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.     

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.     

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.     

Model simulations of NOx and ultrafine particles close to a Swedish highway

Based on the results from a 6-week monitoring campaign in an area close to a major highway north of Stockholm, Sweden, NOx emission factors representative for vehicle speeds of 100-120 km per h were determined to 0.61 g/veh,km for light duty and to 7.1 g/veh,km for heavy duty vehicles. The corresponding factors for particle number were 1.4 x 10(14) and 52 x 10(14) particles/veh,km, determined for an ambient temperature interval of +7 to +17 degrees C. The removal effects of coagulation and dry deposition on total number concentrations were assessed by numerical model simulations. Velocity and turbulence fields, including those produced by the vehicles, were simulated in a Computational Fluid Dynamics (CFD) model. Coagulation was found to be of little importance over the first 100 m downwind of the highway. The high friction velocities over the road surface created by vehicle movements enhanced deposition locally, contributing to the removal of approximately 10% of the particles originally emitted. Beyond a point 10 m downwind of the highway the removal rate was low and the ultrafine particles were almost inert while being advected over the next hundred meters. As a consequence, it seems reasonable to use monitored data from stations close to highways to estimate emission factors for particle number, assuming that the particles are inert. Those "effective" emission factors should be applicable for urban models with a larger spatial resolution.     

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.     

On-line analysis of the size distribution of fine and ultrafine aerosol particles in flue and stack gas of a municipal waste incineration plant: effects of dynamic process control measures and emission reduction devices

The size distribution of particles in the waste gas of a municipal waste incineration plant (23 MW) was measured on-line at two sampling points in the flue-gas duct (700 and 300 degrees C) as well as in the stack gas (80 degrees C). The measurements were performed during both stable combustion conditions and transient operating conditions. The particle measurements were carried out by a mobile system consisting of a home-designed sampling system with dilution device and a scanning mobility particle sizer (SMPS) for the particle size range 17-600 nm as well as an aerodynamic particle sizer (APS) for the size range 500 nm-30 microm. The APS and SMPS data were combined using a special method and a home written software tool. The maximum of the particle-size distribution in the flue gas of the incinerator shifts from about 90 nm at the 700 degrees C sampling point to about 140 nm at the 300 degrees C point, showing the particle growth by coagulation processes and condensation of inorganic and organic gaseous species with decreasing temperature. This finding is consistent with the measured concentration profiles of gaseous organic chemical species in the flue gas. While at flue-gas temperatures of 600-800 degrees C a rich pattern of polycyclic aromatic hydrocarbon species (PAH) is observable, the PAH concentrations are considerably reduced further downstream of the flue-gas channel, where the temperature drops below 500 degrees C. Condensation and reactive bonding of gaseous chemicals onto particulate matter is, among other reasons, responsible for the depletion of gas-phase species. Process control measures, such as firing the backup burners or cleaning of the grate with pressurized air, can cause dynamic changes of the particle-size distribution. Furthermore the flue-gas cleaning measures have great impact onto both the particle concentration and the size distribution. For this reason the impact of one particular emission reduction device, the wet electrostatic dust precipitator (wet-ESP), is evaluated. The wet-ESP reduces considerably the particle concentration over the whole size range. Behind the flue-gas processing units a broad maximum in the particle-size distribution occurs at about 70 nm, but no pronounced particle-size distribution could be observed. The particle concentration level atthis maximum is about 3 magnitudes lower than in the raw flue gas. However, intermittent periods lasting for several minutes of high emissions of ultrafine particles with d < 40 nm were observed. These particles are most likely formed by nucleation processes behind the wet-ESP from gas-phase constituents of the stack gas.     

