On-road and laboratory investigation of low-level PM emissions of a modern diesel particulate filter equipped diesel passenger car

Modern diesel particulate filter (DPF) systems are very effective in reducing particle emissions from diesel vehicles. In this work low-level particulate matter (PM) emissions from a DPF equipped EURO-4 diesel vehicle were studied in the emission test laboratory as well as during real-world chasing on a high-speed test track. Size and time resolved data obtained from an engine exhaust particle sizer (EEPS) and a condensation particle counter (CPC) are presented for both loaded and unloaded DPF condition. The corresponding time and size resolved emission factors were calculated for acceleration, deceleration, steady state driving and during DPF regeneration, and are compared with each other. In addition, the DPF efficiency of the tested vehicle was evaluated during the New European Driving Cycle (NEDC) by real time pre-/post-DPF measurements and was found to be 99.5% with respect to PM number concentration and 99.3% for PM mass, respectively. PM concentrations, which were measured at a distance of about 10 m behind the test car, ranged from 1 to 1.5 times background level when the vehicle was driven on the test track under normal acceleration conditions or at constant speeds below 100 kmh^?1. Only during higher speeds and full load accelerations concentrations above 3 times background level could be observed. The corresponding tests in the emission laboratory confirmed these results. During DPF regeneration the total PM number emission of nucleation mode particles was 3–4 orders of magnitude higher compared to those emitted at the same speed without regeneration, while the level of the accumulation mode particles remained about the same. The majority of the particles emitted during DPF regeneration was found to be volatile, and is suggested to originate from accumulated sulfur compounds.     

Size and composition distributions of particulate matter emissions: part 2--heavy-duty diesel vehicles

Particulate matter (PM) emissions from heavy-duty diesel vehicles (HDDVs) were collected using a chassis dynamometer/dilution sampling system that employed filter-based samplers, cascade impactors, and scanning mobility particle size (SMPS) measurements. Four diesel vehicles with different engine and emission control technologies were tested using the California Air Resources Board Heavy Heavy-Duty Diesel Truck (HHDDT) 5 mode driving cycle. Vehicles were tested using a simulated inertial weight of either 56,000 or 66,000 lb. Exhaust particles were then analyzed for total carbon, elemental carbon (EC), organic matter (OM), and water-soluble ions. HDDV fine (< or =1.8 microm aerodynamic diameter; PM1.8) and ultrafine (0.056-0.1 microm aerodynamic diameter; PM0.1) PM emission rates ranged from 181-581 mg/km and 25-72 mg/km, respectively, with the highest emission rates in both size fractions associated with the oldest vehicle tested. Older diesel vehicles produced fine and ultrafine exhaust particles with higher EC/OM ratios than newer vehicles. Transient modes produced very high EC/OM ratios whereas idle and creep modes produced very low EC/OM ratios. Calcium was the most abundant water-soluble ion with smaller amounts of magnesium, sodium, ammonium ion, and sulfate also detected. Particle mass distributions emitted during the full 5-mode HDDV tests peaked between 100-180 nm and their shapes were not a function of vehicle age. In contrast, particle mass distributions emitted during the idle and creep driving modes from the newest diesel vehicle had a peak diameter of approximately 70 nm, whereas mass distributions emitted from older vehicles had a peak diameter larger than 100 nm for both the idle and creep modes. Increasing inertial loads reduced the OM emissions, causing the residual EC emissions to shift to smaller sizes. The same HDDV tested at 56,000 and 66,000 lb had higher PM0.1 EC emissions (+22%) and lower PM0.1 OM emissions (-38%) at the higher load condition.     

Emission rates and comparative chemical composition from selected in-use diesel and gasoline-fueled vehicles

Emission samples for toxicity testing and detailed chemical characterization were collected from a variety of gasoline- and diesel-fueled in-use vehicles operated on the Unified Driving Cycle on a chassis dynamometer. Gasoline vehicles included normal particle mass (particulate matter [PM]) emitters (tested at 72 and 30 degrees F), "black" and "white" smokers, and a new-technology vehicle (tested at 72 degrees F). Diesel vehicles included current-technology vehicles (tested at 72 and 30 degrees F) and a high PM emitter. Total PM emission rates ranged from below 3 mg/mi up to more than 700 mg/mi for the white smoker gasoline vehicle. Emission rates of organic and elemental carbon (OC/EC), elements (metals and associated analytes), ions, and a variety of particulate and semi-volatile organic compounds (polycyclic aromatic hydrocarbons [PAH], nitro-PAH, oxy-PAH, hopanes, and steranes) are reported for these vehicles. Speciated organic analysis also was conducted on the fuels and lube oils obtained from these vehicles after the emissions testing. The compositions of emissions were highly dependent on the fuel type (gasoline vs. diesel), the state of vehicle maintenance (low, average, or high emitters; white or black smokers), and ambient conditions (i.e., temperature) of the vehicles. Fuel and oil analyses from these vehicles showed that oil served as a repository for combustion byproducts (e.g., PAH), and oil-burning gasoline vehicles emitted PAH in higher concentrations than did other vehicles. These PAH emissions matched the PAH compositions observed in oil.     

