Planning an Environmental Survey for a Nuclear Power Plant Site

Abstract

Subsequent to the 1997 promulgation of the Federal Reference Method (FRM) for monitoring fine particulate matter (PM_2.5) in ambient air, U.S. Environmental Protection Agency (EPA) received reports that the DOW 704 diffusion oil used in the method’s Well Impactor Ninety-Six (WINS) fractionator would occasionally crystallize during field use, particularly under wintertime conditions. Although the frequency of occurrence on a nationwide basis was low, uncertainties existed as to whether crystallization of the DOW 704 oil may adversely affect a sampling event’s data quality. In response to these concerns, EPA and the State of Connecticut Department of Environmental Protection jointly conducted a series of specialized tests to determine whether crystallized oil adversely affected the performance of the WINS fractionator. In the laboratory, an experimental setup used dry ice to artificially induce crystallization of the diffusion oil under controlled conditions. Using primary polystyrene latex calibration aerosols, standard size-selective performance tests of the WINS fractionator showed that neither the position nor the shape of the WINS particle size fractionation curve was substantially influenced by the crystallization of the DOW 704 oil. No large particle bounce from the crystallized impaction surface was observed. During wintertime field tests, crystallization of the DOW 704 oil did not adversely affect measured PM_2.5 concentrations. Regression of measurements with crystallized DOW 704 versus liquid dioctyl sebacate (DOS) oil produced slope, intercept, and R² values of 0.98, 0.1, and 0.997 μg/m³, respectively. Additional field tests validated the use of DOS as an effective impaction substrate. As a result of these laboratory and field tests, DOS oil has been approved by EPA as a substitute for DOW 704 oil. Since the field deployment of DOS oil in 2001, users of this alternative oil have not reported any operational problems associated with its use in the PM_2.5 FRM. Limited field evaluation of the BGI very sharp cut cyclone indicates that it provides a viable alternative to the WINS fractionator.     

Development and evaluation of an impactor for a PM2.5 speciation sampler

A conventional impactor for a particle speciation sampler was developed and validated through laboratory and field tests. The speciation sampler consists of the following components: a PM2.5 conventional impactor that removes particles larger than 2.5 microns, an all-glass, coated honeycomb diffusion denuder, and a 47-mm filter pack. The speciation sampler can operate at two different sampling rates: 10 and 16.7 L/min. An experimental characterization of the impactor's performance was conducted. The impactor's collection efficiency was examined as a function of critical design parameters such as Reynolds number, the distance from the nozzle exit to the impaction plate, and the impaction substrate coating method. The bounce of particles larger than the cut point was successfully minimized by using a greased surface as the impaction substrate. Additionally, a series of field intercomparison experiments were conducted at both 10 and 16.7 L/min airflow. PM2.5 mass and SO4(2-) concentrations were measured and compared with the Federal Reference Method (FRM) and found to be in good agreement. Results of the laboratory chamber tests also indicated that the impactor's performance was in good agreement with the FRM.     

Nonlinear regression adjustments of multiple continuous monitoring methods produce effective characterization of short-term fine particulate matter

This study comprehensively characterizes hourly fine particulate matter (PM(2.5)) concentrations measured via a tapered element oscillating microbalance (TEOM), beta-gauge, and nephelometer from four different monitoring sites in U.S. Environment Protection Agency (EPA) Region 5 (in U.S. states Illinois, Michigan, and Wisconsin) and compares them to the Federal Reference Method (FRM). Hourly characterization uses time series and autocorrelation. Hourly data are compared with FRM by averaging across 24-hr sampling periods and modeling against respective daily FRM concentrations. Modeling uses traditional two-variable linear least-squares regression as well as innovative nonlinear regression involving additional meteorological variables such as temperature and humidity. The TEOM shows a relationship with season and temperature, linear correlation as low as 0.7924 and nonlinear model correlation as high as 0.9370 when modeled with temperature. The beta-gauge shows no relationship with season or meteorological variables. It exhibits a linear correlation as low as 0.8505 with the FRM and a nonlinear model correlation as high as 0.9339 when modeled with humidity. The nephelometer shows no relationship with season or temperature but a strong relationship with humidity is observed. A linear correlation as low as 0.3050 and a nonlinear model correlation as high as 0.9508 is observed when modeled with humidity. Nonlinear models have higher correlation than linear models applied to the same dataset. This correlation difference is not always substantial, which may introduce a tradeoff between simplicity of model and degree of statistical association. This project shows that continuous monitor technology produces valid PM(2.5) characterization, with at least partial accounting for variations in concentration from gravimetric reference monitors once appropriate nonlinear adjustments are applied. Although only one regression technically meets new EPA National Ambient Air Quality Standards (NAAQS) Federal Equivalent Method (FEM) correlation coefficient criteria, several others are extremely close, showing optimistic potential for use of this nonlinear adjustment model in garnering EPA NAAQS FEM approval for continuous PM(2.5) sampling methods.     

