Source Apportionment of Phoenix PM2.5 Aerosol with the Unmix Receptor Model

Abstract

The multivariate receptor model Unmix has been used to analyze a 3-yr PM_2.5 ambient aerosol data set collected in Phoenix, AZ, beginning in 1995. The analysis generated source profiles and overall average percentage source contribution estimates (SCEs) for five source categories: gasoline engines (33 ± 4%), diesel engines (16 ± 2%), secondary SO₄ ^2? (19 ± 2%), crustal/soil (22 ± 2%), and vegetative burning (10 ± 2%). The Unmix analysis was supplemented with scanning electron microscopy (SEM) of a limited number of filter samples for information on possible additional low-strength sources. Except for the diesel engine source category, the Unmix SCEs were generally consistent with an earlier multivariate receptor analysis of essentially the same data using the Positive Matrix Factorization (PMF) model. This article provides the first demonstration for an urban area of the capability of the Unmix receptor model.     

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.     

Comparison of source apportionments of fine particulate matter at two San Jose speciation trends network sites

In this study, the chemical composition of fine particulate matter samples collected at U.S. Environmental Protection Agency Speciation Trends Network sites in San Jose, CA, from February 2000 to February 2005 were analyzed. A San Jose site was initially established at 4th Street and then subsequently moved to Jackson Street in mid-2002. These sites are approximately 1 km apart. There were no known major changes in the nature of the sources in the area over this period. The study used positive matrix factorization model to extract the source profiles and their mass contributions and to compare the results for the congruence of the source apportionments between these two nearby sites. In the case of the 4th Street site, the average mass was apportioned to wood combustion (32.1 +/- 2.5%), secondary nitrate (22.3 +/- 2%), secondary sulfate (10.7 +/- 0.6%), fresh sea salt (7.7 +/- 0.9%), gasoline vehicles (7.3 +/- 0.5%), aged sea salt (6.8 +/- 0.4%), road dust (6.7 +/- 0.7%), diesel emissions (3.9 +/- 0.3%), and a Ni-related industrial source (2.5 +/- 0.4%). At the Jackson Street site, the average mass was apportioned to wood combustion (33.6 +/- 2.6%), secondary nitrate (20.3 +/- 1.9%), secondary sulfate (13.9 +/- 0.9%), aged sea salt (12.4 +/- 0.7%), gasoline vehicle (8.3 +/- 0.6%), fresh sea salt (5.3 +/- 0.5%), diesel emission (3.2 +/- 0.3%), road dust (1.9 +/- 0.1%), and Ni-related industrial source (1.3 +/- 0.1%). Conditional probability function analysis was used to help identify local sources. These results suggested that moving the sampling site a short distance had little effect on the nature of the resolved source types although some differences in their quantitative impacts were obtained in the positive matrix factorization analyses.     

Source apportionment of daily fine particulate matter at Jefferson Street, Atlanta, GA, during summer and winter

The primary emission source contributions to fine organic carbon (OC) and fine particulate matter (PM2.5) mass concentrations on a daily basis in Atlanta, GA, are quantified for a summer (July 3 to August 4, 2001) and a winter (January 2-31, 2002) month. Thirty-one organic compounds in PM2.5 were identified and quantified by gas chromatography/mass spectrometry. These organic tracers, along with elemental carbon, aluminum, and silicon, were used in a chemical mass balance (CMB) receptor model. CMB source apportionment results revealed that major contributors to identified fine OC concentrations include meat cooking (7-68%; average: 36%), gasoline exhaust (7-45%; average: 21%), and diesel exhaust (6-41%; average: 20%) for the summer month, and wood combustion (0-77%; average: 50%); gasoline exhaust (14-69%; average: 33%), meat cooking (1-14%; average: 5%), and diesel exhaust (0-13%; average: 4%) for the winter month. Primary sources, as well as secondary ions, including sulfate, nitrate, and ammonium, accounted for 86 +/- 13% and 112 +/- 15% of the measured PM2.5 mass in summer and winter, respectively.     

