The Steubenville Comprehensive Air Monitoring Program (SCAMP): Analysis of Short-Term and Episodic Variations in PM2.5 Concentrations Using Hourly Air Monitoring Data

Abstract

One-hour average ambient concentrations of particulate matter (PM) with an aerodynamic diameter <2.5 μm (PM_2.5) 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 (NO_x), and ozone (O₃)] concentrations and meteorological conditions also were measured. Although 75% of the 14,682 hourly PM_2.5 concentrations measured during this period were ≤17 μg/m³, concentrations >65 μg/m³ were observed 76 times. On average, PM_2.5 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, PM_2.5 concentrations >65 μg/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 PM_2.5 concentration during these episodes was 76.6 μg/m³. Episodes occurring during climatologically cooler months often featured higher peak concentrations (five had maximum concentrations between 95.0 and 139.6 μg/m³), and many exhibited strong covariation between PM_2.5 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 PM_2.5 reduction strategies for Steubenville, and suggest that studies assessing possible health effects of PM_2.5 should carefully consider exposure issues related to the intraday timing of PM_2.5 episodes, as well as the potential for toxicological interactions among PM_2.5 and primary gaseous pollutants.     

The Steubenville comprehensive air monitoring program (SCAMP): associations among fine particulate matter, co-pollutants, and meteorological conditions

We determined 24-hr average ambient concentrations of PM2.5 and its ionic and carbonaceous components in Steubenville, OH, between May 2000 and May 2002. We also determined daily average gaseous co-pollutant concentrations, meteorological conditions, and pollen and mold spore counts. Data were analyzed graphically and by linear regression and time series models. Multiple-day episodes of elevated fine particulate matter (PM2.5) concentrations often occurred during periods of locally high temperature (especially during summer), high pressure, or low wind speed (especially during winter) and generally ended with the passage of a frontal system. After removing autocorrelation, we observed statistically significant positive associations between concentrations of PM2.5 and concentrations of CO, NOx, and SO2. Associations with NOx and CO exhibited significant seasonal dependencies, with the strongest correlations during fall and winter. NOx, CO, SO2, O3, temperature, relative humidity, and wind speed were all significant predictors of PM2.5 concentration in a time-series model with external regressors, which successfully accounted for 79% of the variance in log-transformed daily PM2.5 concentrations. Coefficient estimates for NOx and temperature varied significantly by season. The results provide insight that may be useful in the development of future PM2.5 reduction strategies for Steubenville. Additionally, they demonstrate the need for PM epidemiology studies in Steubenville (and elsewhere) to carefully consider the potential confounding effects of gaseous co-pollutants, such as CO and NOx, and their seasonally dependent associations with PM2.5.     

Defining the photochemical contribution to particulate matter in urban areas using time-series analysis

The objective of this project is to demonstrate how the ambient air measurement record can be used to define the relationship between O3 (as a surrogate for photochemistry) and secondary particulate matter (PM) in urban air. The approach used is to develop a time-series transfer-function model describing the daily PM10 (PM with less than 10 microm aerodynamic diameter) concentration as a function of lagged PM and current and lagged O3, NO or NO2, CO, and SO2. Approximately 3 years of daily average PM10, daily maximum 8-hr average O3 and CO, daily 24-hr average SO2 and NO2, and daily 6:00 a.m.-9:00 a.m. average NO from the Aerometric Information Retrieval System (AIRS) air quality subsystem are used for this analysis. Urban areas modeled are Chicago, IL; Los Angeles, CA; Phoenix, AZ; Philadelphia, PA; Sacramento, CA; and Detroit, MI. Time-series analysis identified significant autocorrelation in the O3, PM10, NO, NO2, CO, and SO2 series. Cross correlations between PM10 (dependent variable) and gaseous pollutants (independent variables) show that all of the gases are significantly correlated with PM10 and that O3 is also significantly correlated lagged up to two previous days. Once a transfer-function model of current PM10 is defined for an urban location, the effect of an O3-control strategy on PM concentrations is estimated by calculating daily PM10 concentrations with reduced O3 concentrations. Forecasted summertime PM10 reductions resulting from a 5 percent decrease in ambient O3 range from 1.2 microg/m3 (3.03%) in Chicago to 3.9 microg/m3 (7.65%) in Phoenix.     