Assessing source characteristics of PM2.5 in the eastern United States using positive matrix factorization

Fine aerosol (PM2.5) measurements obtained from the first year of operation of the nationwide network of PM2.5 monitors were studied with the factor analysis technique of positive matrix factorization (PMF). PM2.5 mass concentration data were extracted from the Atmospheric Information Retrieval System (AIRS) database of the U.S. Environmental Protection Agency (EPA). PMF was applied to measurements at more than 350 monitoring locations in the eastern half of the United States. Data consisted of PM2.5 24-hr averaged concentrations measured every third day from April through December 1999. The PMF model suggested six factors representing source influences to the PM2.5 mass concentrations at measurement sites. Factor 5, covering much of the Appalachian states, exhibited significant seasonal behavior.     

Air quality measurements from the Fresno Supersite

The Fresno Supersite intends to 1) evaluate non-routine monitoring methods, establishing their comparability with existing methods and their applicability to air quality planning, exposure assessment, and health effects studies; 2) provide a better understanding of aerosol characteristics, behavior, and sources to assist regulatory agencies in developing standards and strategies that protect public health; and 3) support studies that evaluate relationships between aerosol properties, co-factors, and observed health end-points. Supersite observables include in-situ, continuous, short-duration measurements of 1) PM2.5, PM10, and coarse (PM10 minus PM2.5) mass; 2) PM2.5 SO4(-2), NO3-, carbon, light absorption, and light extinction; 3) numbers of particles in discrete size bins ranging from 0.01 to approximately 10 microns; 4) criteria pollutant gases (O3, CO, NOx); 5) reactive gases (NO2, NOy, HNO3, peroxyacetyl nitrate [PAN], NH3); and 6) single particle characterization by time-of-flight mass spectrometry. Field sampling and laboratory analysis are applied for gaseous and particulate organic compounds (light hydrocarbons, heavy hydrocarbons, carbonyls, polycyclic aromatic hydrocarbons [PAH], and other semi-volatiles), and PM2.5 mass, elements, ions, and carbon. Observables common to other Supersites are 1) daily PM2.5 24-hr average mass with Federal Reference Method (FRM) samplers; 2) continuous hourly and 5-min average PM2.5 and PM10 mass with beta attenuation monitors (BAM) and tapered element oscillating microbalances (TEOM); 3) PM2.5 chemical speciation with a U.S. Environmental Protection Agency (EPA) speciation monitor and protocol; 4) coarse particle mass by dichotomous sampler and difference between PM10 and PM2.5 BAM and TEOM measurements; 5) coarse particle chemical composition; and 6) high sensitivity and time resolution scalar and vector wind speed, wind direction, temperature, relative humidity, barometric pressure, and solar radiation. The Fresno Supersite is coordinated with health and toxicological studies that will use these data in establishing relationships with asthma, other respiratory disease, and cardiovascular changes in human and animal subjects.     

