Measurement of ultrafine particle size distributions from coal-, oil-, and gas-fired stationary combustion sources

Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h(-1) and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.     

Measurement of Ultrafine Particle Size Distributions from Coal-, Oil-, and Gas-Fired Stationary Combustion Sources

Abstract

Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h^?1 and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.     

Effect of compression ratio,nozzle opening pressure,engine load,and butanol addition on nanoparticle emissions from a non-road diesel engine

Currently, diesel engines are more preferred over gasoline engines due to their higher torque output and fuel economy. However, diesel engines confront major challenge of meeting the future stringent emission norms (especially soot particle emissions) while maintaining the same fuel economy. In this study, nanosize range soot particle emission characteristics of a stationary (non-road) diesel engine have been experimentally investigated. Experiments are conducted at a constant speed of 1500 rpm for three compression ratios and nozzle opening pressures at different engine loads. In-cylinder pressure history for 2000 consecutive engine cycles is recorded and averaged data is used for analysis of combustion characteristics. An electrical mobility-based fast particle sizer is used for analyzing particle size and mass distributions of engine exhaust particles at different test conditions. Soot particle distribution from 5 to 1000 nm was recorded. Results show that total particle concentration decreases with an increase in engine operating loads. Moreover, the addition of butanol in the diesel fuel leads to the reduction in soot particle concentration. Regression analysis was also conducted to derive a correlation between combustion parameters and particle number emissions for different compression ratios. Regression analysis shows a strong correlation between cylinder pressure-based combustion parameters and particle number emission.

     

Comparative analysis of the structure of carbon materials relevant in combustion

The determination of the structure of carbon materials is an analytical problem that join the research scientific communities involved in the chemical characterization of heavy fuel-derived products (heavy fuel oils, coal-derived fuels, shale oil, etc.) and of carbon materials (polycyclic aromatic compounds, tar, soot) produced in many combustion processes.

The knowledge of the structure of these “difficult” fuels and of the carbon materials produced by incomplete combustion is relevant to research for the best low-environmental impact operation of combustion systems; but an array of many analytical and spectroscopic tools are necessary, and often not sufficient, to attempt the characterization of such complex products and in particular to determine the distribution of molecular masses.

In this paper the size exclusion chromatography using N-methyl-pyrrolidinone as eluent has been applied for the characterization of different carbon materials starting from typical carbon species, commercially available like polyacenaphthylene, carbon black, naphthalene pitch up to combustion products like soot and soot extract collected in fuel-rich combustion systems. Two main fractions were detected, separated and molecular weights (MWs) determined by comparison with polystyrene standards: a first fraction consisted of particles with very large molecular masses (>100 000 u); a second fraction consisted of species in a relatively small MW range (200–600 u). The distribution of these fractions changes in dependence on the carbon sample characteristics.

Fluorescence spectroscopy applied on the fractions separated by size-exclusion chromatography has been used and comparatively interpreted giving indications on the differences and similarities in chemical structure of such different materials.     

Characterization of the incipient smoke point for steam-/air-assisted and nonassisted flares

Flares are important safety devices for pressure relief; at the same time, flares are a significant point source for soot and highly reactive volatile organic compounds (HRVOCs). Currently, simple guidelines for flare operations to maintain high combustion efficiency (CE) remain elusive. This paper fills the gap by investigating the characteristics of the incipient smoke point (ISP), which is widely recognized as the condition for good combustion. This study characterizes the ISP in terms of 100–% combustion inefficiency (CE), percent opacity, absorbance, air assist, steam assist, air equivalence ratio, steam equivalence ratio, exit velocity, vent gas net heating value, and combustion zone net heating value. Flame lengths were calculated for buoyant and momentum-dominated plumes under calm and windy conditions at stable and neutral atmosphere. Opacity was calculated using the Beer–Lambert law based on soot concentration, flame diameter, and mass-specific extinction cross section of soot. The calculated opacity and absorbance were found to be lognormally distributed. Linear relations were established for soot yield versus absorptivity with R² > 0.99 and power-law relations for opacity versus soot emission rate with R² ≥ 0.97 for steam-assisted, air-assisted, and nonassisted flares. The characterized steam/air assists, combustion zone/vent gas heating values, exit velocity, steam, and air equivalence ratios for the incipient smoke point will serve as a useful guideline for efficient flare operations.

