Receptor modeling of source apportionment of Hong Kong aerosols and the implication of urban and regional contribution

Understanding the spatial–temporal variations of source apportionment of PM_2.5 is critical to the effective control of particulate pollution. In this study, two one-year studies of PM_2.5 composition were conducted at three contrasting sites in Hong Kong from November 2000 to October 2001, and from November 2004 to October 2005, respectively. A receptor model, principal component analysis (PCA) with absolute principal component scores (APCS) technique, was applied to the PM_2.5 data for the identification and quantification of pollution sources at the rural, urban and roadside sites. The receptor modeling results identified that the major sources of PM_2.5 in Hong Kong were vehicular emissions/road erosion, secondary sulfate, residual oil combustion, soil suspension and sea salt regardless of sampling sites and sampling periods. The secondary sulfate aerosols made the most significant contribution to the PM_2.5 composition at the rural (HT) (44 ± 3%, mean ± 1σ standard error) and urban (TW) (28 ± 2%) sites, followed by vehicular emission (20 ± 3% for HT and 23 ± 4% for TW) and residual oil combustion (17 ± 2% for HT and 19 ± 1% for TW). However, at the roadside site (MK), vehicular emissions especially diesel vehicle emissions were the major source of PM_2.5 composition (33 ± 1% for diesel vehicle plus 18 ± 2% for other vehicles), followed by secondary sulfate aerosols (24 ± 1%). We found that the contribution of residual oil combustion at both urban and rural sites was much higher than that at the roadside site (2 ± 0.4%), perhaps due to the marine vessel activities of the container terminal near the urban site and close distance of pathway for the marine vessels to the rural site. The large contribution of secondary sulfate aerosols at all the three sites reflected the wide influence of regional pollution. With regard to the temporal trend, the contributions of vehicular emission and secondary sulfate to PM_2.5 showed higher autumn and winter values and lower summer levels at all the sites, particularly for the background site, suggesting that the seasonal variation of source apportionment in Hong Kong was mainly affected by the synoptic meteorological conditions and the long-range transport. Analysis of annual patterns indicated that the contribution of vehicular emission at the roadside was significantly reduced from 2000/01 to 2004/05 (p < 0.05, two-tail), especially the diesel vehicular emission (p < 0.001, two-tail). This is likely attributed to the implementation of the vehicular emission control programs with the tightening of diesel fuel contents and vehicular emission standards over these years by the Hong Kong government. In contrast, the contribution of secondary sulfate was remarkably increased from 2001 to 2005 (p < 0.001, two-tail), indicating a significant growth in regional sulfate pollution over the years.     

Modelling long-range transport of primary particulate material over Europe

This paper uses a simple model of atmospheric transport and an emissions inventory prepared by TNO to estimate the contribution of primary particulate material to PM₁₀ and PM_2.5 concentration across Europe. The resulting population exposure is compared with that of secondary particulates, and it is noted that both primary and secondary contributions will be significantly reduced with the implementation of new protocols under the Convention on Long-Range Transboundary Air Pollution (CLRTAP). Since concentrations of primary PM₁₀ can become elevated in episodic situations, when long-range transport of particulate could, on its own, exceed 24 h average targets of 50 μg m⁻³ over large areas of Europe, such reduction is important for achievement of current air quality standards to control exposure to atmospheric particulate PM₁₀.     

Developing intake fraction estimates with limited data: Comparison of methods in Mexico City