Emissions of PCDD/Fs, PCBs, and PAHs from legacy on-road heavy-duty diesel engines

Exhaust emissions of seventeen 2,3,7,8-substituted polychlorinated dibenzo-p-dioxin/furan (PCDD/F) congeners, tetra-octa PCDD/F homologues, 12 WHO 2005 polychlorinated biphenyl (PCB) congeners, mono-nona chlorinated biphenyl homologues, and 19 polycyclic aromatic hydrocarbons (PAHs) from three legacy diesel engines were investigated. The three engines tested were a 1985 model year GM 6.2 J-series engine, a 1987 model year Detroit Diesel Corporation 6V92 engine, and a 1993 model year Cummins L10 engine. Results were compared to United States’ mobile source inventory for on-road diesel engines, as well as historic and modern diesel engine emission values. The test fuel contained chlorine at 9.8 ppm which is 1.5 orders of magnitude above what is found in current diesel fuel and 3900 ppm sulfur to simulate fuels that would have been available when these engines were produced. Results indicate PCDD/F emissions of 13.1, 7.1, and 13.6 pg International Toxic Equivalency (I-TEQ) L⁻¹ fuel consumed for the three engines respectively, where non-detects are equal to zero. This compares with a United States’ mobile source on-road diesel engine inventory value of 946 pg I-TEQ L⁻¹ fuel consumed and 1.28 pg I-TEQ L⁻¹ fuel consumed for modern engines equipped with a catalyzed diesel particle filter and urea selective catalytic reduction. PCB emissions are 2 orders of magnitude greater than modern diesel engines. PAH results are representative of engines from this era based on historical values and are 3-4 orders of magnitude greater than modern diesel engines.     

Comparison and evaluation of chemically speciated mobile source PM2.5 particulate matter profiles

Mobile sources are significant contributors to ambient PM2.5, 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 PM2.5 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.     

Seasonal variability and source apportionment of metals in the atmospheric deposition in Belgrade

The primary objective of this study is to assess anthropogenic impacts on the environment by determination of element atmospheric depositions. Bulk depositions were collected monthly, from June 2002 to December 2006, at three urban locations in Belgrade. Concentrations of Al, V, Cr, Mn, Fe, Ni, Cu, Zn, Cd and Pb were analyzed by atomic absorption spectrometry and the current deposition fluxes of atmospheric metals were established. Fourier analysis was applied in order to investigate seasonal variation of the monthly data set. Nickel, V, Fe and Al showed pronounced seasonal dependence, while seasonal variation of the other elements was not evident. The enrichment factors of Pb, Zn, Cd and Cu were obviously above those who could have been caused by natural processes, indicating a mainly anthropogenic origin. Nickel was intermediately enriched suggesting participation of both natural and anthropogenic sources. The multivariate receptor model, Unmix, was used to analyze a 5-yr element atmospheric depositions data set. Three main source profiles (mixed road dust, oil combustion and metal processing) were identified and the overall average percentage source contributions determined.     

Emissions of PCDD/Fs,PCBs, and PAHs from legacy on-road heavy-duty diesel engines