Implications: A Recent EPA rule requires an evaluation of visible emissions in terms of opacity in compliance with the standards. In this paper, visible emissions such as soot particles are characterized in terms of opacity at ISP. Since ISP is widely recognized as most efficient flare operation for high combustion efficiency (CE)/destruction efficiency (DE) with initial soot particles formed in the flame, this characterization provides a useful guideline for flare operators in the refinery, oil and gas, and chemical industries to sustain smokeless and high combustion efficiency flaring in compliance with recent EPA regulations, in addition to protecting the environment.     

On airborne nano/micro-sized wear particles released from low-metallic automotive brakes

The paper addresses the wear particles released from commercially available “low-metallic” automotive brake pads subjected to brake dynamometer tests. Particle size distribution was measured in situ and the generated particles were collected. The collected fractions and the original bulk material were analyzed using several chemical and microscopic techniques. The experiments demonstrated that airborne wear particles with sizes between 10 nm and 20 μm were released into the air. The numbers of nanoparticles (<100 nm) were by three orders of magnitude larger when compared to the microparticles. A significant release of nanoparticles was measured when the average temperature of the rotor reached 300 °C, the combustion initiation temperature of organics present in brakes. In contrast to particle size distribution data, the microscopic analysis revealed the presence of nanoparticles, mostly in the form of agglomerates, in all captured fractions. The majority of elements present in the bulk material were also detected in the ultra-fine fraction of the wear particles.     

Measurements of ion concentration in gasoline and diesel engine exhaust

The nanoparticles formed in motor vehicle exhaust have received increasing attention due to their potential adverse health effects. It has been recently proposed that combustion-generated ions may play a critical role in the formation of these volatile nanoparticles. In this paper, we design an experiment to measure the total ion concentration in motor vehicle engine exhaust, and report some preliminary measurements in the exhaust of a gasoline engine (K-car) and a diesel engine (diesel generator). Under the experimental set-up reported in this study and for the specific engines used, the total ion concentration is ca. 3.3×10⁶ cm⁻³ with almost all of the ions smaller than 3 nm in the gasoline engine exhaust, and is above 2.7×10⁸ cm⁻³ with most of the ions larger than 3 nm in the diesel engine exhaust. This difference in the measured ion properties is interpreted as a result of the different residence times of exhaust inside the tailpipe/connecting pipe and the different concentrations of soot particles in the exhaust. The measured ion concentrations appear to be within the ranges predicted by a theoretical model describing the evolution of ions inside a pipe.     

Removal of a cationic dye from aqueous solutions by adsorption onto bentonite clay

The ability of bentonite to remove malachite green from aqueous solutions has been studied for different adsorbate concentrations by varying the amount of adsorbent, temperature, pH and shaking time. Maximum adsorption of the dye, i.e. >90% has been achieved in aqueous solutions using 0.05 g of bentonite at a pH of 9. Thermodynamic parameters such as ΔH°, ΔS° and ΔG° were calculated from the slope and intercept of the linear plots of ln K_D against 1/T. Analysis of adsorption results obtained at 298, 308, 318 and 328 K showed that the adsorption pattern on bentonite seems to follow the Langmuir, Freundlih and D–R isotherms. The temperature increase reduces adsorption capacity by bentonite, due to the enhancement of the desorption step in the mechanism. The numerical values of sorption free energy (E_a) of 1.00–1.12 kJ mol⁻¹ indicated physical adsorption. The kinetic data indicated an intraparticle diffusion process with sorption being first order. The rate constant k was 0.526 min⁻¹. The concentration of malachite green oxalate was measured before and after adsorption by using UV–Vis spectrophotometer.     