The Steubenville comprehensive air monitoring program (SCAMP): overview and statistical considerations

Average concentrations of particulate matter with an aerodynamic diameter less than or equal to 2.5 microm (PM2.5) in Steubenville, OH, have decreased by more than 10 microg/m3 since the landmark Harvard Six Cities Study associated the city's elevated PM2.5 concentrations with adverse health effects in the 1980s. Given the promulgation of a new National Ambient Air Quality Standard (NAAQS) for PM2.5 in 1997, a current assessment of PM2.5 in the Steubenville region is warranted. The Steubenville Comprehensive Air Monitoring Program (SCAMP) was conducted from 2000 through 2002 to provide such an assessment. The program included both an outdoor ambient air monitoring component and an indoor and personal air sampling component. This paper, which is the first in a series of four that will present results from the outdoor portion of SCAMP, provides an overview of the outdoor ambient air monitoring program and addresses statistical issues, most notably autocorrelation, that have been overlooked by many PM2.5 data analyses. The average PM2.5 concentration measured in Steubenville during SCAMP (18.4 microg/m3) was 3.4 microg/m3 above the annual PM2.5 NAAQS. On average, sulfate and organic material accounted for approximately 31% and 25%, respectively, of the total PM2.5 mass. Local sources contributed an estimated 4.6 microg/m3 to Steubenville's mean PM2.5 concentration. PM2.5 and each of its major ionic components were significantly correlated in space across all pairs of monitoring sites in the region, suggesting the influence of meteorology and long-range transport on regional PM2.5 concentrations. Statistically significant autocorrelation was observed among time series of PM2.5 and component data collected at daily and 1-in-4-day frequencies during SCAMP. Results of spatial analyses that accounted for autocorrelation were generally consistent with findings from previous studies that did not consider autocorrelation; however, these analyses also indicated that failure to account for autocorrelation can lead to incorrect conclusions about statistical significance.     

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.     

Hourly measurements of fine particulate sulfate and carbon aerosols at the Harvard-U.S. Environmental Protection Agency Supersite in Boston

Hourly concentrations of ambient fine particle sulfate and carbonaceous aerosols (elemental carbon [EC], organic carbon [OC], and black carbon [BC]) were measured at the Harvard-U.S. Environmental Protection Agency Supersite in Boston, MA, between January 2007 and October 2008. These hourly concentrations were compared with those made using integrated filter-based measurements over 6-day or 24-hr periods. For sulfate, the two measurement methods showed good agreement. Semicontinuous measurements of EC and OC also agreed (but not as well as for sulfate) with those obtained using 24-hr integrated filter-based and optical BC reference methods. During the study period, 24-hr PM2.5 (particulate matter [PM] < or = 2.5 microm in aerodynamic diameter) concentrations ranged from 1.4 to 37.6 microg/m3, with an average of 9.3 microg/m3. Sulfate as the equivalent of ammonium sulfate accounted for 39.1% of the PM2.5 mass, whereas EC and OC accounted for 4.2 and 35.2%, respectively. Hourly sulfate concentrations showed no distinct diurnal pattern, whereas hourly EC and BC concentrations peaked during the morning rush hour between 7:00 and 9:00 a.m. OC concentrations also exhibited nonpronounced, small peaks during the day, most likely related to traffic, secondary organic aerosol, and local sources, respectively.     

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.     

Response of inorganic fine particulate matter to emission changes of sulfur dioxide and ammonia: the eastern United States as a case study

A three-dimensional chemical transport model (PMCAMx) was used to investigate changes in fine particle (PM2.5) concentrations in response to changes in sulfur dioxide (SO2) and ammonia (NH3) emissions during July 2001 and January 2002 in the eastern United States. A uniform 50% reduction in SO2 emissions was predicted to produce an average decrease of PM2.5 concentrations by 26% during July but only 6% during January. A 50% reduction of NH3 emissions leads to an average 4 and 9% decrease in PM2.5 in July and January, respectively. During the summer, the highest concentration of sulfate is in South Indiana (12.8 microg x m(-3)), and the 50% reduction of SO2 emissions results in a 5.7 microg x m(-3) (44%) sulfate decrease over this area. During winter, the SO2 emissions reduction results in a 1.5 microg x m(-3) (29%) decrease of the peak sulfate levels (5.2 microg x m(-3)) over Southeast Georgia. The maximum nitrate and ammonium concentrations are predicted to be over the Midwest (1.9 (-3)g x m(-3) in Ohio and 5.3 microg x m(-3) in South Indiana, respectively) in the summer whereas in the winter these concentrations are higher over the Northeast (3 microg x m(-3) of nitrate in Connecticut and 2.7 microg x m(-3) of ammonium in New York). The 50% NH3 emissions reduction is more effective for controlling nitrate, compared with SO2 reductions, producing a 1.1 microg x m(-3) nitrate decrease over Ohio in July and a 1.2 microg x m(-3) decrease over Connecticut in January. Ammonium decreases significantly when either SO2 or NH3 emissions are decreased. However, the SO2 control strategy has better results in July when ammonium decreases, up to 2 microg x m(-3) (37%), are predicted in South Indiana. The NH3 control strategy has better results in January (ammonium decreases up to 0.4 microg x m(-3) in New York). The spatial and temporal characteristics of the effectiveness of these emission control strategies during the summer and winter seasons are discussed.     

