Source Apportionment of Fine Particulate Matter in the Southeastern United States

Abstract

Particulate matter (PM) less than 2.5 μm in size (PM_2.5)source apportionment by chemical mass balance receptor modeling was performed to enhance regional characterization of source impacts in the southeastern United States. Secondary particles, such as NH₄HSO₄, (NH₄)₂SO₄,NH₄NO₃, and secondary organic carbon (OC) (SOC), formed by atmospheric photochemical reactions, contribute the majority (<50%) of ambient PM_2.5 with strong seasonality. Source apportionment results indicate that motor vehicle and biomass burning are the two main primary sources in the southeast, showing relatively more motor vehicle source impacts rather than biomass burning source impacts in populated urban areas and vice versa in less urbanized areas. Spatial distributions of primary source impacts show that each primary source has distinctively different spatial source impacts. Results also find impacts from shipping activities along the coast. Spatiotemporal correlations indicate that secondary particles are more regionally distributed, as are biomass burning and dust, whereas impacts of other primary sources are more local.     

Source Profiles of Particulate Matter Emissions from a Pilot-Scale Boiler Burning North American Coal Blends

ABSTRACT

Recent awareness of suspected adverse health effects from ambient particulate matter (PM) emission has prompted publication of new standards for fine PM with aerodynamic diameter less than 2.5 μm (PM_2.5). However, scientific data on fine PM emissions from various point sources and their characteristics are very limited. Source apportionment methods are applied to identify contributions of individual regional sources to tropospheric particulate concentrations. The existing industrial database developed using traditional source measurement techniques provides total emission rates only, with no details on chemical nature or size characteristics of particulates. This database is inadequate, in current form, to address source-receptor relationships.

A source dilution system was developed for sampling and characterization of total PM, PM_2.5, and PM₁₀ (i.e., PM with aerodynamic diameter less than 10 μm) from residual oil and coal combustion. This new system has automatic control capabilities for key parameters, such as relative humidity (RH), temperature, and sample dilution. During optimization of the prototype equipment, three North American coal blends were burned using a 0.7-megawatt thermal (MW_t) pulverized coal-fired, pilot-scale boiler. Characteristic emission profiles, including PM_2.5 and total PM soluble acids, and elemental and carbon concentrations for three coal blends are presented.     

Source Apportionment of Ambient Total Suspended Particulates and Coarse Particulate Matter in Urban Areas of Jiaozuo,China

Abstract

Approximately 750 total suspended particulates (TSPs) and coarse particulate matter (PM₁₀) filter samples from six urban sites and a background site and >210 source samples were collected in Jiaozuo City during January 2002 to April 2003. They were analyzed for mass and abundances of 25 chemical components. Seven contributive sources were identified, and their contributions to ambient TSP/PM₁₀ levels at the seven sites in three seasons (spring, summer, and winter days) and a “whole” year were estimated by a chemical mass balance (CMB) receptor model. The spatial TSP average was high in spring and winter days at a level of approximately 530 ～g/m³ and low in summer days at 456 ～g/m³; however, the spatial PM₁₀ average exhibited little variation at a level of approximately 325 ～g/m³, and PM_10-to-TSP ratios ranged from 0.58 to 0.81, which suggested heavy particulate matter pollution existing in the urban areas. Apportionment results indicated that geological material was the largest contributor to ambient TSP/PM₁₀ concentrations, followed by dust emissions from construction activities, coal combustion, secondary aerosols, vehicle movement, and other industrial sources. In addition, paved road dust and re-entrained dust were also apportioned to the seven source types and found soil, coal combustion, and construction dust to be the major contributors.     