Characterization of the fugitive particulate emissions from construction mud/dirt carryout

Although the fugitive dust associated with construction mud/dirt carryout can represent a substantial portion of the particulate matter (PM) emissions inventory in nonattainment areas, it has not been well characterized by direct sampling methods. In this paper, a research program is described that directly determined both PM10 and PM2.5 (particles < or =10 and 2.5 microm in classical aerodynamic diameter, respectively) emission factors for mud/dirt carryout from a major construction project located in metropolitan Kansas City, MO. The program also assessed the contribution of automotive emissions to the total PM2.5 burden and determined the baseline emissions from the test road. As part of the study, both time-integrated and continuous exposure-profiling methods were used to assess the PM emissions, including particle size and elemental composition. This research resulted in overall PM10 and PM2.5 emission factors of 6 and 0.2 g/vehicle, respectively. Although PM10 is within the range of prior U.S. Environmental Protection Agency (EPA) guidance, the PM2.5 emission factor is far lower than previous estimates published by EPA. In addition, based on both the particle size and chemical data obtained in the study, a major portion of the PM2.5 emissions appears to be attributable to automotive exhaust from light-duty, gasoline-powered vehicles and not to the fugitive dust associated with reentrained mud/dirt carryout.     

Development of a Sample Equilibration System for the TEOM Continuous PM Monitor

ABSTRACT

In recent years, scientific discussion has included the influence of thermodynamic conditions (e.g., temperature, relative humidity, and filter face velocity) on PM retention efficiency of filter-based samplers and monitors. Method-associated thermodynamic conditions can, in some instances, dramatically influence the presence of particle-bound water and other light-molecular-weight chemical components such as particulate nitrates and certain organic compounds. The measurement of fine particle mass presents a new challenge for all PM measurement methods, since a relatively greater fraction of the mass is semi-volatile.

The tapered element oscillating microbalance (TEOM) continuous PM monitor is a U.S. Environmental Protection Agency (EPA) PM₁₀ equivalent method (EQPM-1090-079). Several hundred of these monitors are deployed throughout the United States. The TEOM monitor has the unique characteristic of providing direct PM mass measurement without the calibration uncertainty inherent in mass surrogate methods. In addition, it provides high-precision, near-real-time continuous data automatically. Much attention has been given to semi-volatile species retention of the TEOM method.

While using this monitor, it is desirable to maintain as low an operating temperature as practical and to remove unwanted particle-bound water. A new sample equilibration system (SES) has been developed to allow conditioning of the PM sample stream to a lower humidity and temperature level. The SES incorporates a special low-particle-loss Nafion dryer. This paper discusses the configuration and theory of the SES. Performance results include high time-resolved PM_2.5 data comparison between a 30 °C sample stream TEOM monitor with SES and a standard 50 °C TEOM monitor. In addition, 24-hr integrated data are compared with data collected using an EPA PM_2.5 Federal Reference Method (FRM)-type sampler. The SES is a significant development because it can be applied easily to existing TEOM monitors.     

Comparison of particle size distributions and elemental partitioning from the combustion of pulverized coal and residual fuel oil

U.S. Environmental Protection Agency (EPA) research examining the characteristics of primary PM generated by the combustion of fossil fuels is being conducted in efforts to help determine mechanisms controlling associated adverse health effects. Transition metals are of particular interest, due to the results of studies that have shown cardiopulmonary damage associated with exposure to these elements and their presence in coal and residual fuel oils. Further, elemental speciation may influence this toxicity, as some species are significantly more water-soluble, and potentially more bio-available, than others. This paper presents results of experimental efforts in which three coals and a residual fuel oil were combusted in three different systems simulating process and utility boilers. Particle size distributions (PSDs) were determined using atmospheric and low-pressure impaction as well as electrical mobility, time-of-flight, and light-scattering techniques. Size-classified PM samples from this study are also being utilized by colleagues for animal instillation experiments. Experimental results on the mass and compositions of particles between 0.03 and > 20 microns in aerodynamic diameter show that PM from the combustion of these fuels produces distinctive bimodal and trimodal PSDs, with a fine mode dominated by vaporization, nucleation, and growth processes. Depending on the fuel and combustion equipment, the coarse mode is composed primarily of unburned carbon char and associated inherent trace elements (fuel oil) and fragments of inorganic (largely calcium-alumino-silicate) fly ash including trace elements (coal). The three coals also produced a central mode between 0.8- and 2.0-micron aerodynamic diameter. However, the origins of these particles are less clear because vapor-to-particle growth processes are unlikely to produce particles this large. Possible mechanisms include the liberation of micron-scale mineral inclusions during char fragmentation and burnout and indicates that refractory transition metals can contribute to PM < 2.5 microns without passing through a vapor phase. When burned most efficiently, the residual fuel oil produces a PSD composed almost exclusively of an ultrafine mode (approximately 0.1 micron). The transition metals associated with these emissions are composed of water-soluble metal sulfates. In contrast, the transition metals associated with coal combustion are not significantly enriched in PM < 2.5 microns and are significantly less soluble, likely because of their association with the mineral constituents. These results may have implications regarding health effects associated with exposure to these particles.     