Simulation of the evolution of particle size distributions in a vehicle exhaust plume with unconfined dilution by ambient air

Over the past several years, numerous studies have linked ambient concentrations of particulate matter (PM) to adverse health effects, and more recent studies have identified PM size and surface area as important factors in determining the health effects of PM. This study contributes to a better understanding of the evolution of particle size distributions in exhaust plumes with unconfined dilution by ambient air. It combines computational fluid dynamics (CFD) with an aerosol dynamics model to examine the effects of different streamlines in an exhaust plume, ambient particle size distributions, and vehicle and wind speed on the particle size distribution in an exhaust plume. CFD was used to calculate the flow field and gas mixing for unconfined dilution of a vehicle exhaust plume, and the calculated dilution ratios were then used as input to the aerosol dynamics simulation. The results of the study show that vehicle speed affected the particle size distribution of an exhaust plume because increasing vehicle speed caused more rapid dilution and inhibited coagulation. Ambient particle size distributions had an effect on the smaller sized particles (approximately 10 nm range under some conditions) and larger sized particles (>2 microm) of the particle size distribution. The ambient air particle size distribution affects the larger sizes of the exhaust plume because vehicle exhaust typically contains few particles larger than 2 microm. Finally, the location of a streamline in the exhaust plume had little effect on the particle size distribution; the particle size distribution along any streamline at a distance x differed by less than 5% from the particle size distributions along any other streamline at distance x.     

Sources and concentration of nanoparticles (<10 nm diameter) in the urban atmosphere

Whilst limited information on particle size distributions and number concentrations in cities is available, very few data on the very smallest of particles, nanoparticles, have been recorded. Measurements in this study show that road traffic and stationary combustion sources generate a significant number of nanoparticles of diameter <10 nm. Measurements at the roadside (4 m from the kerb) and downwind from the traffic (more than 25 m from the kerb) show that nanoparticles (<10 nm diameter) accounted for more than 36–44% of the total particle number concentrations. Measurements designed to sample the plume of individual vehicles showed that both a diesel- and a petrol-fuelled vehicle generated nanoparticles (<10 nm diameter). The fraction of nanoparticles was even greater in a plume 350 m downwind of a stationary combustion source. On a few occasions, a temporal association between nanoparticles in the size range 3–7 nm and solar radiation was observed in urban background air at times when no other local sources were influential, which suggests that homogeneous nucleation can also be an important source of particles in the urban atmosphere.     

Analysis of exhausts emitted by i.c. engines and stationary burners, by means of u.v. extinction and fluorescence spectroscopy

Optical investigations of the exhausts emitted by internal combustion (i.c.) engines and a stationary burner were performed, in order to assess their relative role as sources of organic matter to the atmosphere. Extinction spectra of air-diluted exhausts in the 200-400 nm u.v. band reveal the expected existence of gaseous trace-species (NO, NO2 and SO2) and carbonaceous particulate matter (soot). In addition, after subtracting the absorption contribution from known species, a strong residual absorption band remains below 250 nm, which is attributed to organic aromatic matter, involving no more than two aromatic rings. A set of ex situ extinction and laser induced fluorescence (LIF) experiments were carried out on condensed combustion-water samples. Extinction measurements from the water samples show absorption spectra similar to those observed from air-diluted samples, which are attributed to low volatility organic compounds, as they are trapped in the condensed phase. Combining the indications of extinction data for both air-diluted and condensed samples, it is suggested that the absorbing species might be molecular clusters of one/two aromatic rings. LIF spectra from condensed samples evidence two fluorescence bands, centered above 300 and 400 nm, respectively, whose intensities correlate with the combustion regimes. Analogous optical analysis on rain samples, collected in an urban area, showed that rain absorption and fluorescence spectra are similar to those found in condensed exhaust samples, which is consistent with the prevailing contribution of i.c. engines to the urban air pollution. The combined experimental data suggest that the absorbing and fluorescent species trapped in the condensed samples are organic (aromatic) compounds, involving mostly one two aromatic rings structural units, since they do not absorb above 250 nm. The overall molecular weight of the trapped material is likely heavy as they show low volatility.     