Exhaust emissions of seventeen 2,3,7,8-substituted polychlorinated dibenzo-p-dioxin/furan (PCDD/F) congeners, tetra–octa PCDD/F homologues, 12 WHO 2005 polychlorinated biphenyl (PCB) congeners, mono–nona chlorinated biphenyl homologues, and 19 polycyclic aromatic hydrocarbons (PAHs) from three legacy diesel engines were investigated. The three engines tested were a 1985 model year GM 6.2 J-series engine, a 1987 model year Detroit Diesel Corporation 6V92 engine, and a 1993 model year Cummins L10 engine. Results were compared to United States’ mobile source inventory for on-road diesel engines, as well as historic and modern diesel engine emission values. The test fuel contained chlorine at 9.8 ppm which is 1.5 orders of magnitude above what is found in current diesel fuel and 3900 ppm sulfur to simulate fuels that would have been available when these engines were produced. Results indicate PCDD/F emissions of 13.1, 7.1, and 13.6 pg International Toxic Equivalency (I-TEQ) L⁻¹ fuel consumed for the three engines respectively, where non-detects are equal to zero. This compares with a United States’ mobile source on-road diesel engine inventory value of 946 pg I-TEQ L⁻¹ fuel consumed and 1.28 pg I-TEQ L⁻¹ fuel consumed for modern engines equipped with a catalyzed diesel particle filter and urea selective catalytic reduction. PCB emissions are 2 orders of magnitude greater than modern diesel engines. PAH results are representative of engines from this era based on historical values and are 3–4 orders of magnitude greater than modern diesel engines.     

Regulated and unregulated emissions from highway heavy-duty diesel engines complying with U.S. Environmental Protection Agency 2007 emissions standards

As part of the Advanced Collaborative Emissions Study (ACES), regulated and unregulated exhaust emissions from four different 2007 model year U.S. Environmental Protection Agency (EPA)-compliant heavy-duty highway diesel engines were measured on an engine dynamometer. The engines were equipped with exhaust high-efficiency catalyzed diesel particle filters (C-DPFs) that are actively regenerated or cleaned using the engine control module. Regulated emissions of carbon monoxide, nonmethane hydrocarbons, and particulate matter (PM) were on average 97, 89, and 86% lower than the 2007 EPA standard, respectively, and oxides of nitrogen (NOx) were on average 9% lower. Unregulated exhaust emissions of nitrogen dioxide (NO2) emissions were on, average 1.3 and 2.8 times higher than the NO, emissions reported in previous work using 1998- and 2004-technology engines, respectively. However, compared with other work performed on 1994- to 2004-technology engines, average emission reductions in the range of 71-99% were observed for a very comprehensive list of unregulated engine exhaust pollutants and air toxic contaminants that included metals and other elements, elemental carbon (EC), inorganic ions, and gas- and particle-phase volatile and semi-volatile organic carbon (OC) compounds. The low PM mass emitted from the 2007 technology ACES engines was composed mainly of sulfate (53%) and OC (30%), with a small fraction of EC (13%) and metals and other elements (4%). The fraction of EC is expected to remain small, regardless of engine operation, because of the presence of the high-efficiency C-DPF in the exhaust. This is different from typical PM composition of pre-2007 engines with EC in the range of 10-90%, depending on engine operation. Most of the particles emitted from the 2007 engines were mainly volatile nuclei mode in the sub-30-nm size range. An increase in volatile nanoparticles was observed during C-DPF active regeneration, during which the observed particle number was similar to that observed in emissions of pre-2007 engines. However, on average, when combining engine operation with and without active regeneration events, particle number emissions with the 2007 engines were 90% lower than the particle number emitted from a 2004-technology engine tested in an earlier program.     

Source apportionment of fine particles in Washington, DC, utilizing temperature-resolved carbon fractions

Integrated ambient particulate matter < or =2.5 microm in aerodynamic diameter (PM2.5) samples were collected at a centrally located urban monitoring site in Washington, DC, on Wednesdays and Saturdays using Interagency Monitoring of Protected Visual Environments samplers. Particulate carbon was analyzed using the thermal optical reflectance method that divides carbon into four organic carbon fractions, pyrolyzed organic carbon, and three elemental carbon fractions. A total of 35 variables measured in 718 samples collected between August 1988 and December 1997 were analyzed. The data were analyzed using Positive Matrix Factorization and 10 sources were identified: sulfate (SO4(2-))-rich secondary aerosol I (43%), gasoline vehicle (21%), SO4(2-)-rich secondary aerosol II (11%), nitrate-rich secondary aerosol (9%), SO4(2-)-rich secondary aerosol III (6%), incinerator (4%), aged sea salt (2%), airborne soil (2%), diesel emissions (2%), and oil combustion (2%). In contrast to a previous study that included only total organic carbon and elemental carbon fractions, motor vehicles were separated into fractions identified as gasoline vehicle and diesel emissions containing carbon fractions whose abundances were different between the two sources. This study indicates that the temperature-resolved carbon fraction data can be utilized to enhance source apportionment, especially with respect to the separation of diesel emissions from gasoline vehicle sources. Conditional probability functions using surface wind data and deduced source contributions aid in the identifications of local sources.     