Particulate carbon measurements in California's San Joaquin Valley

Aerosol carbon sampling methods and biases were evaluated during the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) and Fresno Supersite programs. PM2.5 sampling was conducted using Desert Research Institute (DRI) sequential filter samplers (SFS) from December 1999 through February 2001 at two urban sites (Fresno and Bakersfield), one regional transport site (Angiola), and two boundary sites (Bethel Island and Sierra Nevada Foothills) during CRPAQS in the San Joaquin Valley (SJV). Additional filter-based sampling was done in Fresno as part of the US Environmental Protection Agency (EPA) Supersites program. Organic carbon (OC) and elemental carbon (EC) concentrations were higher during winter (December-February) than summer (June-August) and this trend was most pronounced at Fresno and Bakersfield. OC and EC displayed similar diurnal trends during winter and summer at Fresno and during winter at Angiola. The diurnal pattern at Angiola reflected the transport of secondary pollutants to the site. Collocated measurements of OC and EC on undenuded quartz-fiber filters were made at Fresno with the DRI SFS and the Andersen FRM and RAAS samplers. All average differences in OC between samplers were less than their respective measurement uncertainties. Positive and negative OC biases were evaluated at Fresno using the Andersen RAAS sampler with carbon-denuded and undenuded channels with Teflon-membrane and quartz-fiber filter pairs. Differences between the denuded particle OC and that obtained by subtracting the quartz-behind-Teflon or quartz-behind-quartz OC from the undenuded quartz-fiber front filter were less than twice their measurement uncertainties in most cases. Particulate OC in the denuded channel agreed most closely with the difference between undenuded front and backup quartz-fiber OC.     

PM2.5 assessment in 21 European study centers of ECRHS II: Method and first winter results

The follow-up of a cohort of adults from 29 European centers of the former European Community Respiratory Health Survey (ECRHS) I (1989-1992) will examine the long-term effects of exposure to ambient air pollution on the incidence, course, and prognosis of respiratory diseases, in particular asthma and decline in lung function. The purpose of this article is to describe the methodology and the European-wide quality control program for the collection of particles with 50% cut-off size of 2.5 microm aerodynamic diameter (PM2.5) in the ECRHS II and to present the PM2.5 results from the winter period 2000-2001. Because PM2.5 is not routinely monitored in Europe, we measured PM2.5 mass concentrations in 21 participating centers to estimate background exposure in these cities. A standardized protocol was developed using identical equipment in each center (U.S. Environmental Protection Agency Well Impactor Ninety-Six [WINS] and PQ167 from BGI, Inc.). Filters were weighed in a single central laboratory. Sampling was conducted for 7 days per month for a year. Winter mean PM2.5 mass concentrations (November 2000-February 2001) varied substantially, with Iceland reporting the lowest value (5 microg/m3) and northern Italy the highest (69 microg/m3). A standardized procedure appropriate for PM2.5 exposure assessment in a multicenter study was developed. We expect ECRHS II to have sufficient variation in exposure to assess long-term effects of air pollution in this cohort. Any bias caused by variation in the characteristics of the chosen monitoring location (e.g., proximity to traffic sources) will be addressed in later analyses. Given the homogenous spatial distribution of PM2.5, however, concentrations measured near traffic are not expected to differ substantially from those measured at urban background sites.     