Diesel passenger car PM emissions: From Euro 1 to Euro 4 with particle filter

This paper examines the impact of the emission control and fuel technology development on the emissions of gaseous and, in particular, PM pollutants from diesel passenger cars. Three cars in five configurations in total were measured, and covered the range from Euro 1 to Euro 4 standards. The emission control ranged from no aftertreatment in the Euro 1 case, an oxidation catalyst in Euro 2, two oxidation catalysts and exhaust gas recirculation in Euro 3 and Euro 4, while a catalyzed diesel particle filter (DPF) fitted in the Euro 4 car led to a Euro 4 + DPF configuration. Both certification test and real-world driving cycles were employed. The results showed that CO and HC emissions were much lower than the emission standard over the hot-start real-world cycles. However, vehicle technologies from Euro 2 to Euro 4 exceeded the NOx and PM emission levels over at least one real-world cycle. The NOx emission level reached up to 3.6 times the certification level in case of the Euro 4 car. PM were up to 40% and 60% higher than certification level for the Euro 2 and Euro 3 cars, while the Euro 4 car emitted close or slightly below the certification level over the real-world driving cycles. PM mass reductions from Euro 1 to Euro 4 were associated with a relevant decrease in the total particle number, in particular over the certification test. This was not followed by a respective reduction in the solid particle number which remained rather constant between the four technologies at 0.86 × 10¹⁴ km^?1 (coefficient of variation 9%). As a result, the ratio of solid vs. total particle number ranged from ～50% in Euro 1–100% in Euro 4. A significant reduction of more than three orders of magnitude in solid particle number is achieved with the introduction of the DPF. However, the potential for nucleation mode formation at high speed from the DPF car is an issue that needs to be considered in the over all assessment of its environmental benefit. Finally, comparison of the mobility and aerodynamic diameters of airborne particles led to fractal dimensions dropping from 2.60 (Euro 1) to 2.51 (Euro 4), denoting a more loose structure with improving technology.     

Chemical speciation of PM emissions from heavy-duty diesel vehicles equipped with diesel particulate filter (DPF) and selective catalytic reduction (SCR) retrofits

Four heavy-duty diesel vehicles (HDDVs) in six retrofitted configurations (CRT^®, V-SCRT^®, Z-SCRT^®, Horizon, DPX and CCRT^®) and a baseline vehicle operating without after--treatment were tested under cruise (50 mph), transient UDDS and idle driving modes. As a continuation of the work by Biswas et al. [Biswas, S., Hu, S., Verma, V., Herner, J., Robertson, W.J., Ayala, A., Sioutas, C., 2008. Physical properties of particulate matter (PM) from late model heavy-duty diesel vehicles operating with advanced emission control technologies. Atmospheric Environment 42, 5622–5634.] on particle physical parameters, this paper focuses on PM chemical characteristics (Total carbon [TC], Elemental carbon [EC], Organic Carbon [OC], ions and water-soluble organic carbon [WSOC]) for cruise and UDDS cycles only. Size-resolved PM collected by MOUDI–Nano-MOUDI was analyzed for TC, EC and OC and ions (such as sulfate, nitrate, ammonium, potassium, sodium and phosphate), while Teflon coated glass fiber filters from a high volume sampler were extracted to determine WSOC. The introduction of retrofits reduced PM mass emissions over 90% in cruise and 95% in UDDS. Similarly, significant reductions in the emission of major chemical constituents (TC, OC and EC) were achieved. Sulfate dominated PM composition in vehicle configurations (V-SCRT^®-UDDS, Z-SCRT^®-Cruise, CRT^® and DPX) with considerable nucleation mode and TC was predominant for configurations with less (Z-SCRT^®-UDDS) or insignificant (CCRT^®, Horizon) nucleation. The transient operation increases EC emissions, consistent with its higher accumulation PM mode content. In general, solubility of organic carbon is higher (average ～5 times) for retrofitted vehicles than the baseline vehicle. The retrofitted vehicles with catalyzed filters (DPX, CCRT^®) had decreased OC solubility (WSOC/OC: 8–25%) unlike those with uncatalyzed filters (SCRT^®s, Horizon; WSOC/OC ～ 60–100%). Ammonium was present predominantly in the nucleation mode, indicating that ternary nucleation may be the responsible mechanism for formation of these particles.     

