Comparison of daytime and nighttime concentration profiles and size distributions of ultrafine particles near a major highway

Previously we have conducted systematic measurements of the concentration and size distribution of ultrafine particles in the vicinity of major highways during daytime in Los Angeles. The present study compares these with similar measurements made at night. Particle number concentration was measured by a condensation particle counter (CPC) and size distributions in the size range from 7 to 300 nm were measured by a scanning mobility particle sizer (SMPS). Measurements were taken at 30, 60, 90, 150, and 300 m upwind and downwind from the center of the 1-405 freeway. Average traffic flow at night was about 25% of that observed during the day. Particle number concentration measured at 30 m downwind from the freeway was 80% of previous daytime measurements. This discrepancy between changes in traffic counts and particle number concentrations is apparently due to the decreased temperature, increased relative humidity, and lower wind speed at night. Particle size distributions do not change as dramatically as they did during the daytime. Particle number concentration decays exponentially downwind from the freeway similarly to what was observed during the day, but at a slower rate. No particle number concentration gradient has been observed for the upwind side of the freeway. No PM2.5 and very weak PM10 concentration gradients were observed downwind of thefreeway at night. Ultrafine particle number concentration measured at 300 m downwind from the freeway was still distinguishably higher than upwind background concentration at night. These data may be used to help estimate exposure to ultrafine particles in the vicinity of major highways for epidemiology studies.     

Source strengths of ultrafine and fine particles due to cooking with a gas stove

Cooking, particularly frying, is an important source of particles indoors. Few studies have measured a full range of particle sizes, including ultrafine particles, produced during cooking. In this study, semicontinuous instruments with fine size discriminating ability were used to calculate particle counts in 124 size bins from 0.01 to 2.5 microm. Data were collected at 5 min intervals for 18 months in an occupied house. Tracer gas measurements were made every 10 min in each of 10 rooms of the house to establish air change rates. Cooking episodes (N = 44) were selected meeting certain criteria (high concentrations, no concurrent indoor sources, long smooth decay curves), and the number and volume of particles produced were determined for each size category. For each episode, the particle decay rate was determined and used to determine the source strength for each size category. The selected cooking episodes (mostly frying) were capable of producing about 10(14) particles over the length of the cooking period (about 15 min), more than 90% of them in the ultrafine (< 0.1 microm) range, with an estimated whole-house volume concentration of 50 (microm/cm)3. More than 60% of this volume occurred in the 0.1-0.3 microm range. Frying produced peak numbers of particles at about 0.06 microm, with a secondary peak at 0.01 microm. The peak volume occurred at a diameter of about 0.16 microm. Since the cooking episodes selected were biased toward higher concentrations, the particle concentrations measured during about 600 h of morning and evening cooking over a full year were compared to concentrations measured during noncooking periods at the same times. Cooking was capable of producing more than 10 times the ultrafine particle number observed during noncooking periods. Levels of PM2.5 were increased during cooking by a factor of 3. Breakfast cooking (mainly heating water for coffee and using an electric toaster) produced concentrations about half those produced from more complex dinnertime cooking. Although the number and volume concentrations observed depend on air change rates, house volume, and deposition rates due to fans and filters, the source strengths calculated here are independent of these variables and may be used to estimate number and volume concentrations in other types of homes with widely varying volumes, ventilation rates, and heating and air-conditioning practices.     

In-cabin commuter exposure to ultrafine particles on Los Angeles freeways

Worldwide people are exposed to toxic ultrafine particles (UFP, with diameters (dp) less than 100 nm) and nanoparticles (NP, dp < 50 nm) under a variety of circumstances. To date, very limited information is available on human exposure to freshly emitted UFP and NP while traveling on major roads and freeways. We report in-cabin and outdoor measurements of particle number concentration and size distributions while driving three vehicles on Los Angeles freeways. Particle number concentrations and size distributions were measured under different vehicle ventilation settings. When the circulation fan was set to on, with substantial external air intake, outside changes in particle counts caused corresponding in-cabin changes approximately 30-60 s later, indicating an maximal air exchange rate of about 120-60 h(-1). Maximum in-cabin protection (approximately 85%) was obtained when both fan and recirculation were on. In-cabin and outdoor particle size distributions in the 7.9-217 nm range were observed to be mostly bimodal, with the primary peak occurring at 10-30 nm and the secondary at 50-70 nm. The vehicle's manufacture-installed particle filter offered an in-cabin protection of about 50% for particles in the 7-40 nm size range and 20-30% for particles in the 40 to approximately 200 nm size range. For an hour daily commute exposure, the in-vehicle microenvironment contributes approximately 10-50% of people's daily exposure to UFP from traffic.     

