospheric aerosols in a residential area during the wood combustion season in Sweden

Carbonaceous aerosol particles were observed in a residential area with wood combustion during wintertime in Northern Sweden. Filter samples were analyzed for elemental carbon (EC) and organic carbon (OC) content by using a thermo-optical transmittance method. The light-absorbing carbon (LAC) content was determined by employing a commercial Aethalometer and a custom-built particle soot absorption photometer. Filter samples were used to convert the optical signals to LAC mass concentrations. Additional total PM₁₀ mass concentrations and meteorological parameters were measured. The mean and standard deviation mass concentrations were 4.4±3.6 μg m⁻³ for OC, and 1.4±1.2 μg m⁻³ for EC. On average, EC accounted for 10.7% of the total PM₁₀ and the contribution of OC to the total PM₁₀ was 35.4%. Aethalometer and custom-built PSAP measurements were highly correlated (R²=0.92). The hourly mean value of LAC mass concentration was 1.76 μg m⁻³ (median 0.88 μg m⁻³) for the winter 2005–2006. This study shows that the custom-built PSAP is a reliable alternative for the commercial Aethalometer with the advantage of being a low-cost instrument.     

Physicochemical variations in atmospheric aerosols recorded at sea onboard the Atlantic–Mediterranean 2008 Scholar Ship cruise (Part I): Particle mass concentrations,size ratios,and main chemical components

We report on ambient atmospheric aerosols present at sea during the Atlantic–Mediterranean voyage of Oceanic II (The Scholar Ship) in spring 2008. A record was obtained of hourly PM₁₀, PM_2.5, and PM₁ particle size fraction concentrations and 24-h filter samples for chemical analysis which allowed for comparison between levels of crustal particles, sea spray, total carbon, and secondary inorganic aerosols. On-board monitoring was continuous from the equatorial Atlantic to the Straits of Gibraltar, across the Mediterranean to Istanbul, and back via Lisbon to the English Channel. Initially clean air in the open Atlantic registered PM₁₀ levels <10 μg m^?3 but became progressively polluted by increasingly coarse PM as the ship approached land. Away from major port cities, the main sources of atmospheric contamination identified were dust intrusions from North Africa (NAF), smoke plumes from biomass burning in sub-Saharan Africa and Russia, industrial sulphate clouds and other regional pollution sources transported from Europe, sea spray during rough seas, and plumes emanating from islands. Under dry NAF intrusions PM₁₀ daily mean levels averaged 40–60 μg m^?3 (30–40 μg m^?3 PM_2.5; c. 20 μg m^?3 PM₁), peaking briefly to >120 μg m^?3 (hourly mean) when the ship passed through curtains of higher dust concentrations amassed at the frontal edge of the dust cloud. PM₁/PM₁₀ ratios ranged from very low during desert dust intrusions (0.3–0.4) to very high during anthropogenic pollution plume events (0.8–1).     

Spatial patterns of mobile source particulate matter emissions-to-exposure relationships across the United States

Assessing the public health benefits from air pollution control measures is assisted by understanding the relationship between mobile source emissions and subsequent fine particulate matter (PM_2.5) exposure. Since this relationship varies by location, we characterized its magnitude and geographic distribution using the intake fraction (iF) concept. We considered emissions of primary PM_2.5 as well as particle precursors SO₂ and NO_x from each of 3080 counties in the US. We modeled the relationship between these emissions and total US population exposure to PM_2.5, making use of a source–receptor matrix developed for health risk assessment. For primary PM_2.5, we found a median iF of 1.2 per million, with a range of 0.12–25. Half of the total exposure was reached by a median distance of 150 km from the county where mobile source emissions originated, though this spatial extent varied across counties from within the county borders to 1800 km away. For secondary ammonium sulfate from SO₂ emissions, the median iF was 0.41 per million (range: 0.050–10), versus 0.068 per million for secondary ammonium nitrate from NO_x emissions (range: 0.00092–1.3). The median distance to half of the total exposure was greater for secondary PM_2.5 (450 km for sulfate, 390 km for nitrate). Regression analyses using exhaustive population predictors explained much of the variation in primary PM_2.5 iF (R²=0.83) as well as secondary sulfate and nitrate iF (R²=0.74 and 0.60), with greater near-source contribution for primary than for secondary PM_2.5. We conclude that long-range dispersion models with coarse geographic resolution are appropriate for risk assessments of secondary PM_2.5 or primary PM_2.5 emitted from mobile sources in rural areas, but that more resolved dispersion models are warranted for primary PM_2.5 in urban areas due to the substantial contribution of near-source populations.     

PM composition and source reconciliation in Mexico City

PM_2.5 and PM₁₀ were collected during 24-h sampling intervals from March 1st to 31st, 2006 during the MILAGRO campaign carried out in Mexico City's northern region, in order to determine their chemical composition, oxidative activity and the estimation of the source contributions during the sampling period by means of the chemical mass balance (CMB) receptor model. PM_2.5 concentrations ranged from 32 to 70 μg m⁻³ while that of PM10 did so from 51 to 132 μg m⁻³. The most abundant chemical species for both PM fractions were: OC, EC, SO₄²⁻, NO₃⁻, NH₄⁺, Si, Fe and Ca. The majority of the PM mass was comprised of carbon, up to about 52% and 30% of the PM2.5 and PM10, respectively. PM2.5 constituted more than 50% of PM10. The redox activity, assessed by the dithiothreitol (DTT) assay, was greater for PM_2.5 than for PM₁₀, and did not display significant differences during the sampling period. The PM_2.5 source reconciliation showed that in average, vehicle exhaust emissions were its most important source in an urban site with a 42% contribution, followed by re-suspended dust with 26%, secondary inorganic aerosols with 11%, and industrial emissions and food cooking with 10% each. These results had a good agreement with the Emission Inventory. In average, the greater mass concentration occurred during O₃S that corresponds to a wind shift initially with transport to the South but moving back to the North. Taken together these results show that PM chemical composition, oxidative potential, and source contribution is influenced by the meteorological conditions.     

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.