In urban environments, airborne particles are continuously emitted, followed by atmospheric aging. Also, particles emitted elsewhere, transported by winds, contribute to the urban aerosol. We studied ...the effective density (mass-mobility relationship) and mixing state with respect to the density of particles in central Copenhagen, in wintertime. The results are related to particle origin, morphology, and aging. Using a differential mobility analyzer-aerosol particle mass analyzer (DMA-APM), we determined that particles in the diameter range of 50–400 nm were of two groups: porous soot aggregates and more dense particles. Both groups were present at each size in varying proportions. Two types of temporal variability in the relative number fraction of the two groups were found: soot correlated with intense traffic in a diel pattern and dense particles increased during episodes with long-range transport from polluted continental areas. The effective density of each group was relatively stable over time, especially of the soot aggregates, which had effective densities similar to those observed in laboratory studies of fresh diesel exhaust emissions. When heated to 300 °C, the soot aggregate volatile mass fraction was ∼10%. For the dense particles, the volatile mass fraction varied from ∼80% to nearly 100%.
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IJS, KILJ, NUK, PNG, UL, UM
Soot particle (black carbon) morphology is of dual interest, both from a health perspective and due to the influence of soot on the global climate. In this study, the mass-mobility relationships, and ...thus effective densities, of soot agglomerates from three types of soot emitting sources were determined in situ by combining a differential mobility analyzer (DMA) and an aerosol particle mass analyzer (APM). High-resolution transmission electron microscopy was also used. The soot sources were diesel engines, diffusion flame soot generators, and tapered candles, operated under varying conditions. The soot microstructure was found to be similar for all sources and settings tested, with a distance between the graphene layers of 3.7-3.8 Å. The particle specific surface area was found to vary from 100 to 260 m
2
/g. The particle mass-mobility relationship could be described by a power law function with an average exponent of 2.3 (±0.1) for sources with a volatile mass fraction <10% and primary particle sizes of 11-29 nm. The diesel exhaust from a heavy duty engine at idling had a substantially higher volatile mass fraction and a higher mass-mobility exponent of 2.6. The mass-mobility exponent was essentially independent of the number of primary particles in the range covered (N
pp
= 10-1000). Despite the similar exponents, the effective density varied substantially from source to source. Two parameters were found to alter the effective density: primary particle size and coating mass fraction. A correlation was found between primary particle size and mass-mobility relationship/effective density and an empirical expression relating these parameters is presented. The effects on the DMA-APM results of doubly charged particles and DMA agglomerate alignment were investigated and quantified. Finally, the dataset was compared to three theoretical approaches describing agglomerate particles' mass-mobility relationship.
Copyright 2013 American Association for Aerosol Research
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BFBNIB, GIS, IJS, KISLJ, NUK, PNG, UL, UM, UPUK
Determination of the respiratory tract deposition of airborne particles is critical for risk assessment of air pollution, inhaled drug delivery, and understanding of respiratory disease. With the ...advent of nanotechnology, there has been an increasing interest in the measurement of pulmonary deposition of nanoparticles because of their unique properties in inhalation toxicology and medicine. Over the last century, around 50 studies have presented experimental data on lung deposition of nanoparticles (typical diameter≤100 nm, but here≤300 nm). These data show a considerable variability, partly due to differences in the applied methodologies. In this study, we review the experimental techniques for measuring respiratory tract deposition of nano-sized particles, analyze critical experimental design aspects causing measurement uncertainties, and suggest methodologies for future studies. It is shown that, although particle detection techniques have developed with time, the overall methodology in respiratory tract deposition experiments has not seen similar progress. Available experience from previous research has often not been incorporated, and some methodological design aspects that were overlooked in 30-70% of all studies may have biased the experimental data. This has contributed to a significant uncertainty on the absolute value of the lung deposition fraction of nanoparticles. We estimate the impact of the design aspects on obtained data, discuss solutions to minimize errors, and highlight gaps in the available experimental set of data.
The atmospheric effects of soot aerosols include interference with radiative transfer, visibility impairment, and alteration of cloud formation and are highly sensitive to the manner by which soot is ...internally mixed with other aerosol constituents. We present experimental studies to show that soot particles acquire a large mass fraction of sulfuric acid during atmospheric aging, considerably altering their properties. Soot particles exposed to subsaturated sulfuric acid vapor exhibit a marked change in morphology, characterized by a decreased mobility-based diameter but an increased fractal dimension and effective density. These particles experience large hygroscopic size and mass growth at subsaturated conditions (<90% relative humidity) and act efficiently as cloud-condensation nuclei. Coating with sulfuric acid and subsequent hygroscopic growth enhance the optical properties of soot aerosols, increasing scattering by almost equal to10-fold and absorption by nearly 2-fold at 80% relative humidity relative to fresh particles. In addition, condensation of sulfuric acid is shown to occur at a similar rate on ambient aerosols of various types of a given mobility size, regardless of their chemical compositions and microphysical structures. Representing an important mechanism of atmospheric aging, internal mixing of soot with sulfuric acid has profound implications on visibility, human health, and direct and indirect climate forcing.
