Assessing the relationship between personal particulate and gaseous exposures of senior citizens living in Baltimore, MD

We conducted a multi-pollutant exposure study in Baltimore, MD, in which 15 non-smoking older adult subjects (> 64 years old) wore a multi-pollutant sampler for 12 days during the summer of 1998 and the winter of 1999. The sampler measured simultaneous 24-hr integrated personal exposures to PM2.5, PM10, SO4(2-), O3, NO2, SO2, and exhaust-related VOCs. Results of this study showed that longitudinal associations between ambient PM2.5 concentrations and corresponding personal exposures tended to be high in the summer (median Spearman's r = 0.74) and low in the winter (median Spearman's r = 0.25). Indoor ventilation was an important determinant of personal PM2.5 exposures and resulting personal-ambient associations. Associations between personal PM2.5 exposures and corresponding ambient concentrations were strongest for well-ventilated indoor environments and decreased with ventilation. This decrease was attributed to the increasing influence of indoor PM2.5 sources. Evidence for this was provided by SO4(2-) measurements, which can be thought of as a tracer for ambient PM2.5. For SO4(2-), personal-ambient associations were strong even in poorly ventilated indoor environments, suggesting that personal exposures to PM2.5 of ambient origin are strongly associated with corresponding ambient concentrations. The results also indicated that the contribution of indoor PM2.5 sources to personal PM2.5 exposures was lowest when individuals spent the majority of their time in well-ventilated indoor environments. Results also indicate that the potential for confounding by PM2.5 co-pollutants is limited, despite significant correlations among ambient pollutant concentrations. In contrast to ambient concentrations, PM2.5 exposures were not significantly correlated with personal exposures to PM2.5-10, PM2.5 of non-ambient origin, O3, NO2, and SO2. Since a confounder must be associated with the exposure of interest, these results provide evidence that the effects observed in the PM2.5 epidemiologic studies are unlikely to be due to confounding by the PM2.5 co-pollutants measured in this study.     

Estimated hourly personal exposures to ambient and nonambient particulate matter among sensitive populations in Seattle, Washington

Epidemiological studies of particulate matter (PM) routinely use concentrations measured with stationary outdoor monitors as surrogates for personal exposure. Despite the frequently reported poor correlations between ambient concentrations and total personal exposure, the epidemiologic associations between ambient concentrations and health effects depend on the correlation between ambient concentrations and personal exposure to ambient-generated PM. This paper separates personal PM exposure into ambient and nonambient components and estimates the outdoor contribution to personal PM exposures with continuous light scattering data collected from 38 subjects in Seattle, WA. Across all subjects, the average exposure encountered indoors at home was lower than in all other microenvironments. Cooking and being at school were associated with elevated levels of exposure. Previously published estimates of particle infiltration (Finf) were combined with time-location data to estimate an ambient contribution fraction (alpha, mean = 0.66+/-0.21) for each subject. The mean alpha was significantly lower for subjects monitored during the heating season (0.55+/-0.16) than for those monitored during the nonheating season (0.80+/-0.17). Our modeled alpha estimates agreed well with those estimated with the sulfur-tracer method (slope = 1.08; R2 = 0.67). We modeled exposure to ambient and nonambient PM with both continuous light scattering and 24-hr gravimetric data and found good agreement between the two methods. On average, ambient particles accounted for 48% of total personal exposure (range = 21-80%). The personal activity exposure was highly influenced by time spent away from monitored microenvironments. The median hourly longitudinal correlation between central site concentrations and personal exposures was 0.30. Although both alpha and the nonambient sources influence the personal-central relationship, the latter seems to dominate. Thus, total personal exposure may be poorly predicted by stationary outdoor monitors, particularly among persons whose PM exposure is dominated by nonambient exposures, for example, those living in tightly sealed homes, those who cook, and children.     