Variations in speciated emissions from spark-ignition and compression-ignition motor vehicles in California's south coast air basin

The U.S. Department of Energy Gasoline/Diesel PM Split Study examined the sources of uncertainties in using an organic compound-based chemical mass balance receptor model to quantify the contributions of spark-ignition (SI) and compression-ignition (CI) engine exhaust to ambient fine particulate matter (PM2.5). This paper presents the chemical composition profiles of SI and CI engine exhaust from the vehicle-testing portion of the study. Chemical analysis of source samples consisted of gravimetric mass, elements, ions, organic carbon (OC), and elemental carbon (EC) by the Interagency Monitoring of Protected Visual Environments (IMPROVE) and Speciation Trends Network (STN) thermal/optical methods, polycyclic aromatic hydrocarbons (PAHs), hopanes, steranes, alkanes, and polar organic compounds. More than half of the mass of carbonaceous particles emitted by heavy-duty diesel trucks was EC (IMPROVE) and emissions from SI vehicles contained predominantly OC. Although total carbon (TC) by the IMPROVE and STN protocols agreed well for all of the samples, the STN/IMPROVE ratios for EC from SI exhaust decreased with decreasing sample loading. SI vehicles, whether low or high emitters, emitted greater amounts of high-molecular-weight particulate PAHs (benzo[ghi]perylene, indeno[1,2,3-cd]pyrene, and coronene) than did CI vehicles. Diesel emissions contained higher abundances of two- to four-ring semivolatile PAHs. Diacids were emitted by CI vehicles but are also prevalent in secondary organic aerosols, so they cannot be considered unique tracers. Hopanes and steranes were present in lubricating oil with similar composition for both gasoline and diesel vehicles and were negligible in gasoline or diesel fuels. CI vehicles emitted greater total amounts of hopanes and steranes on a mass per mile basis, but abundances were comparable to SI exhaust normalized to TC emissions within measurement uncertainty. The combustion-produced high-molecular-weight PAHs were found in used gasoline motor oil but not in fresh oil and are negligible in used diesel engine oil. The contributions of lubrication oils to abundances of these PAHs in the exhaust were large in some cases and were variable with the age and consumption rate of the oil. These factors contributed to the observed variations in their abundances to total carbon or PM2.5 among the SI composition profiles.     

Deriving fuel-based emission factor thresholds to interpret heavy-duty vehicle roadside plume measurements

Remote sensing devices have been used for decades to measure gaseous emissions from individual vehicles at the roadside. Systems have also been developed that entrain diluted exhaust and can also measure particulate matter (PM) emissions. In 2015, the California Air Resources Board (CARB) reported that 8% of in-field diesel particulate filters (DPF) on heavy-duty (HD) vehicles were malfunctioning and emitted about 70% of total diesel PM emissions from the DPF-equipped fleet. A new high-emitter problem in the heavy-duty vehicle fleet had emerged. Roadside exhaust plume measurements reflect a snapshot of real-world operation, typically lasting several seconds. In order to relate roadside plume measurements to laboratory emission tests, we analyzed carbon dioxide (CO₂), oxides of nitrogen (NO_X), and PM emissions collected from four HD vehicles during several driving cycles on a chassis dynamometer. We examined the fuel-based emission factors corresponding to possible exceedances of emission standards as a function of vehicle power. Our analysis suggests that a typical HD vehicle will exceed the model year (MY) 2010 emission standards (of 0.2 g NO_X/bhp-hr and 0.01 g PM/bhp-hr) by three times when fuel-based emission factors are 9.3 g NO_X/kg fuel and 0.11 g PM/kg using the roadside plume measurement approach. Reported limits correspond to 99% confidence levels, which were calculated using the detection uncertainty of emissions analyzers, accuracy of vehicle power calculations, and actual emissions variability of fixed operational parameters. The PM threshold was determined for acceleration events between 0.47 and 1.4 mph/sec only, and the NO_X threshold was derived from measurements where after-treatment temperature was above 200°C. Anticipating a growing interest in real-world driving emissions, widespread implementation of roadside exhaust plume measurements as a compliment to in-use vehicle programs may benefit from expanding this analysis to a larger sample of in-use HD vehicles.

