Personal exposure to particulate air pollution in transport microenvironments

Personal measurements of exposure to particulate air pollution (PM₁₀, PM_2.5, PM₁) were simultaneously made during walking and in-car journeys on two suburban routes in Northampton, UK, during the winter of 1999/2000. Comparisons were made between concentrations found in each transport mode by particle fraction, between different particle fractions by transport mode, and between transport microenvironments and a fixed-site monitor located within the study area. High levels of correlation were seen between walking and in-car concentrations for each of the particle fractions (PM₁₀: r²=0.82; PM_2.5: r²=0.98; PM₁: r²=0.99). On an average, PM₁₀ concentrations were 16% higher inside the car than for the walker, but there were no difference in average PM_2.5 and PM₁ concentrations between the two modes. High PM_2.5:PM₁₀ ratios (0.6–0.73) were found to be associated with elevated sulphate levels. The PM_2.5:PM₁₀ and PM₁:PM_2.5 ratios were shown to be similar between walking and in-car concentrations. Concentrations of PM₁₀ were found to be more closely related between transport mode than either mode was with concentrations recorded at the fixed-site (roadside) monitor. The fixed-site monitor was shown to be a poor marker for PM₁₀ concentrations recorded during walking and in-car on a route over 1 km away.     

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.     

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.     

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.     

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.     

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.     

Study of aluminium distribution and speciation in atmospheric particles of different diameters in Nanjing,China

Aluminium (Al) is one of the trace inorganic metals present in atmospheric particles. Al speciation study is essential to better evaluate the mobility, availability, and persistence of trace Al and Al species in the atmosphere. This paper reports Al distribution and speciation in atmospheric particles with aerodynamic diameters >10.0, 10.0–2.5 and <2.5 μm in the urban area of Nanjing, China. Urban particles were collected with a high-volume sampling system equipped with a cascade impactor, which effectively separates the particulate matter into three size ranges. Particulate Al was fractionated into five different forms (insoluble, oxide, organic, carbonate, and exchangeable species) by the modified five-step Tessier's sequential extraction procedure. The main points are as follows: (1) The average levels of Al in PM_2.5, PM_2.5–10 and PM_>10 are 2.02±0.35, 3.04±0.43 and 6.32±0.76 μg m⁻³, respectively, with PM_2.5, PM_2.5–10 and PM_>10 constituting respectively, 17.8±3.1%, 26.7±3.8% and 55.5±6.7% of suspended particulate matter (SPM) mass (11.38 μg m⁻³). (2) The vertical profile of airborne Al in the above three size fractions has been estimated. A significant increase in airborne Al concentrations was found for PM_2.5, PM_2.5–10 and PM_>10 as the sampling height above the ground increased from 2.5 to 17.5 m; however, there was an obvious decrease in airborne Al concentrations between 17.5 and 40.0 m. The maximum mean of total Al in PM_2.5, PM_2.5–10 and PM_>10 occurred between 12.5 and 20.0 m above the ground. (3) The distribution of Al speciation was studied. It was found that the size distribution of airborne Al species followed the order: insoluble species>oxide species>organic species>carbonate species>exchangeable species.     

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.     

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.     

Spatial and temporal variability in outdoor,indoor, and personal PM2.5 exposure

Outdoor, indoor and personal PM_2.5 measurements were made in a population of nonsmoking adults from three communities in the Minneapolis–St. Paul metropolitan area between April and November 1999. Thirty-two healthy adult subjects (23 females, 9 males; mean age 42±10, range: 24–64 yr) were monitored for 2–15 days during the spring, summer, and fall monitoring seasons. Twenty-four hour average gravimetric PM_2.5 samples were collected using a federal reference monitor (Anderson RAAS2.5-300) located at outdoor (O) central sites in the Battle Creek (BCK), East St. Paul (ESP) and Phillips (PHI) communities. Concurrent 24-h average indoor (I) and personal (P), and a limited number of outdoor-at-home (O@H) samples were collected using inertial impactors (PEM™ Model 200, MSP, Inc). The O (geometric mean {GM}=8.6; n=271; range: 1.0–41 μg/m³) were lower than I concentrations (GM=10.7; n=294; range 1.3–131 μg/m³), which were lower than P concentrations (GM=19.0; n=332; range 2.2–298 μg/m³). Correlation coefficients between O concentrations in the three communities were high and measured GM O levels in BCK were significantly lower than ESP, most likely because of local sources, but GM concentrations in PHI were not significantly different from BCK or ESP. On days with paired samples (n=29), O concentrations were significantly lower (mean difference 2.9 μg/m³; p=0.026) than O@H measurements (GM=11.3; range: 3.5–33.8 μg/m³), likely due to local sources in communities. Observed I and P concentrations were more variable, probably because of residential central air conditioning and hours of household ventilation for I and P, and occupational and environmental tobacco smoke exposures outside the residence for P. Across all individuals and days the median PM_2.5 “personal cloud” was 5.7 μg/m³, but the mean of the average for each participant was 15.7 μg/m³, with very low values in participants who did not work outside the home and much higher values in subjects with active lifestyles. Across all households and individuals the correlation between P and O concentrations was not significant, but the overall I–O correlation (0.27) and P–I correlation (0.51) were significant (p<0.05). Relatively little spatial variability was observed in O PM_2.5 concentrations across the three communities compared to the variability associated with I and P samples, and the measured O levels were relatively low compared to other large metropolitan areas in the United States.     