Roadside particulate air pollution in Bangkok

Airborne fine particles of PM(2.5-10) and PM2.5 in Bangkok, Nonthaburi, and Ayutthaya were measured from December 22, 1998, to March 26, 1999, and from November 30, 1999, to December 2, 1999. Almost all the PM10 values in the high-polluted (H) area exceeded the Thailand National Ambient Air Quality Standards (NAAQS) of 120 microg/m3. The low-polluted (L) area showed low PM10 (34-74 microg/m3 in the daytime and 54-89 microg/m3 at night). PM2.5 in the H area varied between 82 and 143 microg/m3 in the daytime and between 45 and 146 microg/m3 at night. In the L area, PM2.5 was quite low both day and night and varied between 24 and 54 microg/m3, lower than the U.S. Environmental Protection Agency (EPA) standard (65 microg/m3). The personal exposure results showed a significantly higher proportion of PM2.5 to PM10 in the H area than in the L area (H = 0.80 +/- 0.08 and L = 0.65 +/- 0.04). Roadside PM10 was measured simultaneously with the Thailand Pollution Control Department (PCD) monitoring station at the same site and at the intersections where police work. The result from dual simultaneous measurements of PM10 showed a good correlation (correlation coefficient: r = 0.93); however, PM levels near the roadside at the intersections were higher than the concentrations at the monitoring station. The relationship between ambient PM level and actual personal exposures was examined. Correlation coefficients between the general ambient outdoors and personal exposure levels were 0.92 for both PM2.5 and PM10. Bangkok air quality data for 1997-2000, including 24-hr average PM10, NO2, SO2, and O3 from eight PCD monitoring stations, were analyzed and validated. The annual arithmetic mean PM10 of the PCD data at the roadside monitoring stations for the last 3 years decreased from 130 to 73 microg/m3, whereas the corresponding levels at the general monitoring stations decreased from 90 to 49 microg/m3. The proportion of days when the level of the 24-hr average PM10 exceeded the NAAQS was between 13 and 26% at roadside stations. PCD data showed PM10 was well correlated with NO2 but not with SO2, suggesting that automobile exhaust is the main source of the particulate air pollution. The results obtained from the simultaneous measurement of PM2.5 and PM10 indicate the potential environmental health hazard of fine particles. In conclusion, Bangkok traffic police were exposed to high levels of automobile-derived particulate air pollution.     

Personal exposures to particles and their relationships with personal activities for chronic obstructive pulmonary disease patients living in Boston

An exposure study of 18 subjects with chronic obstructive pulmonary disease (COPD) living in the Boston, MA, area was conducted. The objective was to examine determinants of personal exposures to particulate matter (PM) with aerodynamic diameters of less than 2.5 microm (PM2.5), less than 10 microm (PM10), and between 2.5 and 10 microm (PM2.5-10). In a previous publication, the analyses of the longitudinal individual-specific relationships among indoor, outdoor, and personal levels showed that the relationships varied by subject and by particle size fraction. In the present paper, statistical and physical models were used to examine personal PM2.5, PM10, and PM2.5-10 exposure covariates. Results indicated that time-weighted indoor concentrations were significant predictors of personal PM2.5, PM10, and PM2.5-10 exposures. Also, time-weighted outdoor concentrations, time spent near smokers, and time spent during transportation were important predictors for PM2.5 but not for personal PM2.5-10 exposures. In turn, time spent cleaning contributed to all size-fraction personal exposures, whereas cooking affected only personal PM2.5-10 exposures. The findings showed that the relationship between personal PM2.5 exposures and the corresponding ambient concentrations was influenced by home air exchange rates (or by ventilation status). Because the particle properties or components causing the health effects are unknown, it is not certain to what extent the risk posed by ambient particles can be reduced by controlling any one of these factors.     