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.     

Particle size distribution and anion content at a traffic site in Sha-Lu, Taiwan.

Ambient air particle concentrations were sampled by two total suspended particle (TSP) samplers, PM10/PM2.5 specific sampler and micro-orifice uniform deposit impactor (MOUDI) during July-October 2000 at a traffic sampling site in central Taiwan. The average TSP concentration (194 microg/m3) was about a factor of two higher than that of the fraction <2.5 microm (93.2 microg/m3). The mean level of the fraction <10 microm collected by MOUDI (93.2 microg/m3) was about 1 1/2 times higher than that of the size class <2.5 microm (43.8 microg/m3). Furthermore, this fraction showed a certain correlation with the TSP concentration. The particle size distribution was bimodal in the ambient air at the traffic site. The major peaks appear at particle diameters between 0.56-1.0 and 3.2-5.6 microm. The percentages of anions contained in TSP were 0.24% F-, 13.7% Cl, 0.52% Br, 12.0% NO-, 18.9% NO2-, and 54.6% SO2-. The Cl-, NO2-, and NO3- size distributions were all unimodal and the major peaks appeared at 3.2-5.6 microm. The SO2 size distribution was bimodal, with major peaks at 0.32-0.56 and 3.2-5.6.     

Chemical characterisation of PM episodes in NE Spain

The chemical composition of ambient particulate matter (PM) varies widely as a function of its main emission sources and of the chemical reactions which take place in the atmosphere. The aim of this study is to obtain the chemical profile of PM10 and PM2.5 during peak PM episodes, thus identifying the main emission sources and/or atmospheric processes which originate the PM episodes. To this end, cluster analysis was applied to a set of PM10 and PM2.5 data collected throughout 2001 in two urban and industrialised areas in NE Spain. As a result of this analysis, five clusters were identified for each site, and the interpretation of their chemical profiles lead to the identification of five types of peak PM episodes for each site: industrial, traffic and regional re-circulation episodes at both sites, plus crustal episodes in Barcelona, and peak traffic and industrial episodes (T+I) in Tarragona. Traffic episodes are characterised by daily means of 23 and 10 microg/m3 of OM+EC in Barcelona and Tarragona in PM10. Levels of secondary inorganic aerosols reach average daily means of 19 and 11 microg/m3 in Barcelona and Tarragona in PM10 during industrial episodes. High levels of sulphate (>5 microg/m3) and ozone (up to 77 microg/m3 daily mean) are good tracers of regional re-circulation episodes. During crustal episodes daily means of crustal elements reach up to 34 microg/m3 in Barcelona. Special attention has been drawn to the composition of the mineral matter during the different PM episodes.     

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.     

Inorganic PM2.5 at a U.S. agricultural site

In this study, we present approximately two years (January 1999-December 2000) of atmospheric NH3, NH4+, HCl, Cl-, HNO3, NO3-, SO2, and SO4= concentrations measured by the annular denuder/filter pack method at an agricultural site in eastern North Carolina. This site is influenced by high NH3 emissions from animal production and fertilizer use in the surrounding area and neighboring counties. The two-year mean NH3 concentration is 5.6 (+/-5.13) microg m(-3). The mean concentration of total inorganic PM2.5, which includes SO4=, NO3-, NH4+, and Cl-, is 8.0 (+/-5.84) microg m(-3). SO4=, NO3-, NH4+, and Cl- represent, respectively, 53, 24, 22, and 1% of measured inorganic PM2.5. NH3 contributes 72% of total NH3 + NH4+, on an average. Equilibrium modeling of the gas+aerosol NH3/H2SO4/HNO3 system shows that inorganic PM2.5 is more sensitive to reductions in gas + aerosol concentrations of sulfate and nitrate relative to NH3.     