Implications: Regulatory agencies, civil society, and the public at large have a growing interest in vehicle emission compliance in the real world. Leveraging roadside plume measurements to identify vehicles with malfunctioning emission control systems is emerging as a viable new and useful method to assess in-use performance. This work proposes fuel-based emission factor thresholds for PM and NOx that signify exceedances of emission standards on a work-specific basis by analyzing real-time emissions in the laboratory. These thresholds could be used to prescreen vehicles before roadside enforcement inspection or other inquiry, enhance and further develop emission inventories, and potentially develop new requirements for heavy-duty inspection and maintenance (I/M) programs, including but not limited to identifying vehicles for further testing.     

Evaluation of solid particle number and black carbon for very low particulate matter emissions standards in light-duty vehicles

To reliably measure at the low particulate matter (PM) levels needed to meet California’s Low Emission Vehicle (LEV III) 3- and 1-mg/mile particulate matter (PM) standards, various approaches other than gravimetric measurement have been suggested for testing purposes. In this work, a feasibility study of solid particle number (SPN, d50 = 23 nm) and black carbon (BC) as alternatives to gravimetric PM mass was conducted, based on the relationship of these two metrics to gravimetric PM mass, as well as the variability of each of these metrics. More than 150 Federal Test Procedure (FTP-75) or Supplemental Federal Test Procedure (US06) tests were conducted on 46 light-duty vehicles, including port-fuel-injected and direct-injected gasoline vehicles, as well as several light-duty diesel vehicles equipped with diesel particle filters (LDD/DPF). For FTP tests, emission variability of gravimetric PM mass was found to be slightly less than that of either SPN or BC, whereas the opposite was observed for US06 tests. Emission variability of PM mass for LDD/DPF was higher than that of both SPN and BC, primarily because of higher PM mass measurement uncertainties (background and precision) near or below 0.1 mg/mile. While strong correlations were observed from both SPN and BC to PM mass, the slopes are dependent on engine technologies and driving cycles, and the proportionality between the metrics can vary over the course of the test. Replacement of the LEV III PM mass emission standard with one other measurement metric may imperil the effectiveness of emission reduction, as a correlation-based relationship may evolve over future technologies for meeting stringent greenhouse standards.

Implications: Solid particle number and black carbon were suggested in place of PM mass for the California LEV III 1-mg/mile FTP standard. Their equivalence, proportionality, and emission variability in comparison to PM mass, based on a large light-duty vehicle fleet examined, are dependent on engine technologies and driving cycles. Such empirical derived correlations exhibit the limitation of using these metrics for enforcement and certification standards as vehicle combustion and after-treatment technologies advance.     

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.     

On-road measurement of fine particle and nitrogen oxide emissions from light- and heavy-duty motor vehicles

An updated assessment of fine particle emissions from light- and heavy-duty vehicles is needed due to recent changes to the composition of gasoline and diesel fuel, more stringent emission standards applying to new vehicles sold in the 1990s, and the adoption of a new ambient air quality standard for fine particulate matter (PM_2.5) in the United States. This paper reports the measurement of emissions from vehicles in a northern California roadway tunnel during summer 1997. Separate measurements were made of uphill traffic in two tunnel bores: one bore carried both light-duty vehicles and heavy-duty diesel trucks, and the second bore was reserved for light-duty vehicles. Ninety-eight percent of the light-duty vehicles were gasoline-powered. In the tunnel, heavy-duty diesel trucks emitted 24, 37, and 21 times more fine particle, black carbon, and sulfate mass per unit mass of fuel burned than light-duty vehicles. Heavy-duty diesel trucks also emitted 15–20 times the number of particles per unit mass of fuel burned compared to light-duty vehicles. Fine particle emissions from both vehicle classes were composed mostly of carbon; diesel-derived particulate matter contained more black carbon (51±11% of PM_2.5 mass) than did light-duty fine particle emissions (33±4%). Sulfate comprised only 2% of total fine particle emissions for both vehicle classes. Sulfate emissions measured in this study for heavy-duty diesel trucks are significantly lower than values reported in earlier studies conducted before the introduction of low-sulfur diesel fuel. This study suggests that heavy-duty diesel vehicles in California are responsible for nearly half of oxides of nitrogen emissions and greater than three-quarters of exhaust fine particle emissions from on-road motor vehicles.     