Evaluations of the chemical mass balance method for determining contributions of gasoline and diesel exhaust to ambient carbonaceous aerosols

The US. Department of Energy Gasoline/Diesel PM Split Study was conducted to assess the sources of uncertainties in using an organic compound-based chemical mass balance receptor model to quantify the relative contributions of emissions from gasoline (or spark ignition [SI]) and diesel (or compression ignition [CI]) engines to ambient concentrations of fine particulate matter (PM2.5) in California's South Coast Air Basin (SOCAB). In this study, several groups worked cooperatively on source and ambient sample collection and quality assurance aspects of the study but worked independently to perform chemical analysis and source apportionment. Ambient sampling included daily 24-hr PM2.5 samples at two air quality-monitoring stations, several regional urban locations, and along freeway routes and surface streets with varying proportions of automobile and truck traffic. Diesel exhaust was the dominant source of total carbon (TC) and elemental carbon (EC) at the Azusa and downtown Los Angeles, CA, monitoring sites, but samples from the central part of the air basin showed nearly equal apportionments of CI and SI. CI apportionments to TC were mainly dependent on EC, which was sensitive to the analytical method used. Weekday contributions of CI exhaust were higher for Interagency Monitoring of Protected Visual Environments (IMPROVE; 41+/-3.7%) than Speciation Trends Network (32+/-2.4%). EC had little effect on SI apportionment. SI apportionments were most sensitive to higher molecular weight polycyclic aromatic hydrocarbons (indeno[123-cd]pyrene, benzo(ghi)perylene, and coronene) and several steranes and hopanes, which were associated mainly with high emitters. Apportionments were also sensitive to choice of source profiles. CI contributions varied from 30% to 60% of TC when using individual source profiles rather than the composites used in the final apportionments. The apportionment of SI vehicles varied from 1% to 12% of TC depending on the specific profile that was used. Up to 70% of organic carbon (OC) in the ambient samples collected at the two fixed monitoring sites could not be apportioned to directly emitted PM emissions.     

Source apportionment of airborne particulate matter in Southeast Texas using a source-oriented 3D air quality model

A nested version of the source-oriented externally mixed UCD/CIT model was developed to study the source contributions to airborne particulate matter (PM) during a two-week long air quality episode during the Texas 2000 Air Quality Study (TexAQS 2000). Contributions to primary PM and secondary ammonium sulfate in the Houston–Galveston Bay (HGB) and Beaumont–Port Arthur (BPA) areas were determined.The predicted 24-h elemental carbon (EC), organic compounds (OC), sulfate, ammonium ion and primary PM_2.5 mass are in good agreement with filter-based observations. Predicted concentrations of hourly sulfate, ammonium ion, and primary OC from diesel and gasoline engines and biomass burning organic aerosol (BBOA) at La Porte, Texas agree well with measurements from an Aerodyne Aerosol Mass Spectrometer (AMS).The UCD/CIT model predicts that EC is mainly from diesel engines and majority of the primary OC is from internal combustion engines and industrial sources. Open burning contributes large fractions of EC, OC and primary PM_2.5 mass. Road dust, internal combustion engines and industries are the major sources of primary PM_2.5. Wildfire dominates the contributions to all primary PM components in areas near the fires. The predicted source contributions to primary PM are in general agreement with results from a chemical mass balance (CMB) model. Discrepancy between the two models suggests that further investigations on the industrial PM emissions are necessary.Secondary ammonium sulfate accounts for the majority of the secondary inorganic PM. Over 80% of the secondary sulfate in the 4 km domain is produced in upwind areas. Coal combustion is the largest source of sulfate. Ammonium ion is mainly from agriculture sources and contributions from gasoline vehicles are significant in urban areas.     