Semicontinuous PM2.5 sulfate and nitrate measurements at an urban and a rural location in New York: PMTACS-NY summer 2001 and 2002 campaigns

Several collocated semicontinuous instruments measuring particulate matter with particle sizes < or =2.5 microm (PM2.5) sulfate (SO4(2-)) and nitrate (NO3-) were intercompared during two intensive field campaigns as part of the PM2.5 Technology Assessment and Characterization Study. The summer 2001 urban campaign in Queens, NY, and the summer 2002 rural campaign in upstate New York (Whiteface Mountain) hosted an operation of an Aerosol Mass Spectrometer, Ambient Particulate Sulfate and Nitrate Monitors, a Continuous Ambient Sulfate Monitor, and a Particle-Into-Liquid Sampler with Ion Chromatographs (PILS-IC). These instruments provided near real-time particulate SO4(2-) and NO3- mass concentration data, allowing the study of particulate SO4(2-)/NO3- diurnal patterns and detection of short-term events. Typical particulate SO4(2-) concentrations were comparable at both sites (ranging from 0 to 20 microg/m3), while ambient urban particulate NO3- concentrations ranged from 0 to 11 microg/m3 and rural NO3- concentration was typically less than 1 microg/m3. Results of the intercomparisons of the semicontinuous measurements are presented, as are results of the comparisons between the semicontinuous and time-integrated filter-based measurements. The comparisons at both sites, in most cases, indicated similar performance characteristics. In addition, charge balance calculations, based on major soluble ionic components of atmospheric aerosol from the PILS-IC and the filter measurements, indicated slightly acidic aerosol at both locations.     

Aerosol ion characteristics during the Big Bend Regional Aerosol and Visibility Observational study

The ionic compositions of particulate matter with aerodynamic diameter < or = 2.5 microm (PM2.5) and size-resolved aerosol particles were measured in Big Bend National Park, Texas, during the 1999 Big Bend Regional Aerosol and Visibility Observational study. The ionic composition of PM2.5 aerosol was dominated by sulfate (SO4(2-)) and ammonium (NH4+). Daily average SO4(2-) and NH4+ concentrations were strongly correlated (R2 = 0.94). The molar ratio of NH4+ to SO4(2-) averaged 1.54, consistent with concurrent measurements of aerosol acidity. The aerosol was observed to be comprised of a submicron fine mode consisting primarily of ammoniated SO4(2-) and a coarse particle mode containing nitrate (NO3-). The NO3- appears to be primarily associated with sea salt particles where chloride has been replaced by NO3-, although formation of calcium nitrate (Ca(NO3)2) is important, too, on several days. Size-resolved aerosol composition results reveal that a size cut in particulate matter with aerodynamic diameter < or = 1 microm would have provided a much better separation of fine and coarse aerosol modes than the standard PM2.5 size cut utilized for the study. Although considerable nitric acid exists in the gas phase at Big Bend, the aerosol is sufficiently acidic and temperatures sufficiently high that even significant future reductions in PM2.5 SO4(2-) are unlikely to be offset by formation of particulate ammonium nitrate in summer or fall.     

Particulate matter in California: part 2--Spatial, temporal, and compositional patterns of PM2.5, PM10-2.5, and PM10

Geographic and temporal variations in the concentration and composition of particulate matter (PM) provide important insights into particle sources, atmospheric processes that influence particle formation, and PM management strategies. In the nonurban areas of California, annual-average PM2.5 and PM10 concentrations range from 3 to 10 microg/m3 and from 5 to 18 microg/m3, respectively. In the urban areas of California, annual-averages for PM2.5 range from 7 to 30 microg/m3, with observed 24-hr peaks reaching levels as high as 160 microg/m3. Within each air basin, exceedances are a mixture of isolated events as well as periods of elevated PM2.5 concentrations that are more prolonged and regional in nature. PM2.5 concentrations are generally highest during the winter months. The exception is the South Coast Air Basin, where fairly high values occur throughout the year. Annual-average PM2.5 mass, as well as the concentrations of major components, declined from 1988 to 2000. The declines are especially pronounced for the sulfate (SO4(2-)) and nitrate (NO3-) components of PM2.5 and PM10) and correlate with reductions in ambient levels of oxides of sulfur (SOx) and oxides of nitrogen (NOx). Annual averages for PM10-2.5 and PM10 exhibited similar downwind trends from 1994 to 1999, with a slightly less pronounced decrease in the coarse fraction.     

