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.     

Real-world vehicle emissions: a summary of the Eleventh Coordinating Research Council On-Road Vehicle Emissions Workshop

The Coordinating Research Council (CRC) held its eleventh workshop in March 2001, focusing on results from the most recent real-world vehicle emissions research. We summarize the presentations from researchers engaged in improving our understanding of the contribution of mobile sources to ambient air quality and emission inventories. Participants in the workshop discussed efforts to improve mobile source emission models and emission inventories, the role of on-board diagnostic (OBD) systems in inspection and maintenance (I/M) programs, particulate matter (PM) emissions, contributions of diesel vehicles to the emission inventory, on-road emissions measurements, fuel effects, unregulated emissions, and microscale and modal emission models, as well as topics for future research.     

Methods of characterizing the distribution of exhaust emissions from light-duty, gasoline-powered motor vehicles in the U.S. fleet

Mobile sources significantly contribute to ambient concentrations of airborne particulate matter (PM). Source apportionment studies for PM10 (PM < or = 10 microm in aerodynamic diameter) and PM2.5 (PM < or = 2.5 microm in aerodynamic diameter) indicate that mobile sources can be responsible for over half of the ambient PM measured in an urban area. Recent source apportionment studies attempted to differentiate between contributions from gasoline and diesel motor vehicle combustion. Several source apportionment studies conducted in the United States suggested that gasoline combustion from mobile sources contributed more to ambient PM than diesel combustion. However, existing emission inventories for the United States indicated that diesels contribute more than gasoline vehicles to ambient PM concentrations. A comprehensive testing program was initiated in the Kansas City metropolitan area to measure PM emissions in the light-duty, gasoline-powered, on-road mobile source fleet to provide data for PM inventory and emissions modeling. The vehicle recruitment design produced a sample that could represent the regional fleet, and by extension, the national fleet. All vehicles were recruited from a stratified sample on the basis of vehicle class (car, truck) and model-year group. The pool of available vehicles was drawn primarily from a sample of vehicle owners designed to represent the selected demographic and geographic characteristics of the Kansas City population. Emissions testing utilized a portable, light-duty chassis dynamometer with vehicles tested using the LA-92 driving cycle, on-board emissions measurement systems, and remote sensing devices. Particulate mass emissions were the focus of the study, with continuous and integrated samples collected. In addition, sample analyses included criteria gases (carbon monoxide, carbon dioxide, nitric oxide/nitrogen dioxide, hydrocarbons), air toxics (speciated volatile organic compounds), and PM constituents (elemental/organic carbon, metals, semi-volatile organic compounds). Results indicated that PM emissions from the in-use fleet varied by up to 3 orders of magnitude, with emissions generally increasing for older model-year vehicles. The study also identified a strong influence of ambient temperature on vehicle PM mass emissions, with rates increasing with decreasing temperatures.     

Trends,temporal and spatial characteristics,and uncertainties in biomass burning emissions in the Pearl River Delta,China

Multi-year inventories of biomass burning emissions were established in the Pearl River Delta (PRD) region for the period 2003–2007 based on the collected activity data and emission factors. The results indicated that emissions of sulfur dioxide (SO₂), nitrogen oxide (NO_x), ammonia (NH₃), methane (CH₄), organic carbon (OC), non-methane volatile organic compounds (NMVOC), carbon monoxide (CO), and fine particulate matter (PM_2.5) presented clear declining trends. Domestic biofuel burning was the major contributor, accounting for more than 60% of the total emissions. The preliminary temporal profiles were established with MODIS fire count information, showing that higher emissions were observed in winter (from November to March) than other seasons. The emissions were spatially allocated into grid cells with a resolution of 3 km × 3  km, using GIS-based land use data as spatial surrogates. Large amount of emissions were observed mostly in the less developed areas in the PRD region. The uncertainties in biomass burning emission estimates were quantified using Monte Carlo simulation; the results showed that there were higher uncertainties in organic carbon (OC) and elemental carbon (EC) emission estimates, ranging from ?71% to 133% and ?70% to 128%, and relatively lower uncertainties in SO₂, NO_x and CO emission estimates. The key uncertainty sources of the developed inventory included emission factors and parameters used for estimating biomass burning amounts.     