Indoor and outdoor air quality investigation at schools in Hong Kong

Five classrooms in Hong Kong (HK), air-conditioned or ceiling fans ventilated, were chosen for investigation of indoor and outdoor air quality. Parameters such as temperature, relative humidity (RH), carbon dioxide (CO2), sulphur dioxide (SO2), nitric oxide (NO), nitrogen dioxide (NO2), respirable particulate matter (PM10), formaldehyde (HCHO), and total bacteria counts were monitored indoors and outdoors simultaneously. The average respirable particulate matter concentrations were higher than the HK Objective, and the maximum indoor PM10 level exceeded 1000 microg/m3. Indoor CO2 concentrations often exceeded 1000 microl/l in air-conditioning and ceiling fan classrooms, indicating inadequate ventilation. Maximum indoor CO2 level reached 5900 microl/l during class at the classroom with cooling tower ventilation. Increasing the rate of ventilation or implementation of breaks between classes is recommended to alleviate the high CO2 level. Other pollution parameters measured in this study complied with the standards. The two most important classroom air quality problems in Hong Kong were PM10 and CO2 levels.     

Short-term temporal variation in PM2.5 mass and chemical composition during the Atlanta Supersite Experiment, 1999

Measurements in urban Atlanta of transient aerosol events in which PM2.5 mass concentrations rapidly rise and fall over a period of 3-6 hr are reported. The data are based on new measurement techniques demonstrated at the U.S. Environmental Protection Agency (EPA) Atlanta Supersite Experiment in August 1999. These independent instruments for aerosol chemical speciation of NO3-, SO4(2-), NH4+, and organic and elemental carbon (OC and EC), reconstructed the observed hourly dry PM2.5 mass to within 20% or better. Data from the experiment indicated that transient PM2.5 events were ubiquitous in Atlanta and were typically characterized by a sudden increase of EC (soot) and OC in the early morning or SO4(2-) in the late afternoon. The frequent temporal decoupling of these events provides insights into their origins, suggesting mobile sources in metro Atlanta as the main contributor to early morning PM2.5 and more regionally located point SO2 sources for afternoon PM2.5 events. The transient events may also have health implications. New data suggest that short-term PM2.5 exposures may lead to adverse health effects. Standard integrated filter-based techniques used in PM2.5 compliance monitoring networks and in most past PM2.5 epidemiologic studies collect samples over 24-hr periods and thus are unable to capture these transient events. Moreover, health-effects studies that focus on daily PM2.5 mass alone cannot evaluate the health implications of the unique and variable chemical properties of these episodes.     

Analysis of a summertime PM2.5 and haze episode in the mid-Atlantic region

Observations of the mass and chemical composition of particles less than 2.5 microm in aerodynamic diameter (PM2.5), light extinction, and meteorology in the urban Baltimore-Washington corridor during July 1999 and July 2000 are presented and analyzed to study summertime haze formation in the mid-Atlantic region. The mass fraction of ammoniated sulfate (SO4(2-)) and carbonaceous material in PM2.5 were each approximately 50% for cleaner air (PM2.5< 10 microg/m3) but changed to approximately 60% and approximately 20%, respectively, for more polluted air (PM2.5>30 microg/m3). This signifies the role of SO4(2-) in haze formation. Comparisons of data from this study with the Interagency Monitoring of Protected Visual Environments network suggest that SO4(2-) is more regional than carbonaceous material and originates in part from upwind source regions. The light extinction coefficient is well correlated to PM2.5 mass plus water associated with inorganic salt, leading to a mass extinction efficiency of 7.6 +/- 1.7 m2/g for hydrated aerosol. The most serious haze episode occurring between July 15 and 19, 1999, was characterized by westerly transport and recirculation slowing removal of pollutants. At the peak of this episode, 1-hr PM2.5 concentration reached approximately 45 microg/m3, visual range dropped to approximately 5 km, and aerosol water likely contributed to approximately 40% of the light extinction coefficient.     