Fine and coarse particulate matter chemical characterization in a heavily industrialized city in central Mexico during Winter 2003

This paper presents the results of the first reported study on fine particulate matter (PM) chemical composition at Salamanca, a highly industrialized urban area of Central Mexico. Samples were collected at six sites within the urban area during February and March 2003. Several trace elements, organic carbon (OC), elemental carbon (EC), and six ions were analyzed to characterize aerosols. Average concentrations of PM with aerodynamic diameter of less than 10 microm (PM10) and fine PM with aerodynamic diameter of less than 2.5 microm (PM2.5) ranged from 32.2 to 76.6 [g m(-3) and 11.1 to 23.7 microg m(-3), respectively. OC (34%), SO4= (25.1%), EC (12.9%), and geological material (12.5%) were the major components of PM2.5. For PM10 geological material (57.9%), OC (17.3%), and SO4= (9.7%) were the major components. Coarse fraction (PM,, -PM2.5), geological material (81.7%), and OC (8.6%) were the dominant species, which amounted to 90.4%. Correlation analysis showed that sulfate in PM2.5 was present as ammonium sulfate. Sulfate showed a significant spatial variation with higher concentrations to the north resulting from predominantly southwesterly winds above the surface layer and by major SO2 sources that include a power plant and refinery. At the urban site of Cruz Roja it was observed that PM2.5 mass concentrations were similar to the submicron fraction concentrations. Furthermore, the correlation between EC in PM2.5 and EC measured from an aethalometer was r(2) = 0.710. Temporal variations of SO2 and nitrogen oxide were observed during a day when the maximum concentration of PM2.5 was measured, which was associated with emissions from the nearby refinery and power plant. From cascade impactor measurements, the three measured modes of airborne particles corresponded with diameters of 0.32, 1.8, and 5.6 microm.     

Assessment of human exposure to ambient particulate matter

Recent epidemiological studies have consistently shown that the acute mortality effects of high concentrations of ambient particulate matter (PM), documented in historic air pollution episodes, may also be occurring at the low to moderate concentrations of ambient PM found in modern urban areas. In London in December 1952, the unexpected deaths due to PM exposure could be identified and counted as integers by the coroners. In modern times, the PM-related deaths cannot be as readily identified, and they can only be inferred as fractional average daily increases in mortality rates using sophisticated statistical filtering and analyses of the air quality and mortality data. The causality of the relationship between exposure to ambient PM and acute mortality at these lower modern PM concentrations has been questioned because of a perception that there is little significant correlation in time between the ambient PM concentrations and measured personal exposure to PM from all sources (ambient PM plus indoor-generated PM). This article shows that the critical factor supporting the plausibility of a linear PM mortality relationship is the expected high correlation in time of people's exposure to PM of ambient origin with measured ambient PM concentrations, as used in the epidemiological time series studies. The presence of indoor and personal sources of PM masks this underlying relationship, leading to confusion in the scientific literature about the strong underlying temporal relationship between personal exposure to PM of ambient origin and ambient PM concentration. The authors show that the sources of PM of non-ambient origin operate independently of the ambient PM concentrations, so that the mortality effect of non-ambient PM, if any, must be independent of the effects of the ambient PM exposures.     

The influences of ambient particle composition and size on particle infiltration in Los Angeles, CA, residences