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BFBNIB, NMLJ, NUK, PNG, SAZU, UL, UM, UPUK
Residential wood combustion is now recognized as a major particle source in many developed countries, and the number of studies investigating the negative health effects associated with wood smoke ...exposure is currently increasing. The combustion appliances in use today provide highly variable combustion conditions resulting in large variations in the physicochemical characteristics of the emitted particles. These differences in physicochemical properties are likely to influence the biological effects induced by the wood smoke particles.
The focus of this review is to discuss the present knowledge on physicochemical properties of wood smoke particles from different combustion conditions in relation to wood smoke-induced health effects. In addition, the human wood smoke exposure in developed countries is explored in order to identify the particle characteristics that are relevant for experimental studies of wood smoke-induced health effects. Finally, recent experimental studies regarding wood smoke exposure are discussed with respect to the applied combustion conditions and particle properties.
Overall, the reviewed literature regarding the physicochemical properties of wood smoke particles provides a relatively clear picture of how these properties vary with the combustion conditions, whereas particle emissions from specific classes of combustion appliances are less well characterised. The major gaps in knowledge concern; (i) characterisation of the atmospheric transformations of wood smoke particles, (ii) characterisation of the physicochemical properties of wood smoke particles in ambient and indoor environments, and (iii) identification of the physicochemical properties that influence the biological effects of wood smoke particles.
Several diesel exhaust (DE) characteristics, comprising both particle and gas phase, recognized as important when linking with health effects, are not reported in human chamber exposure studies. In ...order to understand effects of DE on humans there is a need for better characterization of DE when performing exposure studies. The aim of this study was to determine and quantify detailed DE characteristics during human chamber exposure. Additionally to compare to reported DE properties in conducted human exposures. A wide battery of particle and gas phase measurement techniques have been used to provide detailed DE characteristics including the DE particles (DEP) surface area, fraction and dose deposited in the lungs, chemical composition of both particle and gas phase such as NO, NO2, CO, CO2, volatile organic compounds (including aldehydes, benzene, toluene) and polycyclic aromatic hydrocarbons (PAHs). Eyes, nose and throat irritation effects were determined. Exposure conditions with PM1 (<1 μm) mass concentration 280 μg m−3, number concentration 4 × 105 cm−3 and elemental to total carbon fraction of 82% were generated from a diesel vehicle at idling. When estimating the lung deposited dose it was found that using the size dependent effective density (in contrast to assuming unity density) reduced the estimated respiratory dose by 132% by mass. Accounting for agglomerated structure of DEP prevented underestimation of lung deposited dose by surface area by 37% in comparison to assuming spherical particles. Comparison of DE characteristics reported in conducted chamber exposures showed that DE properties vary to a great extent under the same DEP mass concentration and engine load. This highlights the need for detailed and standardized approach for measuring and reporting of DE properties. Eyes irritation effects, most probably caused by aldehydes in the gas phase, as well as nose irritation were observed at exposure levels below current occupational exposure limit values given for exhaust fumes. Reporting detailed DE characteristics that include DEP properties (such as mass and number concentration, size resolved information, surface area, chemical composition, lung deposited dose by number, mass and surface) and detailed gas phase including components known for their carcinogenic and irritation effect (e.g. aldehydes, benzene, PAHs) can help in determination of key parameters responsible for observed health effects and comparison of chamber exposure studies.
•DE properties vary significantly under the same DEP mass concentration exposure.•Reporting detail DE characteristics is needed to explain observed health effects.•DEP agglomerated structure has to be accounted for to not underestimate lung dose by surface.•Use of size dependent effective density prevents overestimation of lung mass dose.•Gas phase components known for carcinogenic and irritation effect should be reported.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Phthalates are ubiquitous in indoor environments, which raises concern about their endocrine-disrupting properties. However, studies of human uptake from airborne exposure are limited. We studied the ...inhalation uptake and dermal uptake by air-to-skin transfer with clean clothing as a barrier of two deuterium-labeled airborne phthalates: particle-phase D4-DEHP (di(2-ethylhexyl)phthalate) and gas-phase D4-DEP (diethyl phthalate). Sixteen participants, wearing trousers and long-sleeved shirts, were under controlled conditions exposed to airborne phthalates in four exposure scenarios: dermal uptake alone and combined inhalation + dermal uptake of both phthalates. The results showed an average uptake of D4-DEHP by inhalation of 0.0014 ± 0.00088 (μg kg–1 bw)/(μg m–3)/h. No dermal uptake of D4-DEHP was observed during the 3 h exposure with clean clothing. The deposited dose of D4-DEHP accounted for 26% of the total inhaled D4-DEHP mass. For D4-DEP, the average uptake by inhalation + dermal was 0.0067 ± 0.0045 and 0.00073 ± 0.00051 (μg kg–1 bw)/(μg m–3)/h for dermal uptake. Urinary excretion factors of metabolites after inhalation were estimated to 0.69 for D4-DEHP and 0.50 for D4-DEP. Under the described settings, the main uptake of both phthalates was through inhalation. The results demonstrate the differences in uptake of gas and particles and highlight the importance of considering the deposited dose in particle uptake studies.