Real-world vehicle emissions: a summary of the 14th coordinating research council on-road Vehicle Emissions Workshop

The Coordinating Research Council held its 14th Vehicle Emissions Workshop in March 2004, where results of the most recent on-road vehicle emissions research were presented. We summarize ongoing work from researchers who are engaged in improving our understanding of the contribution of mobile sources to ambient air quality and emission inventories. Participants in the workshop discussed efforts to improve mobile source emission models, light- and heavy-duty vehicle emissions measurements, on- and off-road emissions measurements, effects of fuels and lubricating oils on emissions, as well as topics for future research.     

Real-world vehicle emissions: a summary of the Seventeenth Coordinating Research Council On-Road Vehicle Emissions Workshop

The Coordinating Research Council, Inc. (CRC) held its 17th On-Road Vehicle Emissions Workshop in March 2007, where results of the most recent on-road vehicle emissions research were presented. We summarize ongoing work from researchers who are engaged in improving our understanding of the role and contribution of mobile sources to ambient air quality and emission inventories. Participants in the Workshop discussed efforts to improve mobile source emission models, light- and heavy-duty vehicle emissions measurements, on- and off-road emissions measurements, effects of fuels and lubricating oils on emissions, as well as emerging issues and topics for future research.     

Real-world vehicle emissions: a summary of the Thirteenth Coordinating Research Council On-Road Vehicle Emissions Workshop

The Coordinating Research Council held its thirteenth Vehicle Emissions Workshop in April 2003, when results of the most recent on-road vehicle emissions research were presented. Ongoing work from researchers who are engaged in improving understanding of the contribution of mobile sources to ambient air quality and emission inventories is summarized here. Participants in the workshop discussed efforts to improve mobile source emission models, the role of on-board diagnostic systems in inspection and maintenance programs, light- and heavy-duty vehicle emissions measurements, on- and off-road emissions measurements, effects of fuels and lubricating oils on emissions, as well as topics for future research.     

A fuel-based assessment of off-road diesel engine emissions

The use of diesel engines in off-road applications is a significant source of nitrogen oxides (NOx) and particulate matter (PM10). Such off-road applications include railroad locomotives, marine vessels, and equipment used for agriculture, construction, logging, and mining. Emissions from these sources are only beginning to be controlled. Due to the large number of these engines and their wide range of applications, total activity and emissions from these sources are uncertain. A method for estimating the emissions from off-road diesel engines based on the quantity of diesel fuel consumed is presented. Emission factors are normalized by fuel consumption, and total activity is estimated by the total fuel consumed. Total exhaust emissions from off-road diesel equipment (excluding locomotives and marine vessels) in the United States during 1996 have been estimated to be 1.2 x 10(9) kg NOx and 1.2 x 10(8) kg PM10. Emissions estimates published by the U.S. Environmental Protection Agency are 2.3 times higher for both NOx and exhaust PM10 emissions than estimates based directly on fuel consumption. These emissions estimates disagree mainly due to differences in activity estimates, rather than to differences in the emission factors. All current emission inventories for off-road engines are uncertain because of the limited in-use emissions testing that has been performed on these engines. Regional- and state-level breakdowns in diesel fuel consumption by off-road mobile sources are also presented. Taken together with on-road measurements of diesel engine emissions, results of this study suggest that in 1996, off-road diesel equipment (including agriculture, construction, logging, and mining equipment, but not locomotives or marine vessels) was responsible for 10% of mobile source NOx emissions nationally, whereas on-road diesel vehicles contributed 33%.     

Revised estimates of construction activity and emissions: Effects on ozone and elemental carbon concentrations in southern California

Emissions from diesel-powered construction equipment are an important source of nitrogen oxides (NO_x) and particulate matter (PM). A new emission inventory for construction equipment emissions is developed based on surveys of diesel fuel use; the revised inventory is compared to current emission inventories. California's OFFROAD model estimates are 4.5 and 3.1 times greater, for NO_x and PM respectively, than the fuel-based estimates developed here. The most relevant uncertainties are the overall amount of construction activity/diesel fuel use, exhaust emission factors for PM and NO_x, and the spatial allocation of emissions to county level and finer spatial scales. Construction permit data were used in this study to estimate spatial distributions of emissions; the resulting distribution is well correlated with population growth. An air quality model was used to assess the impacts of revised emission estimates. Increases of up to 15 ppb in predicted peak ozone concentrations were found in southern California. Elemental carbon and fine particle mass concentrations were in better agreement with observations using revised emission estimates, whereas negative bias in predictions of ambient NO_x concentrations increased.     