In order to estimate the health benefits of reducing mobile source emissions, analysts typically use detailed atmospheric models to estimate the change in population exposure that results from a given change in emissions. However, this may not be feasible in settings where data are limited or policy decisions are needed in the short term. Intake fraction (iF), defined as the fraction of emissions of a pollutant or its precursor that is inhaled by the population, is a metric that can be used to compare exposure assessment methods in a health benefits analysis context. To clarify the utility of rapid-assessment methods, we calculate particulate matter iFs for the Mexico City Metropolitan Area using five methods, some more resource intensive than others. First, we create two simple box models to describe dispersion of primary fine particulate matter (PM_2.5) in the Mexico City basin. Second, we extrapolate iFs for primary PM_2.5, ammonium sulfate, and ammonium nitrate from US values using a regression model. Third, we calculate iFs by assuming a linear relationship between emissions and population-weighted concentrations of primary PM_2.5, ammonium nitrate, and ammonium sulfate (a particle composition method). Finally, we estimate PM iFs from detailed atmospheric dispersion and chemistry models run for only a short period of time. Intake fractions vary by up to a factor of five, from 23 to 120 per million for primary PM_2.5. Estimates of 60, 7, and 0.7 per million for primary PM, secondary ammonium sulfate, and secondary ammonium nitrate, respectively, represent credible central estimates, with an approximate factor of two uncertainty surrounding each estimate. Our results emphasize that multiple rapid-assessment methods can provide meaningful estimates of iFs in resource-limited environments, and that formal uncertainty analysis, with special attention to model biases and uncertainty, would be important for health benefits analyses.     

Estimation and characterization of children’s ambient generated exposure to PM2.5 using sulphate and elemental carbon as tracers

Children’s exposures to ambient and non-ambient fine particulate matter (PM_2.5) were determined using the sulphate and elemental carbon components of the PM_2.5 mixture as tracers of the ambient contribution during a 6-week winter period in Prince George, British Columbia, Canada. Personal exposures to PM_2.5 were measured in children at 5 elementary schools located throughout the city and ambient samples were collected on school rooftops. Average ambient levels and personal exposures during this time period were 13.8 μg m^?3 and 16.4 μg m^?3 respectively. From the data pooled across individuals, use of the two different tracers indicated identical estimates of median exposure to ambient PM_2.5 (7.5 μg m^?3) and similar estimates of non-ambient generated exposure (6.4 and 5.0 μg m^?3) and infiltration (0.49 and 0.52) for the sulphate and elemental carbon approach, respectively. The median fraction of the ambient concentration resulting in exposure or exposure factors were 0.54 and 0.55 respectively, however lower values of 0.46 and 0.42 were determined from regression analysis. A strong association was found between exposure to ambient PM_2.5 and measured ambient concentrations at both the closest school monitor (median r = 0.92) and a central site (median r = 0.88) demonstrating that the central site monitor was suitable for assessing longitudinal ambient generated exposure throughout the city. These results support the use of elemental carbon as a tracer of ambient generated exposure and the use of ambient data as estimates of longitudinal changes in children’s exposure in this setting. The importance of both ambient and non-ambient sources of PM_2.5 is emphasized by their almost equal contribution to total personal exposures. Comparison with other studies suggests a limited influence of climate and the cold season in Prince George on exposure levels and found similar mean non-ambient generated exposures despite large variability across and within subjects in any given location.     

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.     

Secondary aerosol formation through photochemical reactions estimated by using air quality monitoring data in Taipei City from 1994 to 2003

Analyses of diurnal patterns of PM₁₀ in Taipei City have been performed in this study at different daily ozone maximum concentrations (O_3,max) from 1994 to 2003. In order to evaluate secondary aerosol formation at different ozone levels, CO was used as a tracer of primary aerosol, and O_3,max was used as an index of photochemical activity. Results show that when O_3,max exceeds 120 ppb, the highest photochemical formation of secondary aerosol can be found at 15:00 (local time). The produced secondary aerosol is estimated to contribute 30 μg m⁻³ (43%) of PM₁₀ concentration, and about 77% of the estimated secondary PM₁₀ is composed of PM_2.5. The estimated maximum concentration of secondary aerosol occurs 2–3 h later than the maximum ozone concentration. As revealed in an O₃ episode, PM₁₀ and PM_2.5 vary consistently with O₃ at daytime, which suggests that they are mostly secondary aerosols produced from photochemical reactions. Data collected from Taipei aerosol supersite in 2002 indicates that for all O₃ levels, summertime PM_2.5 is composed of 23%, 20%, 9%, and 7% of organic carbon, sulfate, nitrate, and elemental carbon, respectively. Aerosol number and volume size spectra are dominated by submicron particles either from pollution transport or photochemical reactions. Secondary PM₁₀ concentrations show increasing tendencies for the time between 15:00 and 19:00 from 1994–1996 to 2001–2003. This reveals that the abatement of secondary PM₁₀ becomes more important after pronounced primary PM₁₀ reduction in a metropolis.     