Monitoring and Source Apportionment of Particulate Matter near a Large Phosphorus Production Facility

ABSTRACT

A source apportionment study was conducted to identify sources within a large elemental phosphorus plant that contribute to exceedances of the National Ambient Air Quality Standards (NAAQS) for 24-hr PM₁₀. Ambient data were collected at three monitoring sites from October 1996 through July 1999, and included the following: 24-hr PM₁₀ mass, 24-hr PM_2.5 and PM_10–2.5 mass and chemistry, continuous PM₁₀and PM_2.5 mass, continuous meteorological data, and wind-direction-resolved PM_2.5 and PM₁₀ mass and chemistry. Ambient-based receptor modeling and wind-directional analysis were employed to help identify major sources or source locations and source contributions. Fine-fraction phosphate was the dominant species observed during PM₁₀ exceedances, though in general, re-suspended coarse dusts from raw and processed materials at the plant were also needed to create an exceedance. Major sources that were identified included the calciners, the CO flares, process-related dust, and electric-arc furnace operations.     

Comparison and Evaluation of Chemically Speciated Mobile Source PM2.5 Particulate Matter Profiles

ABSTRACT

Mobile sources are significant contributors to ambient PM_{2 5}, accounting for 50% or more of the total observed levels in some locations. One of the important methods for resolving the mobile source contribution is through chemical mass balance (CMB) receptor modeling. CMB requires chemically speciated source profiles with known uncertainty to ensure accurate source contribution estimates. Mobile source PM profiles are available from various sources and are generally in the form of weight fraction by chemical species. The weight fraction format is commonly used, since it is required for input into the CMB receptor model. This paper examines the similarities and differences in mobile source PM_2.5 profiles that contain data for elements, ions, elemental carbon (EC) and organic carbon (OC), and in some cases speciated organics (e.g., polycyclic aromatic hydrocarbons [PAHs]), drawn from four different sources.

Notable characteristics of the mass fraction data include variability (relative contributions of elements and ions) among supposedly similar sources and a wide range of average EC:OC ratios (0.60 ± 0.53 to 1.42 ± 2.99) for light-duty gasoline vehicles (LDGVs), indicating significant EC emissions from LDGVs in some cases. For diesel vehicles, average EC:OC ratios range from 1.09 ± 2.66 to 3.54 ± 3.07. That different populations of the same class of emitters can show considerable variability suggests caution should be exercised when selecting and using profiles in source apportionment studies.     

Source Apportionment of Particulate Matter (PM10) and Indoor Dust in a University Building

A study on source apportionment of indoor dust and particulate matter (PM₁₀) composition was conducted in a university building by using chemometrics. The objective of this study was to investigate the potential sources of selected heavy metals and ionic species in PM₁₀ and indoor dust. PM₁₀ samples were collected using a low-volume sampler (LVS) and indoor dust was collected using a soft brush. Inductively coupled plasma spectrometry (ICP-MS) was used to determine the concentration of heavy metals, while the concentration of cations and anions was determined by atomic absorption spectrometer (AAS) and ion chromatography (IC), respectively. The concentration of PM₁₀ recorded in the building throughout the sampling period ranged from 20 ± 10 μgm^?3 to 80 ± 33 μgm^?3. The composition of heavy metals in PM₁₀ and indoor dust were dominated by zinc (Zn), followed by lead (Pb), copper (Cu), and cadmium (Cd). Principle component analysis (PCA) and multiple linear regression (MLR) showed that the main sources of pollutants in PM₁₀ came from indoor renovations (73.83%), vehicle emissions (16.38%), earth crust sources (9.68%), and other outdoor sources (0.11%). For indoor dust, the pollutant source was mainly earth crust. This study suggests that chemometrics can be used for forensic investigation to determine the possible sources of indoor contaminants within a public building.     

Receptor Oriented Methods of Air Particulate Source Apportionment

Receptor models have evolved rapidly over the past 13 years but have just recently been recognized as a distinct discipline. The general category of receptor models includes both microscopic and chemical methods of apportioning source contributions to ambient air particulates. The number and variations of these methods have grown rapidly over the past few years and include such methods as automated scanning electron microscopy, chemical mass balance and multivariate procedures. These methods as well as hybrid procedures such as target transformation factor analysis, are reviewed and their boundary conditions, strengths, and weaknesses discussed.     