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

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

Validity of Ambient Levels of Fine Particles as Surrogate for Personal Exposure to Outdoor Air Pollution—Results of the European EXPOLIS-EAS Study (Swiss Center Basel)

ABSTRACT

To evaluate the validity of fixed-site fine particle levels as exposure surrogates in air pollution epidemiology, we considered four indicator groups: (1) PM₂₅ total mass concentrations, (2) sulfur and potassium for regional air pollution, (3) lead and bromine for traffic-related particles, and (4) calcium for crustal particles. Using data from the European EXPOLIS (Air Pollution Exposure Distribution within Adult Urban Populations in Europe) study, we assessed the associations between 48-hr personal exposures and home outdoor levels of the indicators. Furthermore, within-city variability of fine particle levels was evaluated.

Personal exposures to PM_2.5 mass were not correlated to corresponding home outdoor levels (n = 44, r_{S (S)} =r o v ' Spearman (Sp) 0.07). In the group reporting neither relevant indoor sources nor relevant activities, personal exposures and home outdoor levels of sulfur were highly correlated (n = 40, r_Sp = 0.85). In contrast, the associations were weaker for traffic (Pb: n = 44, r_Sp = 0.53; Br: n = 44, r_Sp = 0.21) and crustal (Ca: n = 44, r_Sp = 0.12) indicators. This contrast is consistent with spatially homogeneous regional pollution and higher spatial variability of traffic and crustal indicators observed in Basel, Switzerland.

We conclude that for regional air pollution, fixed-site fine particle levels are valid exposure surrogates. For source-specific exposures, however, fixed-site data are probably not the optimal measure. Still, in air pollution epidemiology, ambient PM_2.5 levels may be more appropriate exposure estimates than total personal PM_2.5 exposure, since the latter reflects a mixture of indoor and outdoor sources.     

PM2.5–10, PM2.5 and associated water-soluble inorganic species at a coastal urban site in the metropolitan region of Rio de Janeiro

The concentrations of PM_2.5−10, PM_2.5 and associated water-soluble inorganic species (WSIS) were determined in a coastal site of the metropolitan region of Rio de Janeiro, Southeastern Brazil, from October 1998 to September 1999 (n=50). Samples were dissolved in water and analyzed for major inorganic ions. The mean (± standard deviation; median) concentrations of PM_2.5−10 and PM_2.5 were, respectively, 26 (± 16; 21) μg m⁻³ and 17 (± 13; 14) μg m⁻³. Their mean concentrations were 1.7–1.8 times higher in dry season (May–October) than in rainy season (November–April). The WSIS comprised, respectively, 34% and 28% of the PM_2.5−10 and PM_2.5 masses. Chloride, Na⁺ and Mg²⁺ were the predominant ions in PM_2.5−10, indicating a significant influence of sea-salt aerosols. In PM_2.5, SO₄²⁻ (∼97% nss-SO₄²⁻) and NH₄⁺ were the most abundant ions and their equivalent concentration ratio (SO₄²⁻/NH₄⁺ ∼1.0) suggests that they were present as (NH₄)₂SO₄ particles. The mean concentration of (NH₄)₂SO₄ was 3.4 μg m⁻³. The mean equivalent PM_2.5 NO₃⁻ concentration was eight times smaller than those of SO₄²⁻ and NH₄⁺. The PM_2.5 NO₃⁻ concentration in dry season was three times higher than in rainy season, probably due to reaction of NaCl (sea salt) with HNO₃ as a result of higher levels of NO_y during the dry season and/or reduced volatilization of NH₄NO₃ due to lower wintertime temperature. Chloride depletion was observed in both size ranges, although more pronouncely in PM_2.5.     

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.     