Measurement of nucleation and soot mode particle emission from a diesel passenger car in real world and laboratory in situ dilution

Uncertainties still remain in the size and number emission of nucleation and soot mode particles from diesel vehicles and understanding of the nucleation process under different ambient conditions. Particle emission measurements were carried out with a EURO-3 certified European diesel passenger car running on low (<10 ppm S) and high (310 ppm S) sulfur fuel. A newly developed in situ diluter which sampled exhaust continuously from the tailpipe and diluted in two steps by a factor of 500–6000 was employed to study nucleation particle formation under well-controlled temperature and humidity conditions. Particle emission measurements were also carried out with a mobile laboratory chasing the exhaust plume of the same vehicle in summer (19–25 °C) and winter (9 °C), with no significant difference of the nucleation or soot mode particle emission found. The particle size distributions compared well with those measured in the laboratory with the same vehicle under identical driving conditions. Simple nucleation and coagulation calculations were compared with the atmospheric and laboratory measurements. It was shown that the primary dilution step had the largest impact on the nucleation mode formation, while the model overpredicted the influence of temperature and humidity. No nucleation mode particles were observed running the diesel vehicle on low (<10 ppm S) fuel.     

Characterisation of particulate matter and gaseous emissions from a large ship diesel engine

Composition of exhaust from a ship diesel engine using heavy fuel oil (HFO) was investigated onboard a large cargo vessel. The emitted particulate matter (PM) properties related to environmental and health impacts were investigated along with composition of the gas-phase emissions. Mass, size distribution, chemical composition and microphysical structure of the PM were investigated. The emission factor for PM was 5.3 g (kg fuel)^?1. The mass size distribution showed a bimodal shape with two maxima: one in the accumulation mode with mean particle diameter D_P around 0.5 μm and one in the coarse mode at D_P around 7 μm. The PM composition was dominated by organic carbon (OC), ash and sulphate while the elemental carbon (EC) composed only a few percent of the total PM. Increase of the PM in exhaust upon cooling was associated with increase of OC and sulphate. Laser analysis of the adsorbed phase in the cooled exhaust showed presence of a rich mixture of polycyclic aromatic hydrocarbon (PAH) species with molecular mass 178–300 amu while PM collected in the hot exhaust showed only four PAH masses.Microstructure and elemental analysis of ship combustion residuals indicate three distinct morphological structures with different chemical composition: soot aggregates, significantly metal polluted; char particles, clean or containing minerals; mineral and/or ash particles. Additionally, organic carbon particles of unburned fuel or/and lubricating oil origin were observed. Hazardous constituents from the combustion of heavy fuel oil such as transitional and alkali earth metals (V, Ni, Ca, Fe) were observed in the PM samples.Measurements of gaseous composition in the exhaust of this particular ship showed emission factors that are on the low side of the interval of global emission factors published in literature for NO_x, hydrocarbons (HC) and CO.     

Dilution and aerosol dynamics within a diesel car exhaust plume—CFD simulations of on-road measurement conditions

Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H₂SO₄–H₂O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads.Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter D_p∼50 nm) at variable operating conditions. Soot mode number concentrations reached up to 10¹³ m⁻³ depending on operating conditions and mixing.For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H₂SO_4(g). The highest simulated nucleation rates were about 0.05–0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle (D_p⩽15 nm) concentrations (>10¹³ m⁻³) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h⁻¹) and high engine rotational speed (>3800 revolutions per minute (rpm)).Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H₂SO₄–H₂O nucleation particles was unrealistically low compared with measurements. The possible role of low and semi-volatile organic components on the growth processes is discussed. Simulations for simplified H₂SO₄–H₂O–octane–gasoil aerosol resulted in sufficient growth of nucleation particles.     