On-Road Motor Vehicle Emissions and Fuel Consumption in Urban Driving Conditions

ABSTRACT

This paper reports on the analysis of on-road vehicle speed, emission, and fuel consumption data collected by four instrumented vehicles. Time-, distance-, and fuel-based average fuel consumption, as well as CO, HC, NO_x, and soot emission factors, were derived. The influences of instantaneous vehicle speed on emissions and fuel consumption were studied. It was found that the fuel-based emission factors varied much less than the time- and distance-based emission factors as instantaneous speed changed. The trends are similar to the results obtained from laboratory tests. The low driving speed contributed to a significant portion of the total emissions over a trip. Furthermore, the on-road data were analyzed using the modal approach. The four standard driving modes are acceleration, cruising, deceleration, and idling. It was found that the transient driving modes (i.e., acceleration and deceleration) were more polluting than the steady-speed driving modes (i.e., cruising and idling) in terms of g/km and g/ sec. These results indicated that the on-road emission measurement is feasible in deriving vehicle emissions and fuel consumption factors in urban driving conditions.     

Light-Duty Motor Vehicle Exhaust Particulate Matter Measurement in the Denver,Colorado, Area

ABSTRACT

A study of particulate matter (PM) emissions from in-use, light-duty vehicles was conducted during the summer of 1996 and the winter of 1997 in the Denver, CO, region. Vehicles were tested as received on chassis dynamometers on the Federal Test Procedure Urban Dynamometer Driving Schedule (UDDS) and the IM240 driving schedule. Both PM10 and regulated emissions were measured for each phase of the UDDS. For the summer portion of the study, 92 gasoline vehicles, 10 diesel vehicles, and 9 gasoline vehicles with visible smoke emissions were tested once. For the winter, 56 gasoline vehicles, 12 diesel vehicles, and 15 gasoline vehicles with visible smoke were tested twice, once indoors at 60 °F and once outdoors at the prevailing temperature. Vehicle model year ranged from 1966 to 1996. Impactor particle size distributions were obtained on a subset of vehicles. Continuous estimates of the particle number emissions were obtained with an electrical aerosol analyzer. This data set is being provided to the Northern Front Range Air Quality Study program and to the State of Colorado and the U.S. Environmental Protection Agency for use in updating emissions inventories.     

A Constant-Volume Rapid Exhaust Dilution System for Motor Vehicle Particulate Matter Number and Mass Measurements

Abstract

An improved version of the constant volume sampling (CVS) methodology that overcomes a number of obstacles that exist with the current CVS dilution tunnel system used in most diesel and gasoline vehicle emissions test facilities is presented. The key feature of the new sampling system is the introduction of dilution air immediately at the vehicle tailpipe. In the present implementation, this is done concentrically through a cylindrical air filter. Elimination of the transfer hose conventionally used to connect the tailpipe to the dilution tunnel significantly reduces the hydrocarbon and particulate matter (PM) storage release artifacts that can lead to wildly incorrect particle number counts and to erroneous filter-collected PM mass. It provides accurate representations of particle size distributions for diesel vehicles by avoiding the particle coagulation that occurs in the transfer hose. Furthermore, it removes the variable delay time that otherwise exists between the time that emissions exit the tailpipe and when they are detected in the dilution tunnel. The performance of the improved CVS system is examined with respect to diesel, gasoline, and compressed natural gas vehicles.     

Status of Control of Motor Vehicle Emissions in California

The State of California, because of an acute air pollution problem has been forced to move ahead on a pioneer basis to control motor vehicle emissions. The Golden State’s program, as put into operation by the Motor Vehicle Pollution Control Board, is discussed in detail. Inspection-installation stations, enforcement and legal requirements relating to crankcase control devices and other facets of the program are presented. Of particular importance is the experience gained by the Board in requiring devices on all new vehicles registered in California and its used vehicle program, affecting vehicles back to the 1950 model year. Recent developments in exhaust control, anticipated installation requirements, and scheduling, as well as an indication of staff long-term planning is also outlined. California’s program is based on the principle that the motor vehicle must be controlled and that sewage no longer can be dumped into the air, if the public health is to be preserved.     