Resolving the interactions between population density and air pollution emissions controls in the San Joaquin Valley, USA

The effectiveness of emissions control programs designed to reduce concentrations of airborne particulate matter with an aerodynamic diameter < 2.5 microm (PM2.5) in California's San Joaquin Valley was studied in the year 2030 under three growth scenarios: low, medium, and high population density. Base-case inventories for each choice of population density were created using a coupled emissions modeling system that simultaneously considered interactions between land use and transportation, area source, and point source emissions. The ambient PM2.5 response to each combination of population density and emissions control was evaluated using a regional chemical transport model over a 3-week winter stagnation episode. Comparisons between scenarios were based on regional average and population-weighted PM2.5 concentrations. In the absence of any emissions control program, population-weighted concentrations of PM2.5 in the future San Joaquin Valley are lowest undergrowth scenarios that emphasize low population density. A complete ban on wood burning and a 90% reduction in emissions from food cooking operations and diesel engines must occur before medium- to high-density growth scenarios result in lower population-weighted concentrations of PM2.5. These trends partly reflect the fact that existing downtown urban cores that naturally act as anchor points for new high-density growth in the San Joaquin Valley are located close to major transportation corridors for goods movement. Adding growth buffers around transportation corridors had little impact in the current analysis, since the 8-km resolution of the chemical transport model already provided an artificial buffer around major emissions sources. Assuming that future emissions controls will greatly reduce or eliminate emissions from residential wood burning, food cooking, and diesel engines, the 2030 growth scenario using "as-planned" (medium) population density achieves the lowest population-weighted average PM2.5 concentration in the future San Joaquin Valley during a severe winter stagnation event. Implications: The San Joaquin Valley is one of the most heavily polluted air basins in the United States that are projected to experience strong population growth in the coming decades. The best plan to improve air quality in the region combines medium- or high-density population growth with rigorous emissions controls. In the absences of controls, high-density growth leads to increased population exposure to PM2.5 compared with low-density growth scenarios (urban sprawl).     

NO2 and SO2 dispersion modeling and relative roles of emission sources over Map Ta Phut industrial area, Thailand

Map Ta Phut industrial area (MA) is the largest industrial complex in Thailand. There has been concern about many air pollutants over this area. Air quality management for the area is known to be difficult, due to lack of understanding of how emissions from different sources or sectors (e.g., industrial, power plant, transportation, and residential) contribute to air quality degradation in the area. In this study, a dispersion study of NO2 and SO2 was conducted using the AERMOD model. The area-specific emission inventories of NOx and SO2 were prepared, including both stack and nonstack sources, and divided into 11 emission groups. Annual simulations were performed for the year 2006. Modeled concentrations were evaluated with observations. Underestimation of both pollutants was Jbund, and stack emission estimates were scaled to improve the modeled results before quantifying relative roles of individual emission groups to ambient concentration overfour selected impacted areas (two are residential and the others are highly industrialized). Two concentration measures (i.e., annual average area-wide concentration or AC, and area-wide robust highest concentration or AR) were used to aggregately represent mean and high-end concentrations Jbfor each individual area, respectively. For AC-NO2, on-road mobile emissions were found to be the largest contributor in the two residential areas (36-38% of total AC-NO2), while petrochemical-industry emissions play the most important role in the two industrialized areas (34-51%). For AR-NO2, biomass burning has the most influence in all impacted areas (>90%) exceptJor one residential area where on-road mobile is the largest (75%). For AC-SO2, the petrochemical industry contributes most in all impacted areas (38-56%). For AR-SO2, the results vary. Since the petrochemical industry was often identified as the major contributor despite not being the largest emitter, air quality workers should pay special attention to this emission group when managing air quality for the MA.     

Particulate emissions from U.S. Department of Defense artillery backblast testing

There is a dearth of information on dust emissions from sources that are unique to the U.S. Department of Defense testing and training activities. However, accurate emissions factors are needed for these sources so that military installations can prepare accurate particulate matter (PM) emission inventories. One such source, coarse and fine PM (PM10 and PM2.5) emissions from artillery backblast testing on improved gun positions, was characterized at the Yuma Proving Ground near Yuma, AZ, in October 2005. Fugitive emissions are created by the shockwave from artillery pieces, which ejects dust from the surface on which the artillery is resting. Other contributions of PM can be attributed to the combustion of the propellants. For a 155-mm howitzer firing a range of propellant charges or zones, amounts of emitted PM10 ranged from -19 g of PM10 per firing event for a zone 1 charge to 92 g of PM10 per firing event for a zone 5. The corresponding rates for PM2.5 were approximately 9 g of PM2.5 and 49 g of PM2.5 per firing. The average measured emission rates for PM1o and PM2.5 appear to scale with the zone charge value. The measurements show that the estimated annual contributions of PM10 (52.2 t) and PM2.5 (28.5 t) from artillery backblast are insignificant in the context of the 2002 U.S. Environment Protection Agency (EPA) PM emission inventory. Using national-level activity data for artillery fire, the most conservative estimate is that backblast would contribute the equivalent of 5 x 10(-4) % and 1.6 x 10(-3)% of the annual total PM10 and PM2.5 fugitive dust contributions, respectively, based on 2002 EPA inventory data.     