Temperature effects on particulate emissions from DPF-equipped diesel trucks operating on conventional and biodiesel fuels

Emissions tests were conducted on two medium heavy-duty diesel trucks equipped with a particulate filter (DPF), with one vehicle using a NOx absorber and the other a selective catalytic reduction (SCR) system for control of nitrogen oxides (NOx). Both vehicles were tested with two different fuels (ultra-low-sulfur diesel [ULSD] and biodiesel [B20]) and ambient temperatures (70ºF and 20ºF), while the truck with the NOx absorber was also operated at two loads (a heavy weight and a light weight). The test procedure included three driving cycles, a cold start with low transients (CSLT), the federal heavy-duty urban dynamometer driving schedule (UDDS), and a warm start with low transients (WSLT). Particulate matter (PM) emissions were measured second-by-second using an Aethalometer for black carbon (BC) concentrations and an engine exhaust particle sizer (EEPS) for particle count measurements between 5.6 and 560 nm. The DPF/NOx absorber vehicle experienced increased BC and particle number concentrations during cold starts under cold ambient conditions, with concentrations two to three times higher than under warm starts at higher ambient temperatures. The average particle count for the UDDS showed an opposite trend, with an approximately 27% decrease when ambient temperatures decreased from 70ºF to 20ºF. This vehicle experienced decreased emissions when going from ULSD to B20. The DPF/SCR vehicle tested had much lower emissions, with many of the BC and particle number measurements below detectable limits. However, both vehicles did experience elevated emissions caused by DPF regeneration. All regeneration events occurred during the UDDS cycle. Slight increases in emissions were measured during the WSLT cycles after the regeneration. However, the day after a regeneration occurred, both vehicles showed significant increases in particle number and BC for the CSLT drive cycle, with increases from 93 to 1380% for PM number emissions compared with tests following a day with no regeneration.

Implications:?The use of diesel particulate filters (DPFs) on trucks is becoming more common throughout the world. Understanding how DPFs affect air pollution emissions under varying operating conditions will be critical in implementing effective air quality standards. This study evaluated particulate matter (PM) and black carbon (BC) emissions with two DPF-equipped heavy-duty diesel trucks operating on conventional fuel and a biodiesel fuel blend at varying ambient temperatures, loads, and drive cycles.     

Emissions of gas- and particle-phase polycyclic aromatic hydrocarbons (PAHs) in the Shing Mun Tunnel,Hong Kong

Real-world vehicle emission factors for seventeen gas and particulate polycyclic aromatic hydrocarbons (PAHs) were quantified in the Shing Mun Tunnel, Hong Kong during summer and winter 2003. Naphthalene, acenaphthylene, and acenaphthene were the most abundant gas PAHs while fluoranthene and pyrene were the most abundant in the particle phase. Most (98%) of the gas PAHs consisted of two- and three-aromatic rings whereas most of the particle-phase PAHs were in four- (～60%) and five-ring (～17%) for fresh exhaust emissions. Average emission factors for the gas- and particle PAHs were 950–2564 μg veh^?1 km^?1 and 22–354 μg veh^?1 km^?1, respectively. Good correlations were found between diesel markers (fluoranthene and pyrene; 0.85) and gasoline markers (benzo[ghi]perylene and indeno[1,2,3-cd]pyrene; 0.96). Higher PAH emission factors were associated with a higher fraction of diesel-fueled vehicles (DV) passing through the tunnel. Separate emission factors were determined from diesel and non-diesel exhaust by the regression intercept method. The average PAH emission factor (i.e., sum of gas and particle phases) from DV (3085 ± 1058 μg veh^?1 km^?1) was ～5 times higher than that from non-diesel-fueled vehicles (NDV, 566 ± 428 μg veh^?1 km^?1). Ratios of DV to NDV emission factors were high for diesel markers (>24); and low for gasoline markers (<0.4).     