Source identification and trends in concentrations of gaseous and fine particulate principal species in Seoul, South Korea

Ambient measurements were made using two sets of annular denuder system during the four seasons (April 2001 to February 2002) and were then compared with the results during the period of 1996-1997 to estimate the trends and seasonal variations in concentrations of gaseous and fine particulate matter (PM2.5) principal species. Annual averages of gaseous HNO3 and NH3 increased by 11% and 6%, respectively, compared with those of the previous study, whereas HONO and SO2 decreased by 11% and 136%, respectively. The PM2.5 concentration decreased by -17%, 35% for SO4(2-), and 29% for NH4+, whereas NO3- increased by 21%. Organic carbon (OC) and elemental carbon (EC) were 12.8 and 5.98 microg/m(-3), accounting for -26 and 12% of PM2.5 concentration, respectively. The species studied accounted for 84% of PM2.5 concentration, ranging from 76% in winter to 97% in summer. Potential source contribution function (PSCF) analysis was used to identify possible source areas affecting air pollution levels at a receptor site in Seoul. High possible source areas in concentrations of PM2.5, NO3-, SO4(2-), NH4+, and K+ were coastal cities of Liaoning province (possibly emissions from oil-fired boilers on ocean liners and fishing vessels and industrial emissions), inland areas of Heibei/Shandong provinces (the highest density areas of agricultural production and population) in China, and typical port cities (Mokpo, Yeosu, and Busan) of South Korea. In the PSCF map for OC, high possible source areas were also coastal cities of Liaoning province and inland areas of Heibei/Shandong provinces in China. In contrast, high possible source areas of EC were highlighted in the south of the Yellow Sea, indicating possible emissions from oil-fired boilers on large ships between South Korea and Southeast Asia. In summary, the PSCF results may suggest that air pollution levels in Seoul are affected considerably by long-range transport from external areas, such as the coastal zone in China and other cities in South Korea, as well as Seoul itself.     

Multiple-year black carbon measurements and source apportionment using delta-C in Rochester, New York

Black carbon (BC), an important component ofthe atmospheric aerosol, has climatic, environmental, and human health significance. In this study, BC was continuously measured using a two-wavelength aethalometer (370 nm and 880 nm) in Rochester; New York, from January 2007 to December 2010. The monitoring site is adjacent to two major urban highways (I-490 and I-590), where 14% to 21% of the total traffic was heavy-duty diesel vehicles. The annual average BC concentrations were 0.76 microg/m3, 0.67 microg/m3, 0.60 microg/m3, and 0.52 microg/m3 in 2007, 2008, 2009, and 2010, respectively. Positive matrix factorization (PMF) modeling was performed using PM2.5 elements, sulfate, nitrate, ammonia, elemental carbon (EC), and organic carbon (OC) data from the US. Environmental Protection Agency (EPA) speciation network and Delta-C (UVBC370nm-BC880nm) data. Delta-C has been previously shown to be a tracer of wood combustion factor It was used as an input variable in source apportionment models for the first time in this study and was found to play an important role in separating traffic (especially diesel) emissions from wood combustion emissions. The result showed the annual average PM2.5 concentrations apportioned to diesel emissions in 2007, 2008, 2009, and 2010 were 1.34 microg/m3, 1.25 microg/m3, 1.13 microg/m3, and 0.97 microg/m3, respectively. The BC conditional probability function (CPF) plots show a large contribution from the highway diesel traffic to elevated BC concentrations. The measurements and modeling results suggest an impact of the US Environmental Protection Agency (EPA) 2007 Heavy-Duty Highway Rule on the decrease ofBC and PM2.5 concentrations during the study period.     

The Southeastern Aerosol Research and Characterization Study, part 3: continuous measurements of fine particulate matter mass and composition

Deployment of continuous analyzers in the Southeastern Aerosol Research and Characterization Study (SEARCH) network began in 1998 and continues today as new technologies are developed. Measurement of fine particulate matter (PM2.5) mass is performed using a dried, 30 degrees C tapered element oscillating microbalance (TEOM). TEOM measurements are complemented by observations of light scattering by nephelometry. Measurements of major constituents include: (1) SO4(2-) via reduction to SO2; (2) NH4+ and NO3- via respective catalytic oxidation and reduction to NO, (3) black carbon (BC) by optical absorption, (4) total carbon by combustion to CO2, and (5) organic carbon by difference between the latter two measurements. Several illustrative examples of continuous data from the SEARCH network are presented. A distinctive composite annual average diurnal pattern is observed for PM2.5 mass, nitrate, and BC, likely indicating the influence of traffic-related emissions, growth, and break up of the boundary layer and formation of ammonium nitrate. Examination of PM2.5 components indicates the need to better understand the continuous composition of the unmeasured "other" category, because it contributes a significant fraction to total mass during periods of high PM2.5 loading. Selected episodes are presented to illustrate applications of SEARCH data. An SO2 conversion rate of 0.2%/hr is derived from an observation of a plume from a coal-fired power plant during early spring, and the importance of local, rural sources of NH3 to the formation of ammonium nitrate in particulate matter (PM) is demonstrated.