Chemical and physical properties of ultrafine diesel exhaust particles sampled downstream of a catalytic trap

The chemical and physical properties of exhaust particles produced by a Caterpillar 3176 C-12 heavy duty diesel engine equipped with a catalytic trap (CRT) are reported. The engine was operated at 600 Nm and 1500 rpm, using fuels containing 15 and 49 ppm sulfur. A two-stage dilution tunnel designed to simulate the reactions that occur when hot combustion products mix with cooler atmospheric air was used. Particle size distributions were measured using a scanning mobility particle sizer (SMPS) and nano-scanning mobility particle sizer (nano SMPS); a nanomicro-orifice uniform deposit impactor (nano MOUDI) collected size-resolved samples for gravimetric and chemical analysis. A nanometer tandem differential mobility analyzer (nano TDMA) was used to measure the volatility and hygroscopicity of 4-15 nm particles. These measurements confirm that the particles consisted primarily of sulfates.     

XRF-analysis of fine and ultrafine particles emitted from laser printing devices

In this work, the elemental composition of fine and ultrafine particles emitted by ten different laser printing devices (LPD) is examined. The particle number concentration time series was measured as well as the particle size distributions. In parallel, emitted particles were size-selectively sampled with a cascade impactor and subsequently analyzed by the means of XRF. In order to identify potential sources for the aerosol's elemental composition, materials involved in the printing process such as toner, paper, and structural components of the printer were also analyzed. While the majority of particle emissions from laser printers are known to consist of recondensated semi volatile organic compounds, elemental analysis identifies Si, S, Cl, Ca, Ti, Cr, and Fe as well as traces of Ni and Zn in different size fractions of the aerosols. These elements can mainly be assigned to contributions from toner and paper. The detection of elements that are likely to be present in inorganic compounds is in good agreement with the measurement of nonvolatile particles. Quantitative measurements of solid particles at 400 °C resulted in residues of 1.6 × 10(9) and 1.5 × 10(10) particles per print job, representing fractions of 0.2% and 1.9% of the total number of emitted particles at room temperature. In combination with the XRF results it is concluded that solid inorganic particles contribute to LPD emissions in measurable quantities. Furthermore, for the first time Br was detected in significant concentrations in the aerosol emitted from two LPD. The analysis of several possible sources identified the plastic housings of the fuser units as main sources due to substantial Br concentrations related to brominated flame retardants.     

Effect of advanced aftertreatment for PM and NOx reduction on heavy-duty diesel engine ultrafine particle emissions

Four heavy-duty and medium-duty diesel vehicles were tested in six different aftertreament configurations using a chassis dynamometer to characterize the occurrence of nucleation (the conversion of exhaust gases to particles upon dilution). The aftertreatment included four different diesel particulate filters and two selective catalytic reduction (SCR) devices. All DPFs reduced the emissions of solid particles by several orders of magnitude, but in certain cases the occurrence of a volatile nucleation mode could increase total particle number emissions. The occurrence of a nucleation mode could be predicted based on the level of catalyst in the aftertreatment, the prevailing temperature in the aftertreatment, and the age of the aftertreatment. The particles measured during nucleation had a high fraction of sulfate, up to 62% of reconstructed mass. Additionally the catalyst reduced the toxicity measured in chemical and cellular assays suggesting a pathway for an inverse correlation between particle number and toxicity. The results have implications for exposure to and toxicity of diesel PM.     