Source identification of fine particles in Washington, DC, by expanded factor analysis modeling

An expanded factor analysis model (ME-2) that is capable of taking into account the influence of independent variables such as wind speed, wind direction, time of year and other variables of the measured fine particle matter (PM2.5) concentration data was utilized for identifying sources of airborne pollutants and providing quantitative estimations of the contribution of each source. The chemical composition data used in this study were obtained from PM2.5 samples collected using the Interagency Monitoring of Protected Visual Environments samplers from August 1999 to December 2001 at an urban monitoring site in Washington, DC. The expanded model has been applied to two different data sets based on the particulate carbon variables. Such an approach had been successfully applied previously and provided improved source resolution in simulated and ambient concentration data. Initially, total OC and EC were used in the expanded model and were compared to the results using conventional positive matrix factorization that had been done previously using the individual carbon fractions data. In the other expanded model analysis, the eight carbon fractions were used during the modeling in order to ascertain if additional source information could be extracted from the data. In both cases, it was possible to separate diesel from spark-ignition vehicles. The use of the individual carbon fractions in the model provides information on what appears to be secondary organic aerosol formation.     

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.     

天然气热风炉与燃烧器在热定形机中的应用

分析了天然气的燃烧过程,并介绍了天然气燃烧器的结构类型与设计计算.讨论了全自动天然气燃烧器的结构组件和燃气阀门组件,研究了天然气直接式热风炉与间接式热风炉的结构,并比较了套筒式、螺旋板式及管板式间接热风炉的结构特点.探讨了天然气直接式热风炉和间接式热风炉与燃烧器在纺织印染热定形机中的开发应用.     

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.     

Iodine content in commonly consumed food in Hong Kong and its changes due to cooking

Levels of iodine of foods found in Hong Kong were analysed in 271 samples from 11 groups, including (i) cereals and grain products, (ii) legumes and vegetables, (iii) meat and poultry, (iv) egg and egg products, (v) milk and milk products, (vi) fish, (vii) crustaceans and mollusks, (viii) non-alcoholic beverages, (ix) condiments and sauces, (x) sashimi and (xi) seaweeds. All food samples were analysed individually as purchased. The iodine in all samples ranged from undetectable to 2.9?g?kg^?1. Seaweeds, iodised salt, seafood, milk and milk products as well as egg and egg products were rich sources of iodine. To estimate the influence of cooking on iodine levels in foods, a total of 15 individual samples were analysed as raw and respective cooked food. The influence of cooking on the iodine level was minimal, except for boiling, as iodine dissolved into the soup.     

Interaction of fine particles and nanoparticles with red blood cells visualized with advanced microscopic techniques

So far, little is known about the interaction of nanoparticles with lung cells, the entering of nanoparticles, and their transport through the blood stream to other organs. The entering and localization of different nanoparticles consisting of differing materials and of different charges were studied in human red blood cells. As these cells do not have any phagocytic receptors on their surface, and no actinmyosin system, we chose them as a model for nonphagocytic cells to study how nanoparticles penetrate cell membranes. We combined different microscopic techniques to visualize fine and nanoparticles in red blood cells: (I) fluorescent particles were analyzed by laser scanning microscopy combined with digital image restoration, (II) gold particles were analyzed by conventional transmission electron microscopy and energy filtering transmission electron microscopy, and (III) titanium dioxide particles were analyzed by energy filtering transmission electron microscopy. By using these differing microscopic techniques we were able to visualize and detect particles < or = 0.2 microm and nanoparticles in red blood cells. We found that the surface charge and the material of the particles did not influence their entering. These results suggest that particles may penetrate the red blood cell membrane by a still unknown mechanism different from phagocytosis and endocytosis.     

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.     

常规间歇蒸煮改造为DDS置换蒸煮的做法和经验

介绍了传统间歇蒸煮在不停机的情况下,改造成高效,节能、环保的DDS置换蒸煮的思路、方法以及改造过程中遇到的问题和解决办法.     