Particle infiltration is a key determinant of the indoor concentrations of ambient particles. Few studies have examined the influence of particle composition on infiltration, particularly in areas with high concentrations of volatile particles, such as ammonium nitrate (NH4NO3). A comprehensive indoor monitoring study was conducted in 17 Los Angeles-area homes. As part of this study, indoor/outdoor concentration ratios during overnight (nonindoor source) periods were used to estimate the fraction of ambient particles remaining airborne indoors, or the particle infiltration factor (FINF), for fine particles (PM2.5), its nonvolatile (i.e., black carbon [BC]) and volatile (i.e., nitrate [NO3-]) components, and particle sizes ranging between 0.02 and 10 microm. FINF was highest for BC (median = 0.84) and lowest for NO3- (median = 0.18). The low FINF for NO3- was likely because of volatilization of NO3- particles once indoors, in addition to depositional losses upon building entry. The FINF for PM2.5 (median = 0.48) fell between those for BC and NO3-, reflecting the contributions of both particle components to PM25. FINF varied with particle size, air-exchange rate, and outdoor NO3- concentrations. The FINF for particles between 0.7 and 2 microm in size was considerably lower during periods of high as compared with low outdoor NO3- concentrations, suggesting that outdoor NO3- particles were of this size. This study demonstrates that infiltration of PM2.5 varies by particle component and is lowest for volatile species, such as NH4NO3. Our results suggest that volatile particle components may influence the ability for outdoor PM concentrations to represent indoor and, thus, personal exposures to particles of ambient origin, because volatilization of these particles causes the composition of PM2.5 to differ indoors and outdoors. Consequently, particle composition likely influences observed epidemiologic relationships based on outdoor PM concentrations, especially in areas with high concentrations of NH4NO3 and other volatile particles.     

Personal exposure to fine particulate matter in elderly subjects: relation between personal, indoor, and outdoor concentrations

The time-series correlation between ambient levels, indoor levels, and personal exposure to PM2.5 was assessed in panels of elderly subjects with cardiovascular disease in Amsterdam, the Netherlands, and Helsinki, Finland. Subjects were followed for 6 months with biweekly clinical visits. Each subject's indoor and personal exposure to PM2.5 was measured biweekly, during the 24-hr period preceding the clinical visits. Outdoor PM2.5 concentrations were measured at fixed sites. The absorption coefficients of all PM2.5 filters were measured as a marker for elemental carbon (EC). Regression analyses were conducted for each subject separately, and the distribution of the individual regression and correlation coefficients was investigated. Personal, indoor, and ambient concentrations were highly correlated within subjects over time. Median Pearson's R between personal and outdoor PM2.5 was 0.79 in Amsterdam and 0.76 in Helsinki. For absorption, these values were 0.93 and 0.81 for Amsterdam and Helsinki, respectively. The findings of this study provide further support for using fixed-site measurements as a measure of exposure to PM2.5 in epidemiological time-series studies.     

Source identification of personal exposure to fine particulate matter using organic tracers

Personal exposure to fine particulate matter (PM2.5) is due to both indoor and outdoor sources. Contributions of sources to personal exposure can be quite different from those observed at ambient sampling locations. The primary goal of this study was to investigate the effectiveness of using trace organic speciation data to help identify sources influencing PM2.5 exposure concentrations. Sixty-four 24-h PM2.5 samples were obtained on seven different subjects in and around Boulder, CO. The exposure samples were analyzed for PM2.5 mass, elemental and organic carbon, organic tracer compounds, water-soluble metals, ammonia, and nitrate. This study is the first to measure a broad distribution of organic tracer compounds in PM2.5 personal samples. PM2.5 mass exposure concentrations averaged 8.4 μg m^?3. Organic carbon was the dominant constituent of the PM2.5 mass. Forty-four organic species and 19 water-soluble metals were quantifiable in more than half of the samples. Fifty-four organic species and 16 water-soluble metals had measurement signal-to-noise ratios larger than two after blank subtraction.The dataset was analyzed by Principal Component Analysis (PCA) to determine the factors that account for the greatest variance. Eight significant factors were identified; each factor was matched to its likely source based primarily on the marker species that loaded the factor. The results were consistent with the expectation that multiple marker species for the same source loaded the same factor. Meat cooking was an important source of variability. The factor that represents meat cooking was highly correlated with organic carbon concentrations (r = 0.84). The correlation between ambient PM2.5 and PM2.5 exposure was relatively weak (r = 0.15). Time participants spent performing various activities was generally not well correlated with PCA factor scores, likely because activity duration does not measure emissions intensity. The PCA results demonstrate that organic tracers can aid in identifying factors that influence personal exposures to PM2.5.     