Transmission electron microscopy investigation of ultrafine coal fly ash particles

Ultrafine (<100 nm) ash particles in three coal fly ashes (CFA) produced by the combustion of three U.S. coals have been examined by high-resolution transmission electron microscopy (HRTEM), energy-dispersive X-ray spectroscopy (EDS), and electron diffraction. These ultrafine particles, either as primary ash particles derived directly from coal minerals or as secondary products of decomposition and vaporization-condensation processes, show quite different morphologies, compositions, and microstructures as compared to particles in coarser, micrometer-size fractions previously examined by CCSEM. An eastern U.S. bituminous CFA sample shows abundant discrete crystalline particles rich in Fe, Ti, and Al in its ultrafine ash fraction, and crystalline phases down to 10 nm size have been identified. Western U.S. low-rank CFA samples contain considerable amounts of alkaline-earth element aggregates in the form of phosphates, silicates, and sulfates and mixed species. Most of them show crystalline or crystalline plus amorphous characteristics. All three ultrafine samples also exhibit carbonaceous particles in the form of soot aggregates with primary particle size typically between 20 and 50 nm. In the western low-rank ultrafine CFAs, these carbonaceous soot particles were typically mixed or coated with multi-element inorganic species.     

Performance of school bus retrofit systems: ultrafine particles and other vehicular pollutants

This study evaluated the performance of retrofit systems for diesel-powered school buses, a diesel oxidation catalyst (DOC) muffler and a spiracle crankcase filtration system (CFS), regarding ultrafine particles (UFPs) and other air pollutants from tailpipe emissions and inside bus cabins. Tailpipe emissions and in-cabin air pollutant levels were measured before and after retrofitting when the buses were idling and during actual pick-up/drop off routes. Retrofit systems significantly reduced tailpipe emissions with a reduction of 20-94% of total particles with both DOC and CFS installed. However, no unequivocal decrease was observed for in-cabin air pollutants after retrofitting. The AC/fan unit and the surrounding air pollutant concentrations played more important roles for determining the in-cabin air quality of school buses than did retrofit technologies. Although current retrofit systems reduce children's exposure while waiting to board at a bus station, retrofitting by itself does not protect children satisfactorily from in-cabin particle exposures. Turning on the bus engine increased in-cabin UFP levels significantly only when the wind blew from the bus' tailpipe toward its hood with its windows open. This indicated that wind direction and window position are significant factors determining how much self-released tailpipe emissions may penetrate into the bus cabin. The use of an air purifier was found to remove in-cabin particles by up to 50% which might be an alternative short-to-medium term strategy to protect children's health.     

Characteristics of nucleation and growth events of ultrafine particles measured in Rochester, NY

Number concentrations and size distributions of particles in the size range of 0.010-0.500 microm were measured in Rochester, NY, from December 2001 to December 2002. The relationships between the number concentrations, gaseous pollutants, and meteorological parameters were examined during particle nucleation events. More than 70% of measured total number concentration was associated with ultrafine particles (UFP, 0.011-0.050 microm). Morning nucleation events typically peaking UFP number concentrations at around 08:00 were apparent in winter months with CO increases. These particles appear to be formed following direct emissions from motorvehicles during morning rush hour. There were also often observed increases in this smaller-sized range particles in the late afternoon during the afternoon rush hour, particularly in winter when the mixing heights remain lowerthan in summer. Strong afternoon nucleation events (> 30,000 cm(-3)) peaking at around 13: 00 were more likely to occur in spiring and summer months. During the prominent nucleation events, peaks of SO2 were strongly associated with the number concentrations of UFP, whereas there were no significant correlations between these events and PM2.5 and CO. Increased SO2 concentrations were observed when the wind direction was northwesterly where three SO2 sources were located. It is hypothesized that UFP formed during the events are sulfuric acid and water from the oxidation of SO2. There were also a more limited number of nucleation events followed by particle growth up to approximately 0.1 microm over periods of up to 18 h. The nucleation and growth events tended to be common in spring months especially in April.     

用SDS-二甲苯体系合成SnO2微粉的研究

用十二烷基硫酸钠（简称ＳＤＳ）－二甲苯微乳液法和化学沉淀法分别合成了ＳnO2微粉样品,并将其制备成旁热式气敏元件,进行气敏性能测定,结果表明,用ＳＤＳ－二甲苯作介质的方法合成的ＳnO2制备成气敏元件,对Ｈ２Ｓ气体的灵敏度与选择性均有较大改善。     

Axial flow cyclone for segregation and collection of ultrafine particles: theoretical and experimental study