PM2.5 source apportionment: reconciling receptor models for U.S. nonurban and urban long-term networks

Chemical mass balance (CMB) and trajectory receptor models were applied to speciated particulate matter with aerodynamic diameter < or =2.5 microm (PM2.5) measurements from Speciation Trends Network (STN; part of the Chemical Speciation Network [CSN]) and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring network across the state of Minnesota as part of the Minnesota PM2.5 Source Apportionment Study (MPSAS). CMB equations were solved by the Unmix, positive matrix factorization (PMF), and effective variance (EV) methods, giving collective source contribution and uncertainty estimates. Geological source profiles developed from local dust materials were either incorporated into the EV-CMB model or used to verify factors derived from Unmix and PMF. Common sources include soil dust, calcium (Ca)-rich dust, diesel and gasoline vehicle exhausts, biomass burning, secondary sulfate, and secondary nitrate. Secondary sulfate and nitrate aerosols dominate PM2.5 mass (50-69%). Mobile sources outweigh area sources at urban sites, and vice versa at rural sites due to traffic emissions. Gasoline and diesel contributions can be separated using data from the STN, despite significant uncertainties. Major differences between MPSAS and earlier studies on similar environments appear to be the type and magnitude of stationary sources, but these sources are generally minor (<7%) in this and other studies. Ensemble back-trajectory analysis shows that the lower Midwestern states are the predominant source region for secondary ammoniated sulfate in Minnesota. It also suggests substantial contributions of biomass burning and soil dust from out-of-state on occasions, although a quantitative separation of local and regional contributions was not achieved in the current study. Supplemental materials are available for this article. Go to the publisher's online edition of the Journal of the Air & Waste Management Association for a summary of input data, Unmix and PMF factor profiles, and additional maps.     

Development of a PM2 5 Emissions Inventory for the South Coast Air Basin

ABSTRACT

With the promulgation of a national PM_2.5 ambient air quality standard, it is important that PM_2.5 emissions inventories be developed as a tool for understanding the magnitude of potential PM2.5 violations. Current PM₁₀ inventories include only emissions of primary particulate matter (1 ^ï PM), whereas, based on ambient measurements, both PM₁₀ and PM2.5 emissions inventories will need to include sources of both 1^ï PM and secondary particulate matter (2^ï PM). Furthermore, the U. S. Environmental Protection Agency’s (EPA) current edition of AP-42 includes size distribution data for 1o PM that overestimate the PM_2.5 fraction of fugitive dust sources by at least a factor of 2 based on recent studies.

This paper presents a PM_2.5 emissions inventory developed for the South Coast Air Basin (SCAB) that for the first time includes both 1^ï PM and 2^ï PM. The former is calculated by multiplying PM₁₀ emissions estimates by the PM_2.5/PM₁₀ ratios for different sources. The latter is calculated from estimated emission rates of gas-phase aerosol precursor and gas to aerosol conversion rates consistent with the measured chemical composition of ambient PM_2.5 concentrations observed in the SCAB. The major finding of this PM_2.5 emissions inventory is that the ^2ï aerosol component is more than twice the ^1ï aerosol component, which may result in widely different control strategies being required for fine PM and coarse PM.     