The 1999 Fresno particulate matter exposure studies: comparison of community, outdoor, and residential PM mass measurements

Two collaborative studies have been conducted by the U.S. Environmental Protection Agency (EPA) National Exposure Research Laboratory (NERL) and National Health and Environmental Effects Research Laboratory to determine personal exposures and physiological responses to particulate matter (PM) of elderly persons living in a retirement facility in Fresno, CA. Measurements of PM and other criteria air pollutants were made inside selected individual residences within the retirement facility and at a central outdoor site on the premises. In addition, personal PM exposure monitoring was conducted for a subset of the participants, and ambient PM monitoring data were available for comparison from the NERL PM research monitoring platform in central Fresno. Both a winter (February 1-28, 1999) and a spring (April 19-May 16, 1999) study were completed so that seasonal effects could be evaluated. During the spring study, a more robust personal exposure component was added, as well as a more detailed evaluation of physical factors, such as air-exchange rate, that are known to influence the penetration of particles into the indoor environment. In this paper, comparisons are made among measured personal PM exposures and PM mass concentrations measured at the NERL Fresno Platform site, outside on the premises of the retirement facility, and inside selected residential apartments at the facility during the two 28-day study periods. The arithmetic daily mean personal PM2.5 exposure during the winter study period was 13.3 micrograms/m3, compared with 9.7, 20.5, and 21.7 micrograms/m3 for daily mean overall apartment, outdoor, and ambient (i.e., platform) concentrations, respectively. The daily mean personal PM2.5 exposure during the spring study period was 11.1 micrograms/m3, compared with 8.0, 10.1, and 8.6 micrograms/m3 for the daily mean apartment, outdoor, and ambient concentrations, respectively.     

Assessment of Human Exposure to Ambient Particulate Matter

ABSTRACT

Recent epidemiological studies have consistently shown that the acute mortality effects of high concentrations of ambient particulate matter (PM), documented in historic air pollution episodes, may also be occurring at the low to moderate concentrations of ambient PM found in modern urban areas. In London in December 1952, the unexpected deaths due to PM exposure could be identified and counted as integers by the coroners. In modern times, the PM-related deaths cannot be as readily identified, and they can only be inferred as fractional average daily increases in mortality rates using sophisticated statistical filtering and analyses of the air quality and mortality data. The causality of the relationship between exposure to ambient PM and acute mortality at these lower modern PM concentrations has been questioned because of a perception that there is little significant correlation in time between the ambient PM concentrations and measured personal exposure to PM from all sources (ambient PM plus indoor-generated PM).

This article shows that the critical factor supporting the plausibility of a linear PM mortality relationship is the expected high correlation in time of people's exposure to PM of ambient origin with measured ambient PM concentrations, as used in the epidemiological time series studies. The presence of indoor and personal sources of PM masks this underlying relationship, leading to confusion in the scientific literature about the strong underlying temporal relationship between personal exposure to PM of ambient origin and ambient PM concentration. The authors show that the sources of PM of non-ambient origin operate independently of the ambient PM concentrations, so that the mortality effect of non-ambient PM, if any, must be independent of the effects of the ambient PM exposures.     

The Steubenville Comprehensive Air Monitoring Program (SCAMP): concentrations and solubilities of PM(2.5) trace elements and their implications for source apportionment and health research