Behavioral and environmental determinants of personal exposures to PM2.5 in EXPOLIS – Helsinki,Finland

Behavioral and environmental determinants of PM_2.5 personal exposures were analyzed for 201 randomly selected adult participants (25–55 years old) of the EXPOLIS study in Helsinki, Finland. Personal exposure concentrations were higher than respective residential outdoor, residential indoor and workplace indoor concentrations for both smokers and non-smokers. Mean personal exposure concentrations of active smokers (31.0±31.4 μg m⁻³) were almost double those of participants exposed to environmental tobacco smoke (ETS) (16.6±11.8 μg m⁻³) and three times those of participants not exposed to tobacco smoke (9.9±6.2 μg m⁻³). Mean indoor concentrations of PM_2.5 when a member of the household smoked indoors (20.8±23.9 μg m⁻³) were approximately 2.5 times the concentrations of PM_2.5 when no smoking was reported (8.2±5.2 μg m⁻³). Interestingly, however, both mean (8.2 μg m⁻³) and median (6.9 μg m⁻³) residential indoor concentrations for non-ETS exposed participants were lower than residential outdoor concentrations (9.5 and 7.3 μg m⁻³, respectively). In simple linear regression models residential indoor concentrations were the best predictors of personal exposure concentrations. Correlations (r²) between PM_2.5 personal exposure concentrations of all participants, both smoking and non-smoking, and residential indoor, workplace indoor, residential outdoor and ambient fixed site concentrations were 0.53, 0.38, 0.17 and 0.16, respectively. Predictors for personal exposure concentrations of non-ETS exposed participants identified in multiple regression were residential indoor concentrations, workplace concentrations and traffic density in the nearest street from home, which accounted for 77% of the variance. Subsequently, step-wise regression not including residential and workplace indoor concentrations as input (as these are frequently not available), identified ambient PM_2.5 concentration and home location, as predictors of personal exposure, accounting for 47% of the variance. Ambient fixed site PM_2.5 concentrations were closely related to residential outdoor concentrations (r²=0.9, p=0.000) and PM_2.5 personal exposure concentrations were higher in summer than during other seasons. Personal exposure concentrations were significantly (p=0.040) higher for individuals living downtown compared with individuals in suburban family homes. Further analysis will focus on comparisons of determinants between Helsinki and other EXPOLIS centers.     

Characteristics of the major chemical constituents of PM2.5 and smog events in Seoul,Korea in 2003 and 2004

One hundred ninety-five chemically speciated samples were collected from March 2003 to February 2005 in the Seoul Metropolitan area to investigate the characteristics of the major components in PM_2.5 and to characterize the chemical variations between smog and non-smog events. The annual average PM_2.5 concentration was 43 μg m⁻³ that is almost three times higher than the US NAAQS annual PM_2.5 standard of 15 μg m⁻³. During this sampling period, smog and yellow sand events were observed on 27 and 10 days, respectively. The PM_2.5 concentrations and its constituents during smog events were about two–three times higher than those during non-smog and yellow sand events. In particular, the mass fractions of secondary aerosols such as sulfate, nitrate, and ammonium during the smog events were higher than those of the other constituents. The mean concentration and mass fraction of secondary organic carbon (SOC) were highest during the winter smog events. Sulfate, nitrate and SOC that can have long residence times were important species during the smog events suggesting that regional scale sources rather than local sources were important. Five-day backward air trajectory analysis showed that the air parcels during smog events passed through the major industrial areas in China more often than those during non-smog events.     