NO2 and SO2dispersion modeling and relative roles of emission sources over Map Ta Phut industrial area,Thailand

Map Ta Phut industrial area (MA) is the largest industrial complex in Thailand. There has been concern about many air pollutants over this area. Air quality management for the area is known to be difficult, due to lack of understanding of how emissions from different sources or sectors (e.g., industrial, power plant, transportation, and residential) contribute to air quality degradation in the area. In this study, a dispersion study of NO₂ and SO₂ was conducted using the AERMOD model. The area-specific emission inventories of NO_x and SO₂ were prepared, including both stack and nonstack sources, and divided into 11 emission groups. Annual simulations were performed for the year 2006. Modeled concentrations were evaluated with observations. Underestimation of both pollutants was found, and stack emission estimates were scaled to improve the modeled results before quantifying relative roles of individual emission groups to ambient concentration over four selected impacted areas (two are residential and the others are highly industrialized). Two concentration measures (i.e., annual average area-wide concentration or AC, and area-wide robust highest concentration or AR) were used to aggregately represent mean and high-end concentrations for each individual area, respectively. For AC-NO₂, on-road mobile emissions were found to be the largest contributor in the two residential areas (36–38% of total AC-NO₂), while petrochemical-industry emissions play the most important role in the two industrialized areas (34–51%). For AR-NO₂, biomass burning has the most influence in all impacted areas (>90%) except for one residential area where on-road mobile is the largest (75%). For AC-SO₂, the petrochemical industry contributes most in all impacted areas (38–56%). For AR-SO₂, the results vary. Since the petrochemical industry was often identified as the major contributor despite not being the largest emitter, air quality workers should pay special attention to this emission group when managing air quality for the MA.

Implications: Effective air quality management in Map Ta Phut Industrial Area, Thailand requires better understanding of how emissions from various sources contribute to the degradation of ambient air quality. Based on the dispersion study here, petrochemical industry was generally identified as the major contributor to ambient NO₂ and SO₂. By accounting for all stack and non-stack sources, on-road mobile emissions were found to be important in some particular areas.     

Effects of improved spatial and temporal modeling of on-road vehicle emissions

Numerous emission and air quality modeling studies have suggested the need to accurately characterize the spatial and temporal variations in on-road vehicle emissions. The purpose of this study was to quantify the impact that using detailed traffic activity data has on emission estimates used to model air quality impacts. The on-road vehicle emissions are estimated by multiplying the vehicle miles traveled (VMT) by the fleet-average emission factors determined by road link and hour of day. Changes in the fraction of VMT from heavy-duty diesel vehicles (HDDVs) can have a significant impact on estimated fleet-average emissions because the emission factors for HDDV nitrogen oxides (NOx) and particulate matter (PM) are much higher than those for light-duty gas vehicles (LDGVs). Through detailed road link-level on-road vehicle emission modeling, this work investigated two scenarios for better characterizing mobile source emissions: (1) improved spatial and temporal variation of vehicle type fractions, and (2) use of Motor Vehicle Emission Simulator (MOVES2010) instead of MOBILE6 exhaust emission factors. Emissions were estimated for the Detroit and Atlanta metropolitan areas for summer and winter episodes. The VMT mix scenario demonstrated the importance of better characterizing HDDV activity by time of day, day of week, and road type. More HDDV activity occurs on restricted access road types on weekdays and at nonpeak times, compared to light-duty vehicles, resulting in 5-15% higher NOx and PM emission rates during the weekdays and 15-40% lower rates on weekend days. Use of MOVES2010 exhaust emission factors resulted in increases of more than 50% in NOx and PM for both HDDVs and LDGVs, relative to MOBILE6. Because LDGV PM emissions have been shown to increase with lower temperatures, the most dramatic increase from MOBILE6 to MOVES2010 emission rates occurred for PM2.5 from LDGVs that increased 500% during colder wintertime conditions found in Detroit, the northernmost city modeled.     

Combustion aerosols: factors governing their size and composition and implications to human health

Particulate matter (PM) emissions from stationary combustion sources burning coal, fuel oil, biomass, and waste, and PM from internal combustion (IC) engines burning gasoline and diesel, are a significant source of primary particles smaller than 2.5 microns (PM2.5) in urban areas. Combustion-generated particles are generally smaller than geologically produced dust and have unique chemical composition and morphology. The fundamental processes affecting formation of combustion PM and the emission characteristics of important applications are reviewed. Particles containing transition metals, ultrafine particles, and soot are emphasized because these types of particles have been studied extensively, and their emissions are controlled by the fuel composition and the oxidant-temperature-mixing history from the flame to the stack. There is a need for better integration of the combustion, air pollution control, atmospheric chemistry, and inhalation health research communities. Epidemiology has demonstrated that susceptible individuals are being harmed by ambient PM. Particle surface area, number of ultrafine particles, bioavailable transition metals, polycyclic aromatic hydrocarbons (PAH), and other particle-bound organic compounds are suspected to be more important than particle mass in determining the effects of air pollution. Time- and size-resolved PM measurements are needed for testing mechanistic toxicological hypotheses, for characterizing the relationship between combustion operating conditions and transient emissions, and for source apportionment studies to develop air quality plans. Citations are provided to more specialized reviews, and the concluding comments make suggestions for further research.     