Source identifications of airborne fine particles using positive matrix factorization and U.S. Environmental Protection Agency positive matrix factorization

The widely used source apportionment model, positive matrix factorization (PMF2), has been applied to various air pollution data. Recently, U.S. Environmental Protection Agency (EPA) developed EPA positive matrix factorization (PMF), a version of PMF that will be freely distributed by EPA. The objectives of this study were to conduct source apportionment studies for particulate matter less than 2.5 microm in aerodynamic diameter (PM(2.5)) speciation data using PMF2 and EPA PMF (version 1.1) and to compare identified sources between the two models. In the present study, ambient PM(2.5) compositional datasets of 24-hr integrated samples collected at EPA Speciation Trends Network monitoring sites in Chicago, IL, and Portland, OR, were analyzed. Both PMF2 and EPA PMF extracted eight sources for the Chicago data and 10 sources for the Portland data. The model-resolved source profiles were similar between two models for both datasets. However, in several sources, the average contributions did not agree well and the time series contributions were not highly correlated. The differences between PMF2 and EPA PMF solutions were caused by the different least-square algorithm and the different nonnegativity constraints. Most of the average source contributions resolved by both models were within 5-95% uncertainty provided by EPA PMF, indicating that the sources resolved by both models were reproducible.     

Particulate matter,nitrogen oxides,ozone, and select volatile organic compounds during a winter sampling period in Logan,Utah, USA

Particulate matter mass (PM), trace gaseous pollutants, and select volatile organic compounds (VOCs) with meteorological variables were measured in Logan, Utah (Cache Valley), for >4 weeks during winter 2017 as part of the Utah Winter Fine Particle Study (UWFPS). Higher PM levels for short time periods and lower ozone (O₃) levels were present due to meteorological and mountain valley conditions. Nitrogenous pollutants were relatively strongly correlated with PM variables. Diurnal cycles of NO_x, O₃, and fine PM(PM 2.5) (aerodynamic diameter <2.5 μm [PM_2.5]) suggested formation from NO_x. O₃ levels increased from early morning into midafternoon, and NO_x and PM_2.5 increased throughout the morning, followed by sharp decreases. Toluene/benzene and xylenes/benzene ratios and VOC correlations with nitrogenous and PM species were indicative of local traffic sources. Wind sector comparisons suggested that pollutant levels were lower when winds were from nearby mountains to the east versus winds from northerly or southerly origins.

Implications: The Cache Valley in Idaho and Utah has been designated a PM_2.5 nonattainment area that has been attributed to air pollution buildup during winter stagnation events. To inform state implementation plans for PM_2.5 in Cache Valley and other PM_2.5 nonattainment areas in Utah, a state and multiagency federal research effort known as the UWFPS was conducted in winter 2017. As part of the UWFPS, the U.S. Environmental Protection Agency (EPA) measured ground-based PM species and their precursors, VOCs, and meteorology in Logan, Utah. Results reported here from the EPA study in Logan provide additional understanding of wintertime air pollution conditions and possible sources of PM and gaseous pollutants as well as being useful for future PM control strategies in this area.     

Source apportionment of PM10 and PM2.5 in five Chilean cities using factor analysis