Levels of outdoor PM2.5, absorbance and sulphur as surrogates for personal exposures among post-myocardial infarction patients in Barcelona,Spain

Outdoor levels of fine particles (PM_2.5; particles <2.5 μm) have been associated with cardiovascular health. Persons with existing cardiovascular disease have been suggested to be especially vulnerable. It is unclear, how well outdoor concentrations of PM_2.5 and its constituents measured at a central site reflect personal exposures in Southern European countries. The objective of the study was to assess the relationship between outdoor and personal concentrations of PM_2.5, absorbance and sulphur among post-myocardial infarction patients in Barcelona, Spain.Thirty-eight subjects carried personal PM_2.5 monitors for 24-h once a month (2–6 repeated measurements) between November 2003 and June 2004. PM_2.5 was measured also at a central outdoor monitoring site. Light absorbance (a proxy for elemental carbon) and sulphur content of filter samples were determined as markers of combustion originating and long-range transported PM_2.5, respectively.There were 110, 162 and 88 measurements of PM_2.5, absorbance and sulphur, respectively. Levels of outdoor PM_2.5 (median 17 μg m³) were lower than personal PM_2.5 even after excluding days with exposure to environmental tobacco smoke (ETS) (median after exclusion 27 μg m³). However, outdoor concentrations of absorbance and sulphur were similar to personal concentrations after exclusion of ETS. When repeated measurements were taken into account, there was a statistically significant association between personal and outdoor absorbance when adjusting for ETS (slope 0.66, p<0.001), but for PM_2.5 the association was weaker (slope 0.51, p=0.066). Adjustment for ETS had little effect on the respective association of S (slope 0.69, p<0.001).Our results suggest that outdoor measurements of absorbance and sulphur can be used to estimate both the daily variation and levels of personal exposures also in Southern European countries, especially when exposure to ETS has been taken into account. For PM_2.5, indoor sources need to be carefully considered.     

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.     

Modeling air quality during the California Regional PM10/PM2.5 Air Quality Study (CPRAQS) using the UCD/CIT source-oriented air quality model – Part III. Regional source apportionment of secondary and total airborne particulate matter

A comprehensive air quality modeling project was carried out to simulate regional source contributions to secondary and total (=primary + secondary) airborne particle concentrations in California's Central Valley. A three-week stagnation episode lasting from December 15, 2000 to January 7, 2001, was chosen for study using the air quality and meteorological data collected during the California Regional PM₁₀/PM_2.5 Air Quality Study (CRPAQS). The UCD/CIT mechanistic air quality model was used with explicit decomposition of the gas phase reaction chemistry to track source contributions to secondary PM. Inert artificial tracers were used with an internal mixture representation to track source contributions to primary PM. Both primary and secondary source apportionment calculations were performed for 15 size fractions ranging from 0.01 to 10 μm particle diameters. Primary and secondary source contributions were resolved for fugitive dust, road dust, diesel engines, catalyst equipped gasoline engines, non-catalyst equipped gasoline engines, wood burning, food cooking, high sulfur fuel combustion, and other anthropogenic sources.Diesel engines were identified as the largest source of secondary nitrate in central California during the study episode, accounting for approximately 40% of the total PM_2.5 nitrate. Catalyst equipped gasoline engines were also significant, contributing approximately 20% of the total secondary PM_2.5 nitrate. Agricultural sources were the dominant source of secondary ammonium ion. Sharp gradients of PM concentrations were predicted around major urban areas. The relative source contributions to PM_2.5 from each source category in urban areas differ from those in rural areas, due to the dominance of primary OC in urban locations and secondary nitrate in the rural areas. The source contributions to ultra-fine particle mass PM_0.1 also show clear urban/rural differences. Wood smoke was found to be the major source of PM_0.1 in urban areas while motor vehicle sources were the major contributor of PM_0.1 in rural areas, reflecting the influence from two major highways that transect the Valley.     

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.     