Regulated and unregulated emissions from modern 2010 emissions-compliant heavy-duty on-highway diesel engines

The U.S. Environmental Protection Agency (EPA) established strict regulations for highway diesel engine exhaust emissions of particulate matter (PM) and nitrogen oxides (NO_x) to aid in meeting the National Ambient Air Quality Standards. The emission standards were phased in with stringent standards for 2007 model year (MY) heavy-duty engines (HDEs), and even more stringent NO_X standards for 2010 and later model years. The Health Effects Institute, in cooperation with the Coordinating Research Council, funded by government and the private sector, designed and conducted a research program, the Advanced Collaborative Emission Study (ACES), with multiple objectives, including detailed characterization of the emissions from both 2007- and 2010-compliant engines. The results from emission testing of 2007-compliant engines have already been reported in a previous publication. This paper reports the emissions testing results for three heavy-duty 2010-compliant engines intended for on-highway use. These engines were equipped with an exhaust diesel oxidation catalyst (DOC), high-efficiency catalyzed diesel particle filter (DPF), urea-based selective catalytic reduction catalyst (SCR), and ammonia slip catalyst (AMOX), and were fueled with ultra-low-sulfur diesel fuel (~6.5 ppm sulfur). Average regulated and unregulated emissions of more than 780 chemical species were characterized in engine exhaust under transient engine operation using the Federal Test Procedure cycle and a 16-hr duty cycle representing a wide dynamic range of real-world engine operation. The 2010 engines’ regulated emissions of PM, NO_X, nonmethane hydrocarbons, and carbon monoxide were all well below the EPA 2010 emission standards. Moreover, the unregulated emissions of polycyclic aromatic hydrocarbons (PAHs), nitroPAHs, hopanes and steranes, alcohols and organic acids, alkanes, carbonyls, dioxins and furans, inorganic ions, metals and elements, elemental carbon, and particle number were substantially (90 to >99%) lower than pre-2007-technology engine emissions, and also substantially (46 to >99%) lower than the 2007-technology engine emissions characterized in the previous study.

Implications:?Heavy-duty on-highway diesel engines equipped with DOC/DPF/SCR/AMOX and fueled with ultra-low-sulfur diesel fuel produced lower emissions than the stringent 2010 emission standards established by the U.S. Environmental Protection Agency. They also resulted in significant reductions in a wide range of unregulated toxic emission compounds relative to older technology engines. The increased use of newer technology (2010+) diesel engines in the on-highway sector and the adaptation of such technology by other sectors such as nonroad, displacing older, higher emissions engines, will have a positive impact on ambient levels of PM, NOx, and volatile organic compounds, in addition to many other toxic compounds.     

Particulate matter in new technology diesel exhaust (NTDE) is quantitatively and qualitatively very different from that found in traditional diesel exhaust (TDE)