In this study, an axial flow cyclone was designed, fabricated, and evaluated at different conditions of air flow rates (Q0) and low-pressure environments (P), especially for the segregation and collection of ultrafine particles. An evaporation/condensation type of aerosol generation system consisting of tube furnace and mixing chamber was employed to produce test aerosols. The test aerosol was then classified by a differential mobility analyzer (DMA) and number concentration was measured by a condensation nuclei counter (CNC) and an electrometer upstream and downstream of the cyclone, respectively. The s-shaped curve of the collection efficiency in submicron particle size range was obtained to be similar to the traditional cyclone found in the literatures when the particles were largerthan 40 nm at Q0 = 1.07, 0.455 L(STP)/min, and P = 4.8-500 Torr. The curve was found to be fitted very well by a semiempirical equation described in this paper. For particles smaller than 40 nm, however, the collection efficiency was unusually increased as the particle diameter was decreased due to the fact that the diffusion deposition becomes the dominant collection mechanism in the low-pressure conditions. A model composed of centrifugal force and diffusion deposition is presented and used to fit the experimental data. The cyclone was demonstrated to separate and collect ultrafine particles effectively in the tested vacuum conditions.     

Real-world emission factors of fine and ultrafine aerosol particles for different traffic situations in Switzerland

Extended field measurements of particle number (size distribution of particle diameters, D, in the range between 18 nm and 10 microm), surface area concentrations, and PM1 and PM10 mass concentrations were performed in Switzerland to determine traffic emissions using a comprehensive set of instruments. Measurements took place at roads with representative traffic regimes: at the kerbside of a motorway (120 km h(-1)), a highway (80-100 km h(-1)), and in an urban area with stop-and-go traffic (0-50 km h(-1)) regulated by light signals. Mean diurnal variations showed that the highest pollutant concentrations were during the morning rush hours, especially of the number density in the nanoparticle size range (D <50 nm). From the differences between up- and downwind concentrations (or differences between kerbside and background concentrations for the urban site), "real-life" emission factors were derived using NOx concentrations to calculate dilution factors. Particle number and volume emission factors of different size ranges (18-50 nm, 18-100 nm, and 18-300 nm) were derived for the total vehicle fleet and separated into a light-duty (LDV) and a heavy-duty vehicle (HDV) contribution. The total particle number emissions per vehicle were found to be about 11.7-13.5 x 10(14) particles km(-1) for constant speed (80-120 km h(-1) and 3.9 x 10(14) particles km(-1) for urban driving conditions. LDVs showed higher emission factors at constant high speed than under urban disturbed traffic flow. In contrast, HDVs emitted more air pollutants during deceleration and acceleration processes in stop-and-go traffic than with constant speed of about 80 km h(-1). On average, one HDV emits a 10-30 times higher amount of particulate air pollutants (in terms of both number and volume) than one LDV.     

PAHs, PAH-induced carcinogenic potency, and particle-extract-Induced cytotoxicity of traffic-related nano/ultrafine particles

Polycyclic aromatic hydrocarbons (PAHs) bound in nano/ ultrafine particles from vehicle emissions may cause adverse health effects. However, little is known about the characteristics of the nanoparticle-bound PAHs and the PAH-associated carcinogenic potency/cytotoxicity; therefore, traffic-related nano/ultrafine particles were collected in this study using a microorifice uniform deposition impactor(MOUDI) and a nano-MOUDI. For PM0.056--18, the difference in size-distribution of particulate total-PAHs between non-after-rain and after-rain samples was statistically significant at alpha = 0.05; however, this difference was not significant for PM0.01--0.056. The PAH correlation between PM0.01--0.1 and PM0.1--1.8 was lower for the after-rain samples than forthe non-after-rain samples. The average particulate total-PAHs in five samplings displayed a trimodal distribution with a major peak in the Aitken mode (0.032--0.056 microm). About half of the particulate total-PAHs were in the ultrafine size range. The BaPeq sums of BaP, IND, and DBA (with toxic equivalence factors > or = 0.1) accounted for approximately 90% of the total-BaPeq in the nano/ultrafine particles, although these three compounds contributed little to the mass of the sampled particles. The mean content of the particle-bound total-PAHs/-BaPeqs and the PAH/BaPeq-derived carcinogenic potency followed the order nano > ultrafine > fine > coarse. For a sunny day sample, the cytotoxicity of particle extracts (using 1:1 (v/v) n-hexane/dichloromethane) was significantly higher (p < 0.05) for the nano (particularly the 10-18 nm)/ultrafine particles than for the coarser particles and bleomycin. Therefore, traffic-related nano and ultrafine particles are possibly cytotoxic.     