A wintertime PM2.5 episode at the Fresno,CA, supersite

A winter PM_2.5 episode that achieved a maximum 24-h average of 138 μg m⁻³ at the Fresno Supersite in California's San Joaquin Valley between 2 and 12 January, 2000 is examined using 5-min to 1-h continuous measurements of mass, nitrate, black carbon, particle-bound PAH, and meteorological measurements. Every day PM_2.5 sampling showed that many episodes, including this one, are missed by commonly applied sixth-day monitoring, even though quarterly averages and numbers of US air quality standard exceedances are adequately estimated. Simultaneous measurements at satellite sites show that the Fresno Supersite represented PM_2.5 within the city, and that half or more of the urban concentrations were present at distant, non-urban locations unaffected by local sources. Most of the primary particles accumulated during early morning and nighttime, decreasing when surface temperatures increased and the shallow radiation inversion coupled to a valleywide layer. When this coupling occurred, nitrate levels increased rapidly over a 10–30 min period as black carbon and gaseous concentrations dropped. This is consistent with a conceptual model in which secondary aerosol forms above the surface layer and is effectively decoupled from the surface for all but the late-morning and early afternoon period. Primary pollutants, such as organic and black carbon, accumulate within the shallow surface layer in urban areas where wood burning and vehicle exhaust emissions are high. Such a model would explain why earlier studies find nitrate concentrations to be nearly the same among widely separated sites in urban areas, as winds aloft of 1 to 6 m s⁻¹ could easily disperse the elevated aerosol throughout the valley.     

Airborne particle PM2.5/PM10 mass distribution and particle-bound PAH concentrations near a medical waste incinerator

This study attempts to determine the influence of air quality in a residential area near a medical waste incineration plant. Ambient air concentrations of polycyclic aromatic hydrocarbons (PAHs), PM₁₀ and PM_2.5 (PM—particulate matter) were determined by collecting air samples in areas both upwind and downwind of the plant. The differences in air pollutant levels between the study area and a reference area 11 km away from the plant were evaluated.Dichotomous samplers were used for sampling PM_2.5 and PM₁₀ from ambient air. Two hundred and twenty samples were obtained from the study area, and 100 samples were taken from a reference area. Samples were weighed by an electronic microbalance and concentrations of PM_2.5 and PM₁₀ were determined. A HPLC equipped with a fluorescence detector was employed to analyze the concentrations of 15 PAHs compounds adsorbed into PM_2.5 and PM₁₀.The experimental results indicated that the average concentrations of PM_2.5 and PM₁₀ were 30.34±17.95 and 36.81±20.45 μg m⁻³, respectively, in the study area, while the average ratio of PM_2.5/PM₁₀ was 0.82±0.01. The concentrations of PM_2.5 and PM₁₀ of the study area located downwind of the incinerator were significantly higher than the study area upwind of the incinerator (P<0.05).The concentration of PAHs in PM_2.5 in the study area was 2.2 times higher than in the reference area (P<0.05). Furthermore, the benzo(a)pyrene concentrations in PM_2.5 and PM₁₀ were 0.11±0.05 ng m⁻³ and 0.12±0.06 ng m⁻³ in the study area, respectively. The benzo(a)pyrene concentrations of PM_2.5 and PM₁₀ in the study area were 7 and 5.3 times higher than in the reference area (P<0.05), respectively.The study indicated that the air quality of PM_2.5, PM₁₀ and PAHs had significant contamination by air pollutants emitted from a medical waste incineration factory, representing a public health problem for nearby residences, despite the factory being equipped with a modern air pollution control system.     