Diesel exhaust (DE) characteristic of pre-1988 engines is classified as a "probable" human carcinogen (Group 2A) by the International Agency for Research on Cancer (IARC), and the U.S. Environmental Protection Agency has classified DE as "likely to be carcinogenic to humans." These classifications were based on the large body of health effect studies conducted on DE over the past 30 or so years. However, increasingly stringent U.S. emissions standards (1988-2010) for particulate matter (PM) and nitrogen oxides (NOx) in diesel exhaust have helped stimulate major technological advances in diesel engine technology and diesel fuel/lubricant composition, resulting in the emergence of what has been termed New Technology Diesel Exhaust, or NTDE. NTDE is defined as DE from post-2006 and older retrofit diesel engines that incorporate a variety of technological advancements, including electronic controls, ultra-low-sulfur diesel fuel, oxidation catalysts, and wall-flow diesel particulate filters (DPFs). As discussed in a prior review (T. W. Hesterberg et al.; Environ. Sci. Technol. 2008, 42, 6437-6445), numerous emissions characterization studies have demonstrated marked differences in regulated and unregulated emissions between NTDE and "traditional diesel exhaust" (TDE) from pre-1988 diesel engines. Now there exist even more data demonstrating significant chemical and physical distinctions between the diesel exhaust particulate (DEP) in NTDE versus DEP from pre-2007 diesel technology, and its greater resemblance to particulate emissions from compressed natural gas (CNG) or gasoline engines. Furthermore, preliminary toxicological data suggest that the changes to the physical and chemical composition of NTDE lead to differences in biological responses between NTDE versus TDE exposure. Ongoing studies are expected to address some of the remaining data gaps in the understanding of possible NTDE health effects, but there is now sufficient evidence to conclude that health effects studies of pre-2007 DE likely have little relevance in assessing the potential health risks of NTDE exposures.     

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%.     

Source apportionment of visual impairment during the California regional PM10/PM2.5 air quality study

Gases and particulate matter predictions from the UCD/CIT air quality model were used in a visibility model to predict source contributions to visual impairment in the San Joaquin Valley (SJV), the southern portion of California's Central Valley, during December 2000 and January 2001. Within the SJV, daytime (0800–1700 PST) light extinction was dominated by scattering associated with airborne particles. Measured daytime particle scattering coefficients were compared to predicted values at approximately 40 locations across the SJV after correction for the increased temperature and decreased relative humidity produced by “smart heaters” placed upstream of nephelometers. Mean fractional bias and mean fractional error were ?0.22 and 0.65, respectively, indicating reasonable agreement between model predictions and measurements. Particulate water, nitrate, organic matter, and ammonium were the major particulate species contributing to light scattering in the SJV. Daytime light extinction in the SJV averaged between December 25, 2000 and January 7, 2001 was mainly associated with animal ammonia sources (28%), diesel engines (18%), catalyst gasoline engines (9%), other anthropogenic sources (9%), and wood smoke (7%) with initial and boundary conditions accounting for 13%. The source apportionment results from this study apply to wintertime conditions when airborne particulate matter concentrations are typically at their annual maximum. Further study would be required to quantify source contributions to light extinction in other seasons.     

Evaluation of catalyzed and electrically heated filters for removal of particulate emissions from diesel-A- and JP-8-fueled engines

In-service diesel engines are a significant source of particulate matter (PM) emissions, and they have been subjected to increasingly strict emissions standards. Consequently, the wide-scale use of some type of particulate filter is expected. This study evaluated the effect of an Engelhard catalyzed soot filter (CSF) and a Rypos electrically heated soot filter on the emissions from in-service diesel engines in terms of PM mass, black carbon concentration, particle-bound polycyclic aromatic hydrocarbon concentration, and size distribution. Both filters capture PM. The CSF relies on the engine's exhaust to reach the catalyst regeneration temperature and oxidize soot, whereas the electrically heated filter contains a heating element to oxidize soot. The filters were installed on several military diesel engines. Particle concentrations and compositions were measured before and after installation of the filter and again after several months of operation. Generally, the CSF removed at least 90% of total PM, and the removal efficiency improved or remained constant after several months of operation. In contrast, the electrical filters removed 44-69% of PM mass. In addition to evaluating the soot filters, the sampling team also compared the results of several real-time particle measurement instruments to traditional filter measurements of total mass.     