Development of molecular marker source profiles for emissions from on-road gasoline and diesel vehicle fleets

As part of the Gasoline/Diesel PM Split Study, relatively large fleets of gasoline vehicles and diesel vehicles were tested on a chassis dynamometer to develop chemical source profiles for source attribution of atmospheric particulate matter in California's South Coast Air Basin. Gasoline vehicles were tested in cold-start and warm-start conditions, and diesel vehicles were tested through several driving cycles. Tailpipe emissions of particulate matter were analyzed for organic tracer compounds, including hopanes, steranes, and polycyclic aromatic hydrocarbons. Large intervehicle variation was seen in emission rate and composition, and results were averaged to examine the impacts of vehicle ages, weight classes, and driving cycles on the variation. Average profiles, weighted by mass emission rate, had much lower uncertainty than that associated with intervehicle variation. Mass emission rates and elemental carbon/organic carbon (EC/OC) ratios for gasoline vehicle age classes were influenced most by use of cold-start or warm-start driving cycle (factor of 2-7). Individual smoker vehicles had a large range of mass and EC/OC (factors of 40 and 625, respectively). Gasoline vehicle age averages, data on vehicle ages and miles traveled in the area, and several assumptions about smoker contributions were used to create emissions profiles representative of on-road vehicle fleets in the Los Angeles area in 2001. In the representative gasoline fleet profiles, variation was further reduced, with cold-start or warm-start and the representation of smoker vehicles making a difference of approximately a factor of two in mass emission rate and EC/OC. Diesel vehicle profiles were created on the basis of vehicle age, weight class, and driving cycle. Mass emission rate and EC/OC for diesel averages were influenced by vehicle age (factor of 2-5), weight class (factor of 2-7), and driving cycle (factor of 10-20). Absolute and relative emissions of molecular marker compounds showed levels of variation similar to those of mass and EC/OC.     

Evolution of vehicle exhaust particles in the atmosphere

Aerosol mass spectrometer (AMS) measurements are used to characterize the evolution of exhaust particulate matter (PM) properties near and downwind of vehicle sources. The AMS provides time-resolved chemically speciated mass loadings and mass-weighted size distributions of nonrefractory PM smaller than 1 microm (NRPM1). Source measurements of aircraft PM show that black carbon particles inhibit nucleation by serving as condensation sinks for the volatile and semi-volatile exhaust gases. Real-world source measurements of ground vehicle PM are obtained by deploying an AMS aboard a mobile laboratory. Characteristic features of the exhaust PM chemical composition and size distribution are discussed. PM mass and number concentrations are used with above-background gas-phase carbon dioxide (CO2) concentrations to calculate on-road emission factors for individual vehicles. Highly variable ratios between particle number and mass concentrations are observed for individual vehicles. NRPM1 mass emission factors measured for on-road diesel vehicles are approximately 50% lower than those from dynamometer studies. Factor analysis of AMS data (FA-AMS) is applied for the first time to map variations in exhaust PM mass downwind of a highway. In this study, above-background vehicle PM concentrations are highest close to the highway and decrease by a factor of 2 by 200 m away from the highway. Comparison with the gas-phase CO2 concentrations indicates that these vehicle PM mass gradients are largely driven by dilution. Secondary aerosol species do not show a similar gradient in absolute mass concentrations; thus, their relative contribution to total ambient PM mass concentrations increases as a function of distance from the highway. FA-AMS of single particle and ensemble data at an urban receptor site shows that condensation of these secondary aerosol species onto vehicle exhaust particles results in spatial and temporal evolution of the size and composition of vehicle exhaust PM on urban and regional scales.     

Exhaust Temperature Profiles for Application of Passive Diesel Particulate Filters to Solid Waste Collection Vehicles in California

Abstract

To reduce public exposure to diesel particulate matter (DPM), the California Air Resources Board has begun adoption of a series of rules to reduce these emissions from in-use heavy-duty vehicles. Passive diesel particulate filter (DPF) after-treatment technologies are a cost-effective method to reduce DPM emissions and have been used on a variety of vehicles worldwide. Two passive DPFs were interim-verified in California and approved federally for use in most 1994–2002 engine families for vehicles meeting min engine exhaust temperature requirements for successful filter regeneration. Some vehicles, however, may not be suited to passive DPFs because of lower engine exhaust temperatures. The purpose of this study was to determine the applicability of two types of passive DPFs to solid waste collection vehicles, the group of vehicles for which California recently mandated in-use DPM reductions. We selected 60 collection vehicles to represent the four main types of collection vehicle duty cycles—roll-offs, and front-end, rear, and side loaders—and collected second-by-second engine exhaust temperature readings for one week from each vehicle. As a group, the collection vehicles exhibited low engine exhaust temperatures, making the application of passive DPFs to these vehicles difficult. Only 35% of tested vehicles met the temperature requirements for one passive DPF, whereas 60% met the temperature requirements for the other. Engine exhaust temperatures varied by vehicle type. Side and front-end loaders met the engine exhaust temperature requirements in the greatest number of cases with ～50–90% achieving the required regeneration temperatures. Only 8–25% of the rear loader and roll-off collection vehicles met the engine exhaust temperature requirements. Solid waste collection vehicles represent a diverse fleet with a variety of duty cycles. Low engine exhaust temperatures will need to be addressed for successful use of passive DPFs in this application.     