Iron solubility related to particle sulfur content in source emission and ambient fine particles

The chemical factors influencing iron solubility (soluble iron/total iron) were investigated in source emission (e.g., biomass burning, coal fly ash, mineral dust, and mobile exhaust) and ambient (Atlanta, GA) fine particles (PM2.5). Chemical properties (speciation and mixing state) of iron-containing particles were characterized using X-ray absorption near edge structure (XANES) spectroscopy and micro-X-ray fluorescence measurements. Bulk iron solubility (soluble iron/total iron) of the samples was quantified by leaching experiments. Major differences were observed in iron solubility in source emission samples, ranging from low solubility (<1%, mineral dust and coal fly ash) up to 75% (mobile exhaust and biomass burning emissions). Differences in iron solubility did not correspond to silicon content or Fe(II) content. However, source emission and ambient samples with high iron solubility corresponded to the sulfur content observed in single particles. A similar correspondence between bulk iron solubility and bulk sulfate content in a series of Atlanta PM2.5 fine particle samples (N = 358) further supported this trend. In addition, results of linear combination fitting experiments show the presence of iron sulfates in several high iron solubility source emission and ambient PM2.5 samples. These results suggest that the sulfate content (related to the presence of iron sulfates and/or acid-processing mechanisms by H(2)SO(4)) of iron-containing particles is an important proxy for iron solubility.     

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.     

Source apportionment of molecular markers and organic aerosol. 3. Food cooking emissions

The chemical mass balance model is applied to a large dataset of organic molecular marker concentrations to apportion ambient organic aerosol to food cooking emissions in Pittsburgh, Pennsylvania. Ambient concentrations of key cooking markers such as palmitoleic acid, oleic acid, and cholesterol are well correlated, which implies the existence of well-defined source profiles. However, significant inconsistencies exist between the ambient data and published source profiles. Most notably, the ambient ratio of palmitoleic-acid-to-oleic-acid is more than a factor of 10 greater than essentially all published source profiles. This problem is not unique to Pittsburgh. The reason for this discrepancy is not known but it means that both acids cannot be fit simultaneously by CMB. CMB analysis is performed using three different combinations of food cooking source profiles and molecular markers. Although all three solutions have high statistical quality, the amount of OC apportioned to food cooking emissions varies by a factor of 9. Differences in fitting species and source profile marker-to-organic-carbon ratios cause most of the large systematic biases between the different solutions. The best CMB model includes two alkanoic acids as fitting species in addition to other cooking markers, which helps constrain the source contribution estimates. It also includes two meat cooking source profiles to account for the variability in the ambient data. This model apportions 320+/-140 ng-C m(-3) or 10% of the study average ambient organic carbon to food cooking emissions. Although these results illustrate the significant challenges created by source profile variability, the strong correlations in the ambient dataset underscore the significant promise that molecular markers hold for source apportionment analysis.     

Sources of fine particles in a rural midwestern U.S. area

Ambient PM2.5 (particulate matter < or = 2.5 microm in aerodynamic diameter) samples collected at a rural monitoring site in Bondville, IL on every third day using Interagency Monitoring of Protected Visual Environments (IMPROVE) sampler were analyzed through the application of the positive matrix factorization (PMF). The particulate carbon fractions were obtained from the thermal optical reflectance method that divides particulate carbon into four organic carbon, pyrolyzed organic carbon (OP), and three elemental carbon fractions. A total of 257 samples collected between March 2001 and May 2003 analyzed for 35 species were used and eight sources were identified: summer-high secondary sulfate aerosol (40%), secondary nitrate aerosol (32%), gasoline vehicle (9%), OP-high secondary sulfate aerosol (7%), selenium-high secondary sulfate aerosol (4%), airborne soil (4%), aged sea salt (2%), and diesel emissions (2%). The compositional profiles for gasoline vehicle and diesel emissions are similar to those estimated in other U.S. areas. Backward trajectories indicate that the highly elevated airborne soil impacts were likely caused by Asian and Saharan dust storms. Potential source contribution function analyses show the potential source areas and pathways of secondary sulfate aerosols, especially the regional influences of the biogenic as well as anthropogenic secondary aerosol.