The elemental compositions of the water-soluble and acid-digestible fractions of 24-hr integrated fine particulate matter (PM(2.5)) samples collected in Steubenville, OH, from 2000 to 2002 were determined using dynamic reaction cell inductively coupled plasma-mass spectrometry. The water-soluble elemental compositions of PM(2.5) samples collected at four satellite monitoring sites in the surrounding region were also determined. Fe was the most abundant but least water soluble of the elements determined at the Steubenville site, having a mean ambient concentration of 272 ng/m3 and a median fractional solubility of 6%. Fe solubility and its correlations with SO4(2-) and temperature varied significantly by season, consistent with the hypothesis that secondary sulfates may help to mobilize soluble Fe under suitable summertime photochemical conditions. Significantly higher ambient concentrations were observed at Steubenville than at each of the four satellite sites for 10 of the 18 elements (Al, As, Ca, Cd, Fe, Mg, Mn, Na, Pb, and Zn) determined in the water-soluble PM(2.5) fraction. Concentrations of Fe, Mn, and Zn at Steubenville were substantially higher than concentrations reported recently for larger U.S. cities. Receptor modeling identified seven sources affecting the Steubenville site. An (NH4)2SO4-dominated source, likely representing secondary PM(2.5) from coal-fired plants to the west and southwest of Steubenville, accounted for 42% of the PM(2.5) mass, and two sources likely dominated by emissions from motor vehicles and from iron and steel facilities in the immediate Steubenville vicinity accounted for 20% and 10%, respectively. Other sources included an NH4NO3 source (15%), a crustal source (6%), a mixed nonferrous metals and industrial source (3%), and a primary coal combustion source (3%). Results suggest the importance of very different regional and local source mechanisms in contributing to PM(2.5) mass at Steubenville and reinforce the need for further research to elucidate whether metals such as Fe, Mn, and Zn play a role in the PM(2.5) health effects observed previously there.     

The Steubenville Comprehensive Air Monitoring Program (SCAMP): analysis of short-term and episodic variations in PM2.5 concentrations using hourly air monitoring data

One-hour average ambient concentrations of particulate matter (PM) with an aerodynamic diameter < 2.5 microm (PM2.5) were determined in Steubenville, OH, between June 2000 and May 2002 with a tapered element oscillating microbalance (TEOM). Hourly average gaseous copollutant [carbon monoxide (CO), sulfur dioxide (SO2), nitrogen oxide (NOx), and ozone (O3)] concentrations and meteorological conditions also were measured. Although 75% of the 14,682 hourly PM2.5 concentrations measured during this period were < or = 17 microg/m3, concentrations > 65 microg/m3 were observed 76 times. On average, PM2.5 concentrations at Steubenville exhibited a diurnal pattern of higher early morning concentrations and lower afternoon concentrations, similar to the diurnal profiles of CO and NO(x). This pattern was highly variable; however, PM2.5 concentrations > 65 microg/m3 were never observed during the mid-afternoon between 1:00 p.m. and 5:00 p.m. EST. Twenty-two episodes centered on one or more of these elevated concentrations were identified. Five episodes occurred during the months June through August; the maximum PM2.5 concentration during these episodes was 76.6 microg/m3. Episodes occurring during climatologically cooler months often featured higher peak concentrations (five had maximum concentrations between 95.0 and 139.6 microg/m3), and many exhibited strong covariation between PM2.5 and CO, NO(x), or SO2. Case studies suggested that nocturnal surface-based temperature inversions were influential in driving high nighttime concentrations of these species during several cool season episodes, which typically had dramatically lower afternoon concentrations. These findings provide insights that may be useful in the development of PM2.5 reduction strategies for Steubenville, and suggest that studies assessing possible health effects of PM2.5 should carefully consider exposure issues related to the intraday timing of PM2.5 episodes, as well as the potential for toxicological interactions among PM2.5, and primary gaseous pollutants.     

Effects of SO2 and NOx emission reductions on PM2.5 mass concentrations in the southeastern United States

Measurements from sites of the Southeastern Aerosol Research and Characterization (SEARCH) program, made from 1998 to 2001, are used with a thermodynamic equilibrium model, Simulating Composition of Atmospheric Particles at Equilbrium (SCAPE2), to extend an earlier investigation of the responses of fine particulate nitrate (NO3-) and fine particulate matter (PM2.5) mass concentrations to changes in concentrations of nitric acid (HNO3) and sulfate (SO42-). The responses were determined for a projected range of variations of SO42- and HNO3 concentrations resulting from adopted and proposed regulatory initiatives. The predicted PM2.5 mass concentration decreases averaged 1.8-3.9 microg/m3 for SO42- decreases of 46-63% from current concentrations. Combining the S042- decrease with a 40% HNO3 decrease from current concentrations (approximating expected mobile-source oxides of nitrogen [NOx] reductions by 2020) yielded additional incremental reductions of mean predicted PM2.5 mass concentration of 0.2 microg/m3 for three nonurban sites and 0.8-1 microg/m3 for one nonurban and two urban sites. Increasing the HNO3 reduction to 55% (an estimate of adding Clear Skies Phase II NOx reductions) yielded additional incremental reductions of mean predicted PM2.5 mass concentration of 0-0.4 microg/m3. Because of the well-documented losses of particulate NO3- from Federal Reference Method (FRM) filters, only a fraction of these incremental changes would be observed.     