Reaction of arsenic vapor species with fly ash compounds: kinetics and speciation of the reaction with calcium silicates

In coal combustion systems, the partitioning of arsenic between the vapor and solid phases is determined by the interaction of arsenic vapors with fly ash compounds under post-combustion conditions. This partitioning is affected by gas–solid reactions between the calcium components of the ash particles and arsenic vapors. In this study, bench scale experiments were conducted with calcium compounds typical of coal-derived fly ash to determine product formation, the extent of reaction and reaction rates when contacted by arsenic oxide vapors. Experiments conducted with arsenic trioxide (As₄O_6(g)) vapors in contact with calcium oxide, di-calcium silicate and mono-calcium silicate over the temperature range 600–1000 °C indicated that these solids were capable of reacting with arsenic vapor species in both air and nitrogen. Calcium arsenate was the observed reaction product in all the samples analyzed. Maximum capture of arsenic occurred at 1000 °C with calcium oxide being the most effective of the three solids over the range of temperatures studied. Using a shrinking core model for a first order reaction and the results from intrinsic kinetic experiments conducted in air, the reaction rate constants were found to be 1.4×10⁻³exp(−2776/T) m/s for calcium oxide particles, 7.2×10⁻³exp(−3367/T) m/s for di-calcium silicate particles and 5.5×10⁻³exp(−3607/T) m/s for mono-calcium silicate particles. These results therefore suggest that any calcium present in fly ash can react with arsenic vapor and capture the metal in water-insoluble forms of the less hazardous As(V) oxidation state.     

Modelling aerosol number distributions from a vehicle exhaust with an aerosol CFD model

Vehicular traffic contributes significantly to the aerosol number concentrations at the local scale by emitting primary soot particles and forming secondary nucleated nanoparticles. Because of their potential health effects, more attention is paid to the traffic induced aerosol number distributions.The aim of this work is to explain the phenomenology leading to the formation and the evolution of the aerosol number distributions in the vicinity of a vehicle exhaust using numerical modelling. The emissions are representative of those of a light-duty diesel truck without a diesel particle filter. The atmospheric flow is modelled with a computational fluid dynamics (CFD) code to describe the dispersion of pollutants at the local scale. The CFD code, coupled to a modal aerosol model (MAM) describing the aerosol dynamics, is used to model the tailpipe plume of a vehicle with emissions corresponding to urban driving conditions. On the basis of available measurements in Schauer et al. (1999), three surrogate species are chosen to treat the semi-volatile organic compounds in the emissions.The model simulates the formation of the aerosol distribution in the exhaust plume of a vehicle as follows. After emission to the atmosphere, particles are formed by nucleation of sulphuric acid and water vapour depending strongly on the thermodynamic state of the atmosphere and on the dilution conditions. The semi-volatile organic compounds are critical for the rapid growth of nanoparticles through condensation. The semi-volatile organic compounds are also important for the evolution of primary soot particles and can contribute substantially to their chemical composition.The most influential parameters for particle formation are the sulphur fuel content, the semi-volatile organic emissions and also the mass and initial diameter of the soot particles emitted. The model is able to take into account the complex competition between nucleation, condensation and dilution, as well as the interactions among the different aerosol modes. This type of model is a useful tool to better understand the dynamics leading to the formation of traffic induced aerosol distributions. However, some key issues such as the turbulence in the exhaust plume and in the wake of the car, the magnitude and chemical composition of semi-volatile organic emissions and the possible nucleation of organic species need to be investigated further to improve our understanding of ultrafine particle formation.     