Size and composition distributions of particulate matter emissions: part 1--light-duty gasoline vehicles

Size-resolved particulate matter (PM) emitted from light-duty gasoline vehicles (LDGVs) was characterized using filter-based samplers, cascade impactors, and scanning mobility particle size measurements in the summer 2002. Thirty LDGVs, with different engine and emissions control technologies (model years 1965-2003; odometer readings 1264-207,104 mi), were tested on a chassis dynamometer using the federal test procedure (FTP), the unified cycle (UC), and the correction cycle (CC). LDGV PM emissions were strongly correlated with vehicle age and emissions control technology. The oldest models had average ultrafine PM0.1 (0.056- to 0.1-microm aerodynamic diameter) and fine PM1.8 (< or =1.8-microm aerodynamic diameter) emission rates of 9.6 mg/km and 213 mg/km, respectively. The newest vehicles had PM0.1 and PM1.8 emissions of 51 microg/km and 371 microg/km, respectively. Light duty trucks and sport utility vehicles had PM0.1 and PM1.8 emissions nearly double the corresponding emission rates from passenger cars. Higher PM emissions were associated with cold starts and hard accelerations. The FTP driving cycle produced the lowest emissions, followed by the UC and the CC. PM mass distributions peaked between 0.1- and 0.18-microm particle diameter for all vehicles except those emitting visible smoke, which peaked between 0.18 and 0.32 microm. The majority of the PM was composed of carbonaceous material, with only trace amounts of water-soluble ions. Elemental carbon (EC) and organic matter (OM) had similar size distributions, but the EC/OM ratio in LDGV exhaust particles was a strong function of the adopted emissions control technology and of vehicle maintenance. Exhaust from LDGV classes with lower PM emissions generally had higher EC/OM ratios. LDGVs adopting newer technologies were characterized by the highest EC/OM ratios, whereas OM dominated PM emissions from older vehicles. Driving cycles with cold starts and hard accelerations produced higher EC/OM ratios in ultrafine particles.     

Contribution of motor vehicle emissions to organic carbon and fine particle mass in Pittsburgh, Pennsylvania: Effects of varying source profiles and seasonal trends in ambient marker concentrations

We present estimates of the vehicular contribution to ambient organic carbon (OC) and fine particle mass (PM) in Pittsburgh, PA using the chemical mass balance (CMB) model and a large dataset of ambient molecular marker concentrations. Source profiles for CMB analysis are selected using a method of comparing the ambient ratios of marker species with published profiles for gasoline and diesel vehicle emissions. The ambient wintertime data cluster on a hopanes/EC ratio–ratio plot, and therefore can be explained by a large number of different source profile combinations. In contrast, the widely varying summer ambient ratios can be explained by a more limited number of source profile combinations. We present results for a number of different CMB scenarios, all of which perform well on the different statistical tests used to establish the quality of a CMB solution. The results illustrate how CMB estimates depend critically on the marker-to-OC and marker-to-PM ratios of the source profiles. The vehicular contribution in the winter is bounded between 13% and 20% of the ambient OC (274±56–416±72 ng-C m⁻³). However, variability in the diesel profiles creates uncertainty in the gasoline–diesel split. On an OC basis, one set of scenarios suggests gasoline dominance, while a second set indicates a more even split. On a PM basis, all solutions indicate a diesel-dominated split. The summer CMB solutions do not present a consistent picture given the seasonal shift and wide variation in the ambient hopanes-to-EC ratios relative to the source profiles. If one set of source profiles is applied to the entire dataset, gasoline vehicles dominate vehicular OC in the winter but diesel dominates in the summer. The seasonal pattern in the ambient hopanes-to-EC ratios may be caused by photochemical decay of hopanes in the summer or by seasonal changes in vehicle emission profiles.     