Particulate matter and manganese exposures in Toronto,Canada

Methylcyclopentadienyl manganese tricarbonyl (MMT) is a manganese-based gasoline additive used to enhance automobile performance. MMT has been used in Canadian gasoline for about 20 yr. Because of the potential for increased levels of Mn in particulate matter resulting from automotive exhausts, a large-scale population-based exposure study (∼1000 participant periods) was conducted in Toronto, Canada, to estimate the distribution of 3-day average personal exposures to particulate matter (PM_2.5 and PM₁₀) and Mn. A stratified, three-stage, two-phase probability, longitudinal sample design of the metropolitan population was employed. Residential indoor and outdoor, and ambient levels (at a fixed site and on a roof) of PM_2.5, PM₁₀, and Mn were also measured. Supplementary data on traffic counts, meteorology, MMT levels in gasoline, personal occupations, and activities (e.g. amount of vehicular usage) were collected. Overall precision (%RSD) for analysis of duplicate co-located samples ranged from 2.5 to 5.0% for particulate matter and 3.1 to 5.5% for Mn. The detection limits were 1.47 and 3.45 μg m^-3 for the PM₁₀ and PM_2.5 fractions, respectively, and 5.50 and 1.83 ng m^-3 for Mn in PM₁₀ and PM_2.5, respectively. These low detection limits permitted the reporting of concentrations for >98% of the samples. For PM₁₀, the personal particulate matter levels (median 48.5 μg m^-3) were much higher than either indoor (23.1 μg m^-3) or outdoor levels (23.6 μg m^-3). The median levels for PM_2.5 for personal, indoor, and outdoor were 28.4, 15.4 and 13.2 μg m^-3, respectively. The correlation between PM_2.5 personal exposures and indoor concentrations was high (0.79), while correlations between personal and the outdoor, fixed site and roof site were low (0.16–0.27). Indoor Mn concentration distributions (in PM_2.5 and PM₁₀), unlike particulate matter, exhibited much lower and less variable levels that the corresponding outdoor data. The median personal exposure was 8.0 ng m^-3, compared with 4.7 and 8.6 ng m^-3, respectively, for the indoor and outdoor distributions. The highest correlations occurred for personal vs indoor data (0.56) and for outdoor vs roof site data (0.66), and vs fixed site data (0.56). The concentration of Mn in particulate matter, expressed in ppm (w/w), revealed that the fixed site was the highest, followed by the roof site, outdoor, indoor, and personal. The personal and indoor data showed a statistically significant correlation (0.68) while all other correlations between personal or indoor data and outdoor or fixed-site data were quite small. The low correlations of personal and indoor levels with outdoor levels suggest that different sources in the indoor and outdoor microenvironments produce particle matter with dissimilar composition. The correlation results indicate that neither the roof- nor fixed-site concentrations can adequately predict personal particulate matter or Mn exposures.     

Spatial representativeness and scales of transport during the 1995 integrated monitoring study in California's San Joaquin Valley

Daily measurements of PM₁₀ mass and chemical composition were obtained for the period 1–14 November 1995 from a saturation monitoring network around Corcoran, and for varying portions of the period 9 December 1995–6 January 1996 for three networks around Bakersfield, Fresno, and the Kern Wildlife Refuge, in California's San Joaquin Valley. During the latter period, monitoring locations were also operated along the boundaries and across the width of the Valley. The Corcoran, Bakersfield, and Fresno networks consisted of 12–25 sites, located in areas of about 300–800 km². Each network also included one core site, situated at a pre-existing monitoring location, with more extensive and more temporally resolved measurements. Mean concentrations of PM₁₀ and its constituents varied from core-site concentrations by 20% or more over distances ranging from 4 to 14 km. Local source influences were observed to affect sites over distances of less than 1 km, but primary particulate emissions were also transported over urban or sub-regional scales of approximately 10–30 km during the winter and greater than 30 km in the fall. During winter, gas-phase precursors of secondary aerosol may have been transported over distances of approximately 100 km, but little evidence was found for transport of primary PM on such a scale.     

PM10 measurements at McMurdo Station,Antarctica

PM₁₀ aerosols at McMurdo Station, Antarctica were sampled continuously during the austral summers of 1995–1996 and 1996–1997. PM₁₀ (particles with aerodynamic diameters less than 10 μm) mass concentrations at Hut Point, located less than 1 km from downtown McMurdo, averaged 3.4 μg m⁻³, more than an order of magnitude lower than the USEPA annual average National Ambient Air Quality Standard (NAAQS) of 50 μg m⁻³. Concentrations of methanesulfonate and nitrate were similar to those measured at other Antarctic coastal sites. Non-sea-salt sulfate (NSS) concentrations on Ross Island were higher than those found at other coastal locations. The average elemental carbon concentration (129 ng m⁻³) downwind of the station was two orders of magnitude higher than those measured at remote coastal and inland Antarctic sites during summer. Average sulfur dioxide concentrations (746 ng m⁻³) were 3–44 times higher than those reported for coastal Antarctica. Concentrations of Pb and Zn were 17 and 46 times higher than those reported for the South Pole. A methanesulfonate to biogenic sulfate ratio (R) of 0.47 was derived that is consistent with the proposed temperature dependence of R.     