Synchronous-scan fluorescence spectra of Chlorella vulgaris solution

The characterization of the Chlorella vulgaris solution was carried out using synchronous-scan spectroscopy. The range of concentration of algae and Fe(III) in aqueous solutions were 5 × 10⁸–8 × 10⁹ cells l⁻¹ and 10–60 μM, respectively. Effective characterization method used was synchronous-scan fluorescence spectroscopy. The wavelength difference (Δλ) of 90 nm was maintained between excitation and emission wavelengths; 90 nm was found to be the best Δλ for effective characterization of Chlorella vulgaris solution with or without quencher species (e.g., Fe(III), humic acid (HA)) for the first time. The peak was observed at about EX 236.6 nm/EM 326.6 nm for synchronous-scan fluorescence spectra. The fluorescence quenching of algae in system of algae–Fe(III)–HA was studied using synchronous-scan spectroscopy for the first time. Fe(III) was clearly the effective quencher. The relationship between I₀/I (quenching efficiency) and c (concentration of Fe(III) added) was a linear correlation for the algae solution with Fe(III). Also, Aldrich humic acid was found to be an effective quencher. pH effect on synchronous-scan fluorescence intensity of algal solution with Fe(III) and/or HA was evident.     

Volatile nanoparticle formation and growth within a diluting diesel car exhaust

A major source of particle number emissions is road traffic. However, scientific knowledge concerning secondary particle formation and growth of ultrafine particles within vehicle exhaust plumes is still very limited. Volatile nanoparticle formation and subsequent growth conditions were analyzed here to gain a better understanding of "real-world" dilution conditions. Coupled computational fluid dynamics and aerosol microphysics models together with measured size distributions within the exhaust plume of a diesel car were used. The impact of soot particles on nucleation, acting as a condensational sink, and the possible role of low-volatile organic components in growth were assessed. A prescribed reduction of soot particle emissions by 2 orders of magnitude (to capture the effect of a diesel particle filter) resulted in concentrations of nucleation-mode particles within the exhaust plume that were approximately 1 order of magnitude larger. Simulations for simplified sulfuric acid-water vapor gas-oil containing nucleation-mode particles show that the largest particle growth is located in a recirculation zone in the wake of the car. Growth of particles within the vehicle exhaust plume up to detectable size depends crucially on the relationship between the mass rate of gaseous precursor emissions and rapid dilution. Chassis dynamometer measurements indicate that emissions of possible hydrocarbon precursors are significantly enhanced under high engine load conditions and high engine speed. On the basis of results obtained for a diesel passenger car, the contributions from light diesel vehicles to the observed abundance of measured nucleation-mode particles near busy roads might be attributable to the impact of two different time scales: (1) a short one within the plume, marked by sufficient precursor emissions and rapid dilution; and (2) a second and comparatively long time scale resulting from the mix of different precursor sources and the impact of atmospheric chemistry.     

Predominance of soot-mode ultrafine particles in Santiago de Chile: Possible sources

A monitoring campaign was performed in Santiago de Chile during a winter month of 2003 and 2006 (July) using several instruments to measure the size distribution of particulate material. For the first time, the size distribution of ultrafine particles was measured in Santiago, and an estimation of its sources was done by analyzing its temporal variation. The study was performed in three sites; one of them is located in the eastern part of Santiago, a sector with low particle concentration and about 100 m from a busy street. The other site is located in the western part, which is the sector that has the highest concentration of fine and coarse particle matter during winter, also located far from a street. The third site is located within 5 m from the busiest street in Santiago. In all stations traffic is the dominating source for fine and ultrafine particles and the size distribution is peaked towards 60–100 nm (soot mode). Only in the site near the street, it is possible to see a clear peak towards smaller sizes (10–30 nm). The size distribution measurements presented here indicate that aerosol dynamics play a more important role for the Santiago case as compared to cleaner cities in Europe. Changes in the particle size during different hours of the day reflect both variations in meteorological mixing conditions as well as effects of aerosol dynamic processes such as coagulation, condensation and dry deposition. A relative increase in the number of the larger ultrafine particles (d ≥ 70 nm), as compared to the number of smaller particles (d < 70 nm) correlated with wind speed is an indication of pollution transport with aged particles from other parts of the city.     

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.