Fugitive Dust Emission Source Profiles and Assessment of Selected Control Strategies for Particulate Matter at Gravel Processing Sites in Taiwan

Abstract

Particles emitted from gravel processing sites are one contributor to worsening air quality in Taiwan. Major pollution sources at gravel processing sites include gravel and sand piles, unpaved roads, material crushers, and bare ground. This study analyzed fugitive dust emission characteristics at each pollution source using several types of particle samplers, including total suspended particulates (TSP), suspended particulate (PM₁₀), fine suspended particulate (PM_2.5), particulate sizer, and dust-fall collectors. Furthermore, silt content and moisture in the gravel were measured to develop particulate emission factors. The results showed that TSP (<100 µm) concentrations at the boundary of gravel sites ranged from 280 to 1290 µg/m³, which clearly exceeds the Taiwan hourly air quality standard of 500 µg/m³. Moreover, PM₁₀ concentrations, ranging from 135 to 550 µg/m³, were also above the daily air quality standard of 125 µg/m³ and approximately 1.2 and 1.5 times the PM_2.5 concentrations, ranging from 105 to 470 µg/m³. The size distribution analysis reveals that mass mean diameter and geometric standard deviation ranged from 3.2 to 5.7 µm and from 2.82 to 5.51, respectively. In this study, spraying surfactant was the most effective control strategy to abate windblown dust from unpaved roads, having a control efficiency of approximately 93%, which is significantly higher than using paved road strategies with a control efficiency of approximately 45%. For paved roads, wet suppression provided the best dust control efficiencies ranging from 50 to 83%. Re-vegetation of disturbed ground had dust control efficiencies ranging from 48 to 64%.     

Fine Particulate Matter Emissions Inventories: Comparisons of Emissions Estimates with Observations from Recent Field Programs

Abstract

Emissions inventories of fine particulate matter (PM_2.5) were compared with estimates of emissions based on data emerging from U.S. Environment Protection Agency Particulate Matter Supersites and other field programs. Six source categories for PM_2.5 emissions were reviewed: on-road mobile sources, nonroad mobile sources, cooking, biomass combustion, fugitive dust, and stationary sources. Ammonia emissions from all of the source categories were also examined. Regional emissions inventories of PM in the exhaust from on-road and nonroad sources were generally consistent with ambient observations, though uncertainties in some emission factors were twice as large as the emission factors. In contrast, emissions inventories of road dust were up to an order of magnitude larger than ambient observations, and estimated brake wear and tire dust emissions were half as large as ambient observations in urban areas. Although comprehensive nationwide emissions inventories of PM_2.5 from cooking sources and biomass burning are not yet available, observational data in urban areas suggest that cooking sources account for approximately 5–20% of total primary emissions (excluding dust), and biomass burning sources are highly dependent on region. Finally, relatively few observational data were available to assess the accuracy of emission estimates for stationary sources. Overall, the uncertainties in primary emissions for PM_2.5 are substantial. Similar uncertainties exist for ammonia emissions. Because of these uncertainties, the design of PM_2.5 control strategies should be based on inventories that have been refined by a combination of bottom-up and top-down methods.     

Defining the Photochemical Contribution to Particulate Matter in Urban Areas Using Time-Series Analysis

Abstract

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 μm 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 μg/m³ (3.03%) in Chicago to 3.9 μg/m³ (7.65%) in Phoenix.     

Sensitivity Analysis and Evaluation of MicroFacCO: A Microscale Motor Vehicle Emission Factor Model for CO Emissions

ABSTRACT

This paper presents a sensitivity analysis of a microscale emission factor model (MicroFacCO) for predicting realtime site-specific motor vehicle CO emissions to input variables, as well as a limited field study evaluation of the model. The sensitivity analysis has shown that MicroFacCO emission estimates are very sensitive to vehicle fleet composition, speed, and ambient temperature. For the present U.S. traffic fleet, the CO emission rate (g/mi) is increased by more than 500% at 5 mph in comparison with a speed greater than 40 mph and by ~67% at ambient temperatures of 45 °F and ≥95 °F in comparison with an ambient temperature of 75 °F.     