Field performance of dichotomous sequential PM air samplers

For over one year, the Environmental Protection Commission of Hillsborough County (EPCHC) in Tampa, Florida, operated two dichotomous sequential particulate matter air samplers collocated with a manual Federal Reference Method (FRM) air sampler at a waterfront site on Tampa Bay. The FRM was alternately configured as a PM_2.5, then as a PM₁₀ sampler. For the dichotomous sampler measurements, daily 24-h integrated PM_2.5 and PM_10–2.5 ambient air samples were collected at a total flow rate of 16.7 l min⁻¹. A virtual impactor split the air into flow rates of 1.67 and 15.0 l min⁻¹ onto PM_10–2.5 and PM_2.5 47-mm diameter PTFE^® filters, respectively. Between the two dichotomous air samplers, the average concentration, relative bias and relative precision were 13.3 μg m⁻³, 0.02% and 5.2% for PM_2.5 concentrations (n=282), and 12.3 μg m⁻³, 3.9% and 7.7% for PM_10–2.5 concentrations (n=282). FRM measurements were alternate day 24-h integrated PM_2.5 or PM₁₀ ambient air samples collected onto 47-mm diameter PTFE^® filters at a flow rate of 16.7 l min⁻¹. Between a dichotomous and a PM_2.5 FRM air sampler, the average concentration, relative bias and relative precision were 12.4 μg m⁻³, −5.6% and 8.2% (n=43); and between a dichotomous and a PM₁₀ FRM air sampler, the average concentration, relative bias and relative precision were 25.7 μg m⁻³, −4.0% and 5.8% (n=102). The PM_2.5 concentration measurement standard errors were 0.95, 0.79 and 1.02 μg m⁻³; for PM₁₀ the standard errors were 1.06, 1.59, and 1.70 μg m⁻³ for two dichotomous and one FRM samplers, respectively, which indicate the dichotomous samplers have superior technical merit. These results reveal the potential for the dichotomous sequential air sampler to replace the combination of the PM_2.5 and PM₁₀ FRM air samplers, offering the capability of making simultaneous, self-consistent determinations of these particulate matter fractions in a routine ambient monitoring mode.     

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).     

Seasonal and shorter-term variations in particulate atmospheric nitrate in Baltimore

Fine particle nitrate concentrations were measured at 10-min intervals for approximately 9.5 months beginning on 14 February 2002, at the Baltimore Supersite Ponca St. location using an R&P 8400N semi-continuous monitor. The measurement results were used to characterize seasonal and shorter-term excursions in nitrate concentrations and determine their influence on PM_2.5 concentrations. Over the 9.5-month study period, nitrate levels of 1.7±1.6 μg m⁻³ accounted for 11.4% of the PM_2.5 mass. Monthly averages ranged from 0.8 μg m⁻³ in August to 2.9 μg m⁻³ in November, and accounted for 4.7–17.3% of monthly PM_2.5 mass. Hourly averages, however, were often larger, especially in the colder months, owing to numerous relatively short-term transients, where hourly nitrate concentrations exceeded 5.0 μg m⁻³. These often occurred along with NO_x and ultrafine particle transients during the morning commute hours.A total of 275 short-term transients (31.7% of the total) exceeding 1.0 μg m⁻³ were identified. These were associated with one of three sets of conditions. The first, most typical (177, i.e. 64.4% of the 275 incidences), is characterized by high NO_x typically between 0500 and 0800EST and is attributed to early morning commute traffic activity. The second type occurred during the afternoon due to photochemical activity. The excursions in the afternoon occurred infrequently (only 9.5% of all the observed transients) during the study period and were characterized by less elevated nitrate concentrations than morning and nighttime transients. The third (72, i.e. 26.2% of the 275 transients) occurred at night, typically between 2000EST and 0200EST.Multiple linear regression analysis between nitrate excursions and volume size distributions indicates that particulate nitrate observed is closely related to the near accumulation (0.1–0.2 μm) and droplet modes (0.5–1.0 μm) in the morning hours, and associated with the droplet (0.5–1.0 μm) and coarse modes (1.0–2.5 μm) for nighttime transients, suggesting that processes governing particulate nitrate formation depend on time-of-day.