Measurements of the physical properties of particles in the urban atmosphere

Measurements of the physical properties of particles in the atmosphere of a UK urban area have been made, including particle number count by condensation nucleus counters with different lower particle size cut-offs; particle size distributions using a Scanning Mobility Particle Sizer; total particle Fuchs surface area using an epiphaniometer and particle mass using Tapered Element Oscillating Micro-balance (TEOM) instruments with size selective (PM₁₀ and PM_2.5) inlets. Mean particle number counts at three sites range from 2.86×10⁴ to 9.60×10⁴ cm^-3. A traffic-influenced location showed a substantially higher ratio of particle number to PM₁₀ mass than a nearby background location despite being some 70 m from the roadway. Operating two condensation nucleus counters in tandem to determine particles in the 3–7 nm size range by difference showed signficant numbers of particles in this range, apparently related to homogeneous nucleation processes. Measurements with the Scanning Mobility Particle Sizer showed a clear difference between roadside size distributions and those at a nearby background location with an additional mode in the roadside samples below 10 nm diameter. Particle number counts were found to show a significant linear correlation with PM₁₀ mass (r²=0.44; n=44 for 24 h data at an urban background location), although during one period of high pollution a curvilinear relationship was found. Measurements of the diurnal variation in PM₁₀ mass, particle number count and Fuchs surface area show the same general pattern of behaviour of the three variables, explicable in terms of vehicle emission source strength and atmospheric dispersion, although the surface area growth was out of phase with the particle number and mass. It appears that particle number gives the clearest indication of recent road traffic emissions.     

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.     

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.     

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.     

Assessment of road users’ elemental carbon personal exposure levels,London, UK

Little is known about particulate elemental carbon (EC) personal exposure levels, a key component of diesel exhaust, specifically in transport microenvironments. A method utilizing the optical properties of EC particles has been applied to personal exposure measurement filter samples. In a series of field studies carried out in London, UK, during 1999–2000 over 400 fine particle (PM_2.5) personal exposure level measurements were taken for journeys in bicycle, bus, car and underground rail transport microenvironments, along three main fixed routes. The particulate EC contribution to the PM_2.5 personal exposure was assessed indirectly by means of an optical technique and with the development and use of a size fraction specific and site-specific calibration curve. In this first EC personal exposure study of transport users geometric mean exposure levels in the summer field campaign were 11.2 μg m⁻³ (GSD=2.7) for cyclists, 13.6 μg m⁻³ (GSD=1.9) for bus passengers and 21.6 μg m⁻³ (GSD=2.1) for car drivers; corresponding exposure levels in the winter were 16.4 μg m⁻³ (GSD=1.8), 18.6 μg m⁻³ (GSD=2.3) and 27.3 μg m⁻³ (GSD=2.0), respectively. EC/PM_2.5 ratios were approximately 0.5–0.6 for bicycle and bus modes and 0.7–0.8 for the car mode. EC/PM_2.5 ratios for different routes ranged from approximately 0.7 for Route 1 to 0.4 for Route 3. Cyclists had the lowest exposure to EC, and car occupants the highest exposure. A large difference in exposure levels between a central high traffic density route and the other less central routes was observed. Particulate EC was a very significant proportion of the total PM_2.5 personal exposure and EC personal exposure levels were considerably higher than reported fixed site monitor EC concentrations.     

Source-to-receptor pathways of anthropogenic PM2.5 in Detroit,Michigan: Comparison of two inhalation exposure studies

Recent studies have attributed toxic effects of ambient fine particulate matter (aerodynamic diameter ≤ 2.5 μm; PM_2.5) to physical and/or chemical properties rather than total mass. However, identifying specific components or sources of a complex mixture of ambient PM_2.5 that are responsible for adverse health effects is still challenging. In order to improve our understanding of source-to-receptor pathways for ambient PM_2.5 (links between sources of ambient PM_2.5 and measures of biologically relevant dose), integrated inhalation toxicology studies using animal models and concentrated air particles (CAPs) were completed in southwest Detroit, a community where the pediatric asthma rate is more than twice the national average. Ambient PM_2.5 was concentrated with a Harvard fine particle concentrator housed in AirCARE1, a mobile air research laboratory which facilitates inhalation exposure studies in real-world settings. Detailed characterizations of ambient PM_2.5 and CAPs, identification of major emission sources of PM_2.5, and quantification of trace elements in the lung tissues of laboratory rats that were exposed to CAPs for two distinct 3-day exposure periods were completed.This paper describes the physical/chemical properties and sources of PM_2.5, pulmonary metal concentrations and meteorology from two different 3-day exposure periods—both conducted at the southwest Detroit location in July 2003—which resulted in disparate biological effects. More specifically, during one of the exposure periods, ambient PM_2.5-derived trace metals were recovered from lung tissues of CAPs-exposed animals, and these metals were linked to local combustion point sources in southwest Detroit via receptor modeling and meteorology; whereas in the other exposure period, no such trace metals were observed. By comparing these two disparate results, this investigation was able to define possible links between PM_2.5 emitted from refineries and incinerators and biologically relevant dose, which in turn may be associated with observed health effects.