Characterization of Particulate Matter and Gaseous Emissions of a C-130H Aircraft

Abstract

The gaseous and nonvolatile particulate matter (PM) emissions of two T56-A-15 turboprop engines of a C-130H aircraft stationed at the 123rd Airlift Wing in the Kentucky Air National Guard were characterized. The emissions campaign supports the Strategic Environmental Research and Development Program (SERDP) project WP-1401 to determine emissions factors from military aircraft. The purpose of the project is to develop a comprehensive emissions measurement program using both conventional and advanced techniques to determine emissions factors of pollutants, and to investigate the spatial and temporal evolutions of the exhaust plumes from fixed and rotating wing military aircraft. Standard practices for the measurement of gaseous emissions from aircraft have been well established; however, there is no certified methodology for the measurement of aircraft PM emissions. In this study, several conventional instruments were used to physically characterize and quantify the PM emissions from the two turboprop engines. Emissions samples were extracted from the engine exit plane and transported to the analytical instrumentation via heated lines. Multiple sampling probes were used to assess the spatial variation and obtain a representative average of the engine emissions. Particle concentrations, size distributions, and mass emissions were measured using commercially available aerosol instruments. Engine smoke numbers were determined using established Society of Automotive Engineers (SAE) practices, and gaseous species were quantified via a Fourier-transform infrared-based gas analyzer. The engines were tested at five power settings, from idle to take-off power, to cover a wide range of operating conditions. Average corrected particle numbers (PNs) of (6.4–14.3) × 10⁷ particles per cm³ and PN emission indices (EI) from 3.5 × 10¹⁵ to 10.0 × 10¹⁵ particles per kg-fuel were observed. The highest PN EI were observed for the idle power conditions. The mean particle diameter varied between 50 nm at idle to 70 nm at maximum engine power. PM mass EI ranged from 1.6 to 3.5 g/kg-fuel for the conditions tested, which are in agreement with previous T56 engine measurements using other techniques. Additional PM data, smoke numbers, and gaseous emissions will be presented and discussed.     

Daily Variability of Motor Vehicle Emissions Derived from Traffic Counter Data

ABSTRACT

This work studied the daily variability of mobile sources in rural and urban areas, in and around the Atlanta Metropolitan Area. Traffic counter data collected during the 1992 Southern Oxidants Study Atlanta Intensive Study were used to analyze the spatial and temporal distribution of traffic volume. A simple method to study the daily variability of mobile emissions from the different types of urban and rural roads is presented. The method is based on hourly traffic volume data and emission factors and it has been generalized to describe the daily variability of mobile emissions for urban and rural areas and for the whole modeling domain. Implications of this study for improving mobile emission inventories are also discussed.     

An Integrated Modeling System for the Estimation of Motor Vehicle Emissions

ABSTRACT

The paper provides a summary of accomplished and ongoing activities in the field of motor vehicle emission modeling in Europe. These activities have led to the development of a system of methods and conesponding computer models that address all the issues related to motor vehicle emissions that are of interest to policy-makers, institutions, and the automotive and oil industries. The Coordination of Information on Air Emissions/Computer Program to Calculate Emissions from Road Traffic (CORLNAIR/COPERT) methodology for the estimation of emissions from road vehicles is presented and compared with other models. A COPERT-based approach for microscale traffic emission estimation, with direct application in regional and urban emission inventories, is outlined, and relevant case studies are briefly discussed. The FOREMOVE model, developed for forecasts of motor vehicle emissions, is presented, together with some results from its application in the European Auto/Oil program. Particular attention is given to modeling the deterioration of in-use vehicles. Finally, the major areas of further research in the field of vehicle emissions in Europe are indicated.     

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.