Chile is a fast-growing country with important industrial activities near urban areas. In this study, the mass and elemental concentrations of PM10 and PM2.5 were measured in five major Chilean urban areas. Samples of particles with diameter less than 10 microm (PM10) and 2.5 microm (PM2.5) were collected in 1998 in Iquique (northern Chile), Valparaiso, Vi?a del Mar, Rancagua (central Chile), and Temuco (southern Chile). Both PM10 and PM2.5 annual mean concentrations (PM10: 56.9-77.6 microg/m3; PM2.5: 22.4-42.6 microg/m3) were significantly higher than the corresponding European Union (EU) and U.S. Environmental Protection Agency (EPA) air quality standards. Moreover, the 24-hr PM10 and PM2.5 U.S. standards were exceeded infrequently for some of the cities (Rancagua and Valparaiso). Elements ranging from Mg to Pb were detected in the aerosol samples using X-ray fluorescence (XRF). For each of the five cities, factor analysis (FA) was applied to identify and quantify the sources of PM10 and PM2.5. The agreement between calculated and measured mass and elemental concentrations was excellent in most of the cities. Both natural and anthropogenic sources were resolved for all five cities. Soil and sea were the most important contributors to coarse particles (PM10-PM2.5), whereas their contributions to PM2.5 were negligible. Emissions from Cu smelters and oil refineries (and/or diesel combustion) were identified as important sources of PM2.5, particularly in the industrial cities of Rancagua, Valparaiso, and Vi?a del Mar. Finally, motor vehicles and wood burning were significant sources of both PM2.5 and PM10 in most of the cities (wood burning was not identified in Iquique).     

Design of a cost-effective weighing facility for PM2.5 quality assurance

The U.S. Environmental Protection Agency (EPA) Quality Assurance (QA) Guidance Document 2.12: Monitoring PM2.5 in Ambient Air Using Designated Reference or Class I Equivalent Methods (Document 2.12) requires conditioning of PM2.5 filters at 20-23 degrees C and 30-40% relative humidity (RH) for 24 hr prior to gravimetric analysis. Variability of temperature and humidity may not exceed +/-2 degrees C and +/-5% RH during the conditioning period. The quality assurance team at EPA Region 2's regional laboratory designed a PM2.5 weighing facility that operates well within these strict performance requirements. The traditional approach to meeting the performance requirements of Document 2.12 for PM2.5 filter analysis is to build a walk-in room, with costs typically exceeding $100,000. The initial one-time capital cost for the laboratory at EPA's Edison, NJ, facility was approximately $24,000. Annual costs [e.g., National Institute of Standards and Technology (NIST) recertifications and nitrogen replacement cylinders used for humidity control] are approximately $500. The average 24-hr variabilities in temperature and RH in the Region 2 weighing chamber are small, +/-0.2 degrees C and +/-0.8% RH, respectively. The mass detection limit for the PM2.5 weighing system of 47-mm stretched Teflon (lab blank) filters is 6.3 microg. This facility demonstrates an effective and economical example for states and other organizations planning PM2.5 weighing facilities.     

Using continuous PM2.5 monitoring data to report an air quality index

As stated in 40 CFR 58, Appendix G (2000), statistical linear regression models can be applied to relate PM2.5 continuous monitoring (CM) measurements with federal reference method (FRM) measurements, collocated or otherwise, for the purpose of reporting the air quality index (AQI). The CM measurements can then be transformed via the model to remove any bias relative to FRM measurements. The resulting FRM-like modeled measurements may be used to provide more timely reporting of a metropolitan statistical area's (MSA's) AQI. Of considerable importance is the quality of the model used to relate the CM and FRM measurements. The use of a poor model could result in misleading AQI reporting in the form of incorrectly claiming either good or bad air quality. This paper describes a measure of adequacy for deciding whether a statistical linear regression model that relates FRM and continuous PM2.5 measurements is sufficient for use in AQI reporting. The approach is the U.S. Environmental Protection Agency's (EPA's) data quality objectives (DQO) process, a seven-step strategic planning approach to determine the most appropriate data type, quality, quantity, and synthesis for a given activity. The chosen measure of model adequacy is r2, the square of the correlation coefficient between FRM measurements and their modeled counterparts. The paper concludes by developing regression models that meet this desired level of adequacy for the MSAs of Greensboro/Winston-Salem/High Point, NC; and Davenport/Moline/Rock Island, IA/IL. In both cases, a log transformation of the data appeared most appropriate. For the data from the Greensboro/Winston-Salem/High Point MSA, a simple linear regression model of the FRM and CM measurements had an r2 of 0.96, based on 227 paired observations. For the data from the Davenport/Moline/Rock Island MSA, due to seasonal differences between CM and FRM measurements, the simple linear regression model had to be expanded to include a temperature dependency, resulting in an r2 of 0.86, based on 214 paired observations.     