Source apportionment of fine particles in Tennessee using a source-oriented model

Source apportionment of fine particles (PM2.5, particulate matter < 2 microm in aerodynamic diameter) is important to identify the source categories that are responsible for the concentrations observed at a particular receptor. Although receptor models have been used to do source apportionment, they do not fully take into account the chemical reactions (including photochemical reactions) involved in the formation of secondary fine particles. Secondary fine particles are formed from photochemical and other reactions involving precursor gases, such as sulfur dioxide, oxides of nitrogen, ammonia, and volatile organic compounds. This paper presents the results of modeling work aimed at developing a source apportionment of primary and secondary PM2.5. On-road mobile source and point source inventories for the state of Tennessee were estimated and compiled. The national emissions inventory for the year 1999 was used for the other states. U.S. Environmental Protection Agency Models3/Community Multi-Scale Air Quality modeling system was used for the photochemical/secondary particulate matter modeling. The modeling domain consisted of a nested 36-12-4-km domain. The 4-km domain covered the entire state of Tennessee. The episode chosen for the modeling runs was August 29 to September 9, 1999. This paper presents the approach used and the results from the modeling and attempts to quantify the contribution of major source categories, such as the on-road mobile sources (including the fugitive dust component) and coal-fired power plants, to observed PM2.5 concentrations in Tennessee. The results of this work will be helpful in policy issues targeted at designing control strategies to meet the PM2.5 National Ambient Air Quality Standards in Tennessee.     

Combustion Aerosols: Factors Governing Their Size and Composition and Implications to Human Health

ABSTRACT

Particulate matter (PM) emissions from stationary combustion sources burning coal, fuel oil, biomass, and waste, and PM from internal combustion (IC) engines burning gasoline and diesel, are a significant source of primary particles smaller than 2.5 μm (PM_2.5) in urban areas. Combustion-generated particles are generally smaller than geologically produced dust and have unique chemical composition and morphology. The fundamental processes affecting formation of combustion PM and the emission characteristics of important applications are reviewed. Particles containing transition metals, ultrafine particles, and soot are emphasized because these types of particles have been studied extensively, and their emissions are controlled by the fuel composition and the oxidant-tem-perature-mixing history from the flame to the stack. There is a need for better integration of the combustion, air pollution control, atmospheric chemistry, and inhalation health research communities. Epidemiology has demonstrated that susceptible individuals are being harmed by ambient PM. Particle surface area, number of ultrafine particles, bioavailable transition metals, polycyclic aromatic hydrocarbons (PAH), and other particle-bound organic compounds are suspected to be more important than particle mass in determining the effects of air pollution. Time- and size-resolved PM measurements are needed for testing mechanistic toxicological hypotheses, for characterizing the relationship between combustion operating conditions and transient emissions, and for source apportionment studies to develop air quality plans. Citations are provided to more specialized reviews, and the concluding comments make suggestions for further research.     

Source contributions to primary organic aerosol: Comparison of the results of a source-resolved model and the chemical mass balance approach

A source-resolved model has been developed to predict the contribution of different sources to primary organic aerosol concentrations. The model was applied to the eastern US during a 17 day pollution episode beginning on 12 July 2001. Primary organic matter (OM) and elemental carbon (EC) concentrations are tracked for eight different sources: gasoline vehicles, non-road diesel vehicles, on-road diesel vehicles, biomass burning, wood burning, natural gas combustion, road dust, and all other sources. Individual emission inventories are developed for each source and a three-dimensional chemical transport model (PMCAMx) is used to predict the primary OM and EC concentrations from each source. The source-resolved model is simple to implement and is faster than existing source-oriented models. The results of the source-resolved model are compared to the results of chemical mass balance models (CMB) for Pittsburgh and multiple urban/rural sites from the Southeastern Aerosol Research and Characterization (SEARCH) network. Significant discrepancies exist between the source-resolved model and the CMB model predictions for some of the sources. There is strong evidence that the organic PM emissions from natural gas combustion are overestimated. It also appears that the OM and EC emissions from wood burning and off-road diesel are too high in the Northeastern US. Other similarities and discrepancies between the source-resolved model and the CMB model for primary OM and EC are discussed along with problems in the current emission inventory for certain sources.