Direct identification of trace metals in fine and ultrafine particles in the Detroit urban atmosphere

Exposure to airborne particulates containing low concentrations of heavy metals, such as Pb, As, and Se, may have serious health effects. However, little is known about the speciation and particle size of these airborne metals. Fine- and ultrafine particles with heavy metals in aerosol samples from the Detroit urban area, Michigan, were examined in detail to investigate metal concentrations and speciation. The characterization of individual particles was completed using high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) combined with conventional high-resolution TEM techniques. The trace elements, Pb, As, La, Ce, Sr, Zn, Cr, Se, Sn, Y, Zr, Au, and Ag, were detected, and the elemental distributions were mapped in situ atthe nanoscale. The crystal structures of the particles containing Pb, Sr, Zn, and Au were determined from their electron diffraction patterns. Based on the characterization of the representative trace element particles, the potential health effects are discussed. Most of the trace element particles detected in this study were within a range of 0.01-1.0 microm in size, which has the longest atmospheric residence time (approximately 100 days). Increased chemical reactivity owing to the size of nanoparticles may be expected for most of the trace metal particles observed.     

Characteristics of metals in nano/ultrafine/fine/coarse particles collected beside a heavily trafficked road

Fine particles emitted from vehicles have adverse health effects because of their sizes and chemical compositions. Therefore, this study attempted to characterize the metals in nano (0.010 < Dp < 0.056 microm), ultrafine (Dp < 0.1 microm), fine (Dp < 2.5 microm), and coarse (2.5 < Dp < 10 microm) particles collected near a busy road using a microorifice uniform deposition impactor (MOUDI) and a Nano-MOUDI. The nano particles were found to contain more of traffic-related metals (Pb, Cd, Cu, Zn, Ba, and Ni) than particles of other sizes, although crustal metals accounted for over 90% of all the particulate metals. Most crustal metals, Ba, Ni, Pb, and Zn in ultrafine particles displayed Aitken modes due to their local origins. The Ag, Cd, Cr, Ni, Pb, Sb, V, and Zn were 37, 50, 28, 30, 24, 64, 38, and 22% by mass, respectively, in < 0.1-microm particles, with submicron mass median diameters (MMDs) in PM(0.01-18) (except Zn) (particularly the < 0.1-microm MMDs for Cd and Sb). These levels raise potential health issues. Particle-bound Zn was more abundant in the accumulation mode than in the nucleation/condensation mode, but the opposite was true for Ag, Cd, and Sb. The Ag, Ba, Cd, Pb, Sb, V, and Zn contents in nano particles were strongly associated with diesel fuel, while the Cu, Mn, and Sr in particles < 0.1 microm were more strongly associated with gasoline. The high content of Si in nano particles, more associated with diesel soot than with gasoline exhaust, is another health concern.     

Exposure to fine and ultrafine particles from secondhand smoke in public places before and after the smoking ban, Italy 2005

Background

A smoking ban in all indoor public places was enforced in Italy on 10 January 2005.

Methods

We compared indoor air quality before and after the smoking ban by monitoring the indoor concentrations of fine (<2.5 μm diameter, PM_2.5) and ultrafine particulate matter (<0.1 μm diameter, UFP). PM_2.5 and ultrafine particles were measured in 40 public places (14 bars, six fast food restaurants, eight restaurants, six game rooms, six pubs) in Rome, before and after the introduction of the law banning smoking (after 3 and 12 months). Measurements were taken using real time particle monitors (DustTRAK Mod. 8520 TSI; Ultra‐fine Particles Counter‐TRAK Model 8525 TSI). The PM_2.5 data were scaled using a correction equation derived from a comparison with the reference method (gravimetric measurement). The study was completed by measuring urinary cotinine, and pre‐law and post‐law enforcement among non‐smoking employees at these establishments

Results

In the post‐law period, PM_2.5 decreased significantly from a mean concentration of 119.3 μg/m³ to 38.2 μg/m³ after 3 months (p<0.005), and then to 43.3 μg/m³ a year later (p<0.01). The UFP concentrations also decreased significantly from 76 956 particles/cm³ to 38 079 particles/cm³ (p<0.0001) and then to 51 692 particles/cm³ (p<0.01). Similarly, the concentration of urinary cotinine among non‐smoking workers decreased from 17.8 ng/ml to 5.5 ng/ml (p<0.0001) and then to 3.7 ng/ml (p<0.0001).