Morphology and composition of particles emitted from conventional and alternative fuel vehicles

Size, morphology, and composition of airborne particles strongly affect human health and visibility, precipitation, and the kinetic characteristics of particles. In this study, the morphology and chemical composition of particles emitted from conventional (diesel and gasoline) and alternative (CNG and methanol) fuel vehicles were characterized through scanning electron microscopy (SEM) and energy-dispersive X-ray (EDX). The SEM images revealed that the size of primary particles (without agglomeration) was approximately 10 nm in the exhaust from all the tested vehicles. The particles emitted from gasoline vehicle (GV), CNG vehicle (CNGV), and methanol vehicle (MV) had the same median diameter, 62 nm, which was smaller than those from heavy diesel vehicle (HDV) and light diesel vehicle (LDV). Soot was observed in the HDV, LDV, and GV samples but not in the CNGV and MV. The fractal dimension, which was used to quantify the degree of irregularity of soot, was 1.752 ± 0.014, 1.789 ± 0.076, and 1.769 ± 0.006 in the exhaust from HDV, LDV, and GV samples, respectively. The particles discharged by all tested vehicles contained the elements C, O, Fe, and Na. The main element in the samples of HDV, LDV, and GV was C, while O was the main element in the samples of alternative fuel vehicles. The profiles of minor elements were more complex in the emissions of alternative fuel vehicles than those in the emissions of conventional fuel vehicles. The results improved our understanding of the morphology and elemental composition of particles emitted from vehicles powered by diesel, gasoline, CNG, and methanol.

     

Characterization of exhaust particles from military vehicles fueled with diesel,gasoline, and JP-8

Diluted exhaust from selected military aircraft ground-support equipment (AGE) was analyzed for particulate mass, elemental carbon (EC) and organic carbon (OC), SO4(2-), and size distributions. The experiments occurred at idle and load conditions and utilized a chassis dynamometer. The selected AGE vehicles operated on gasoline, diesel, and JP-8. These military vehicles exhibited concentrations, size distributions, and emission factors in the same range as those reported for nonmilitary vehicles. The diesel and JP-8 emission rates for PM ranged from 0.092 to 1.1 g/kg fuel. The EC contributed less and the OC contributed more to the particulate mass than reported in recent studies of vehicle emissions. Overall, the particle size distribution varied significantly with engine condition, with the number of accumulation mode particles and the count median diameter (CMD) increasing as engine load increased. The SO4(2-) analyses showed that the distribution of SO4(2-) mass mirrored the distribution of particle mass.     

Development and preliminary evaluation of a particulate matter emission factor model for European motor vehicles

Although modeling of gaseous emissions from motor vehicles is now quite advanced, prediction of particulate emissions is still at an unsophisticated stage. Emission factors for gasoline vehicles are not reliably available, since gasoline vehicles are not included in the European Union (EU) emission test procedure. Regarding diesel vehicles, emission factors are available for different driving cycles but give little information about change of emissions with speed or engine load. We have developed size-specific speed-dependent emission factors for gasoline and diesel vehicles. Other vehicle-generated emission factors are also considered and the empirical equation for re-entrained road dust is modified to include humidity effects. A methodology is proposed to calculate modal (accelerating, cruising, or idling) emission factors. The emission factors cover particle size ranges up to 10 microns, either from published data or from user-defined size distributions. A particulate matter emission factor model (PMFAC), which incorporates virtually all the available information on particulate emissions for European motor vehicles, has been developed. PMFAC calculates the emission factors for five particle size ranges [i.e., total suspended particulates (TSP), PM10, PM5, PM2.5, and PM1] from both vehicle exhaust and nonexhaust emissions, such as tire wear, brake wear, and re-entrained road dust. The model can be used for an unlimited number of roads and lanes, and to calculate emission factors near an intersection in user-defined elements of the lane. PMFAC can be used for a variety of fleet structures. Hot emission factors at the user-defined speed can be calculated for individual vehicles, along with relative cold-to-hot emission factors. The model accounts for the proportions of distance driven with cold engines as a function of ambient temperature and road type (i.e., urban, rural, or motorway). A preliminary evaluation of PMFAC with an available dispersion model to predict the airborne concentration in the urban environment is presented. The trial was on the A6 trunk road where it passes through Loughborough, a medium-size town in the English East Midlands. This evaluation for TSP and PM10 was carried out for a range of traffic fleet compositions, speeds, and meteorological conditions. Given the limited basis of the evaluation, encouraging agreement was shown between predicted and measured concentrations.