Mass-size distributions of particulate sulfate, nitrate, and ammonium in a particulate matter nonattainment region in southern Taiwan

Concentrations and distributions of three major water-soluble ion species (sulfate, nitrate, and ammonium) contained in ambient particles were measured at three sampling sites in the Kao-ping ambient air quality basin, Taiwan. Ambient particulate matter (PM) samples were collected in a Micro-orifice Uniform Deposit Impactor from February to July 2003 and were analyzed for water-soluble ion species with an ion chromatograph. The PM1/ PM2.5 and PM1/PM10 concentration ratios at the emission source site were 0.73 and 0.53 and were higher than those (0.68 and 0.48) at the background site because there are more combustion sources (i.e., industrial boilers and traffic) around the emission source site. Mass-size distributions of PM NO3- were found in both the fine and coarse modes. SO4(2-)and NH4+ were found in the fine particle mode (PM2.5), with significant fractions of submicron particles (PM1). The source site had higher PM1/PM10(79, 42, and 90%) and PM1/PM2.5 concentration ratios (90, 58, and 93%) for the three major inorganic secondary aerosol components (SO4(2-), NO3-, and NH4+) than the receptor site (65, 27, and 65% for PM1/PM10, 69, 51, and 70% for PM1/PM2.5. Results obtained in this study indicate that the PM1 (submicron aerosol particles) fraction plays an important role in the ambient atmosphere at both emission source and receptor sites. Further studies regarding the origin and formation of ambient secondary aerosols are planned.     

Characterization of major chemical components of fine particulate matter in North Carolina

This paper presents measurements of daily sampling of fine particulate matter (PM2.5) and its major chemical components at three urban and one rural locations in North Carolina during 2002. At both urban and rural sites, the major insoluble component of PM2.5 is organic matter, and the major soluble components are sulfate (SO4(2-)), ammonium (NH4(+)), and nitrate (NO3(-)). NH4(+) is neutralized mainly by SO4(2-) rather than by NO3(-), except in winter when SO4(2-) concentration is relatively low, whereas NO3(-) concentration is high. The equivalent ratio of NH4(+) to the sum of SO4(2-) and NO3(-) is < 1, suggesting that SO4(2-) and NO3(-) are not completely neutralized by NH4(+). At both rural and urban sites, SO4(2-) concentration displays a maximum in summer and a minimum in winter, whereas NO3(-) displays an opposite seasonal trend. Mass ratio of NO3(-) to SO4(2-) is consistently < 1 at all sites, suggesting that stationary source emissions may play an important role in PM2.5 formation in those areas. Organic carbon and elemental carbon are well correlated at three urban sites although they are poorly correlated at the agriculture site. Other than the daily samples, hourly samples were measured at one urban site. PM2.5 mass concentrations display a peak in early morning, and a second peak in late afternoon. Back trajectory analysis shows that air masses with lower PM2.5 mass content mainly originate from the marine environment or from a continental environment but with a strong subsidence from the upper troposphere. Air masses with high PM2.5 mass concentrations are largely from continental sources. Our study of fine particulate matter and its chemical composition in North Carolina provides crucial information that may be used to determine the efficacy of the new National Ambient Air Quality Standard (NAAQS) for PM fine. Moreover, the gas-to-particle conversion processes provide improved prediction of long-range transport of pollutants and air quality.