Conclusion

The application of the smoking ban led to a considerable reduction in the exposure to indoor fine and ultrafine particles in hospitality venues, confirmed by a contemporaneous reduction of urinary cotinine.     

Apportionment of motor vehicle emissions from fast changes in number concentration and chemical composition of ultrafine particles near a roadway intersection

High frequency spikes in ultrafine number concentration near a roadway intersection arise from motor vehicles that accelerate after a red light turns green. The present work describes a method to determine the contribution of motor vehicles to the total ambient ultrafine particle mass by correlating these number concentration spikes with fast changes in ultrafine particle chemical composition measured with the nano aerosol mass spectrometer, NAMS. Measurements were performed at an urban air quality monitoring site in Wilmington, Delaware during the summer and winter of 2009. Motor vehicles were found to contribute 48% of the ultrafine particle mass in the winter measurement period, but only 16% of the ultrafine particle mass in the summer period. Chemical composition profiles and contributions to the ultrafine particle mass of spark vs diesel vehicles were estimated by correlating still camera images, chemical composition and spike contribution at each time interval.. The spark and diesel contributions were roughly equal, but the uncertainty in the split was large. The distribution of emissions from individual vehicles was determined by correlating camera images with the spike contribution to particle number concentration at each time interval. A small percentage of motor vehicles were found to emit a disproportionally large concentration of ultrafine particles, and these high emitters included both spark ignition and diesel vehicles.     

Single particle characterization of ultrafine and accumulation mode particles from heavy duty diesel vehicles using aerosol time-of-flight mass spectrometry

The aerodynamic size and chemical composition of individual ultrafine and accumulation mode particle emissions (Da = 50-300 nm) were characterized to determine mass spectral signatures for heavy duty diesel vehicle (HDDV) emissions that can be used for atmospheric source apportionment. As part of this study, six in-use HDDVs were operated on a chassis dynamometer using the heavy heavy-duty diesel truck (HHDDT) five-cycle driving schedule under different simulated weight loads. The exhaust emissions were passed through a dilution/residence system to simulate atmospheric dilution conditions, after which an ultrafine aerosol time-of-flight mass spectrometer (UF-ATOFMS) was used to sample and characterize the HDDV exhaust particles in real-time. This represents the first study where refractory species including elemental carbon and metals are characterized directly in HDDV emissions using on-line mass spectrometry. The top three particle classes observed with the UF-ATOFMS comprise 91% of the total particles sampled and show signatures indicative of a combination of elemental carbon (EC) and engine lubricating oil. In addition to the vehicle make/year, the effects of driving cycle and simulated weight load on exhaust particle size and composition were investigated.     

Model simulations of particle aggregation effect on colloid exchange between streams and streambeds

Colloids found in natural streams have large reactive surface areas, which makes them significant absorbents and carriers for pollutants. Stream-subsurface exchange plays a critical role in regulating the transport of colloids and contaminants in natural streams. Previous process-based multiphase exchange models were developed without consideration of colloid-colloid interaction. However, many studies have indicated that aggregation is a significant process and needs to be considered in stream process analysis. Herein, a new colloid exchange model was developed by including particle aggregation in addition to colloid settling and filtration. Self-preserving size distribution concepts and classical aggregation theory were employed to model the aggregation process. Model simulations indicate that under conditions of low filtration and high degree of particle-particle interaction, aggregation could either decrease or increase the amount of colloids retained in streambeds, depending on the initial particle size. Thus, two possible cases may occur including enhanced colloid deposition and facilitated colloid transport. Also, when the aggregation rate is high and filtration increases, more particles are retained by bed sediments due to filtration, and fewer are aggregated, which reduces the extent of aggregation effect on colloid deposition. The work presented here will contribute to a better understanding and prediction of colloid transport phenomena in natural streams.