The relationship between real-time and time-integrated coarse (2.5-10 micrm), intermodal (1-2.5 microm), and fine (<2.5 microm) particulate matter in the Los Angeles basin

A periodic review of the National Ambient Air Quality Standards for Particulate Matter by the U.S. Environmental Protection Agency (EPA) will assess the standards with respect to levels, particle size, and averaging times. Some members of the scientific community in the United States and Europe have suggested the use of PM1 instead of PM2.5 as the fine particle measurement standard. This proposed standard is intended to reduce the influence of coarse particle sources on PM2.5, because some evidence suggests that PM1-2.5 is dominated by coarse particulate matter (PM) sources. In this study, coarse (PM2.5-10), intermodal (PM1-2.5), and fine (PM2.5) mass concentrations at four different sites are measured with continuous and time-integrated sampling devices. The main objective is to compare variations in these three size ranges while considering the effects of location, sources, weather, wind speed, and wind direction. Results show strong correlations between PM1 and intermodal PM in receptor sites. The contribution of PM1-2.5 to PM2.5 is highest in the summer months, most likely due to enhanced long-range transport. Coarse PM is poorly correlated with intermodal PM. Continuous data suggest that PM1 is growing into PM1-2.5 via complex processes involving stagnation of the aerosol during high relative humidity conditions, followed by advection during daytime hours.     

Calibration of sharp cut impactors for indoor and outdoor particle sampling

A low-flow rate, sharp cut point inertial impaction sampler was developed in 1986 that has been widely used in PM exposure studies in the United States and several other countries. Although sold commercially as the MS&T Area Sampler, this sampler is widely referred to as the Harvard Impactor, since the initial use was at the Harvard School of Public Health. Impactor nozzles for this sampler have been designed and characterized for flows of 4, 10, 20, and 23 L/min and cut points of 1, 2, 5, and 10 microns. An improved method for determining the actual collecting efficiency curve was developed and used for the recent impactor calibrations reported here. It consists of placing a multiplet reduction impactor inline just downstream of the vibrating orifice aerosol generator to remove the multiplets, thus allowing only the singlet particle s to penetrate through to the impactor being calibrated This paper documents the techniques and results of recent nozzle calibrations for this sampler and compares it with other size-selective inertial impactors. In general, the impactors were found to have sharp cutoff characteristics. Particle interstage losses for all of the impactors were very low, with the exception of the 10-micron cut size 20 L/min impactor, which had greater losses due to the higher flow rate. All of the 2.5-micron cut nozzle laboratory calibrations compare favorably to the U.S. Environmental Protection Agency (EPA) WINS-96 fine particle mass (PM2.5) impactor calibration data.     

Particulate matter in California: part 1--Intercomparison of several PM2.5, PM10-2.5, and PM10 monitoring networks

It will be many years before the recently deployed network of fine particulate matter with an aerodynamic diameter less than 2.5 microm (PM2.5) Federal Reference Method (FRM) samplers produces information on nonattainment areas, trends, and source impacts. However, data on PM2.5 and its major constituents have been routinely collected in California for the past 20 years. The California Air Resources Board operated as many as 20 dichotomous (dichot) samplers for PM2.5 and coarse PM (PM10-2.5). The California Acid Deposition Monitoring Program (CADMP) collected 12-h-average PM2.5 and PM10 from 1988 to 1995 at ten urban and rural sites and 24-h-average PM2.5 at five urban sites since 1995. Beginning in 1994, the Children's Health Study collected 2-week averages of PM2.5 in 12 communities in southern California using the Two-Week Sampler (TWS). Comparisons of collocated samples establish relationships between the dichot, CADMP, and TWS samplers and the 82-site network of PM2.5 FRM samplers deployed since 1999 in California. PM mass data from the different monitoring programs have modest to high correlation to FRM mass data, fairly small systematic biases and negative proportional biases ranging from 7 to 22%. If the biases are taken into account, all of the programs should be considered comparable with the FRM program. Thus, historical data can be used to develop long-term PM trends in California.     

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.     

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.