Emissions of organic compounds and trace metals in fine particulate matter from motor vehicles: a tunnel study in Houston, Texas

Fine particulate matter (PM) samples collected in a highway tunnel in Houston, TX, were analyzed to quantify the concentrations of 14 n-alkanes, 12 polycyclic aromatic hydrocarbons, and nine petroleum biomarkers, as well as 21 metals, with the ultimate aim of identifying appropriate tracers for diesel engines. First, an exploratory multivariate dimensionality reduction technique called principal component analysis (PCA) was employed to identify all potential candidates for tracers. Next, emission indices were calculated to interpret PCA results physically. Emission indices of n-heneicosane, n-docosane, n-tricosane, n-tetracosane, n-pentacosane, fluoranthene, and pyrene were correlated highly and increased strongly with percentage carbon present in the tunnel emanating from diesel vehicles. This suggests that these organic compounds are useful molecular markers to separate emissions from diesel and gasoline engines. Additionally, the results are the first quantification of the metal composition of PM with aerodynamic diameters smaller than 2.5 microm (PM2.5) emissions from mobile sources in Houston. PCA of trace metal concentrations followed by emission index calculations revealed that barium in fine airborne particles can be linked quantitatively to diesel engine emissions, demonstrating its role as an elemental tracer for heavy-duty trucks.     

Size- and density-distributions and sources of polycyclic aromatic hydrocarbons in urban road dust

Polycyclic aromatic hydrocarbons (PAHs) present in size- and density-fractionated road dust were measured to identify the important fractions in urban runoff and to analyse their sources. Road dust was collected from a residential area (Shakujii) and a heavy traffic area (Hongo Street). The sampling of road dust from the residential area was conducted twice in different seasons (autumn and winter). The collected road dust was separated into three or four size-fractions and further fractionated into light (<1.7 g/cm3) and heavy (>1.7 g/cm3) fractions by using cesium chloride solution. Light particles constituted only 4.0+/-1.4%, 0.69+/-0.03% and 3.4+/-1.0% of the road dust by weight for Shakujii (November), Shakujii (February) and Hongo Street, respectively but contained 28+/-10%, 33+/-3% and 44+/-8% of the total PAHs, respectively. The PAH contents in the light fractions were 1-2 orders of magnitude higher than those in the heavy fractions. In the light fractions, the 12PAH contents in February were significantly higher than the 12PAH contents in November (P<0.01), whereas in the heavy fractions, no significant difference was found (P>0.05). Cluster analysis revealed that there was a significant difference in the PAH profiles between locations rather than between size-fractions, density-fractions and sampling times. Multiple regression analysis indicated that asphalt/pavement was the major source of Shakujii road dust, and that tyre and diesel vehicle exhaust were the major sources of finer and coarser fractions collected from Hongo Street road dust, respectively.     

Evaluation of Catalyzed and Electrically Heated Filters for Removal of Particulate Emissions from Diesel-A- and JP-8-Fueled Engines

Abstract

In-service diesel engines are a significant source of particulate matter (PM) emissions, and they have been subjected to increasingly strict emissions standards. Consequently, the wide-scale use of some type of particulate filter is expected. This study evaluated the effect of an Engelhard catalyzed soot filter (CSF) and a Rypos electrically heated soot filter on the emissions from in-service diesel engines in terms of PM mass, black carbon concentration, particle-bound polycyclic aromatic hydrocarbon concentration, and size distribution. Both filters capture PM. The CSF relies on the engine's exhaust to reach the catalyst regeneration temperature and oxidize soot, whereas the electrically heated filter contains a heating element to oxidize soot. The filters were installed on several military diesel engines. Particle concentrations and compositions were measured before and after installation of the filter and again after several months of operation. Generally, the CSF removed at least 90% of total PM, and the removal efficiency improved or remained constant after several months of operation. In contrast, the electrical filters removed 44-69% of PM mass. In addition to evaluating the soot filters, the sampling team also compared the results of several real-time particle measurement instruments to traditional filter measurements of total mass.