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IJS, KILJ, NUK, PNG, UL, UM
Today, engineered nanomaterials are frequently used. Nanosized titanium dioxide (TiO.sub.2) has been extensively used for many years and graphene is one type of emerging nanomaterial. Occupational ...airborne exposures to engineered nanomaterials are important to ensure safe workplaces and to extend the information needed for complete risk assessments. The main aim of this study was to characterize workplace emissions and exposure of graphene nanoplatelets, graphene oxide, TiO.sub.2 nanofibers (NFs) and nanoparticles (NPs) during down-stream industrial handling. Surface contaminations were also investigated to assess the potential for secondary inhalation exposures. In addition, a range of different sampling and aerosol monitoring methods were used and evaluated. The results showed that powder handling, regardless of handling graphene nanoplatelets, graphene oxide, TiO.sub.2 NFs, or NPs, contributes to the highest particle emissions and exposures. However, the exposure levels were below suggested occupational exposure limits. It was also shown that a range of different methods can be used to selectively detect and quantify nanomaterials both in the air and as surface contaminations. However, to be able to make an accurate determination of which nanomaterial that has been emitted a combination of different methods, both offline and online, must be used.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Diesel exhaust is carcinogenic and exposure to diesel particles cause health effects. We investigated the toxicity of diesel exhaust particles designed to have varying physicochemical properties in ...order to attribute health effects to specific particle characteristics. Particles from three fuel types were compared at 13% engine intake O.sub.2 concentration: MK1 ultra low sulfur diesel (DEP13) and the two renewable diesel fuels hydrotreated vegetable oil (HVO13) and rapeseed methyl ester (RME13). Additionally, diesel particles from MK1 ultra low sulfur diesel were generated at 9.7% (DEP9.7) and 17% (DEP17) intake O.sub.2 concentration. We evaluated physicochemical properties and histopathological, inflammatory and genotoxic responses on day 1, 28, and 90 after single intratracheal instillation in mice compared to reference diesel particles and carbon black. Moderate variations were seen in physical properties for the five particles: primary particle diameter: 15-22 nm, specific surface area: 152-222 m.sup.2/g, and count median mobility diameter: 55-103 nm. Larger differences were found in chemical composition: organic carbon/total carbon ratio (0.12-0.60), polycyclic aromatic hydrocarbon content (1-27 mug/mg) and acid-extractable metal content (0.9-16 mug/mg). Intratracheal exposure to all five particles induced similar toxicological responses, with different potency. Lung particle retention was observed in DEP13 and HVO13 exposed mice on day 28 post-exposure, with less retention for the other fuel types. RME exposure induced limited response whereas the remaining particles induced dose-dependent inflammation and acute phase response on day 1. DEP13 induced acute phase response on day 28 and inflammation on day 90. DNA strand break levels were not increased as compared to vehicle, but were increased in lung and liver compared to blank filter extraction control. Neutrophil influx on day 1 correlated best with estimated deposited surface area, but also with elemental carbon, organic carbon and PAHs. DNA strand break levels in lung on day 28 and in liver on day 90 correlated with acellular particle-induced ROS. We studied diesel exhaust particles designed to differ in physicochemical properties. Our study highlights specific surface area, elemental carbon content, PAHs and ROS-generating potential as physicochemical predictors of diesel particle toxicity.
The hygroscopic properties of submicron soot particles during internal mixing with gaseous sulfuric acid have been investigated using a combined tandem differential mobility analyzer (TDMA) and ...differential mobility analyzer–aerosol particle mass analyzer (DMA‐APM) technique. Fresh particles exhibit no change in mobility size and mass at subsaturated conditions, whereas particles exposed to gaseous sulfuric acid (109–1010 molecule cm−3, 12 s contact time) experience significant mobility size and mass changes with increasing relative humidity (RH). The DMA‐APM measurements reveal that particles of all sizes exposed to H2SO4 vapor gain mass with increasing RH because of absorption of water by sulfuric acid coating. However, on the basis of mobility size measurements using TDMA, upon humidification H2SO4‐coated soot agglomerates display distinct hygroscopic growth patterns depending on their initial size and the mass fraction of condensed sulfuric acid. While small particles experience an increase in their mobility sizes, larger particles exhibit a marked shrinkage due to compaction. We suggest that determination of the hygroscopic properties of soot particles using a TDMA alone can be inconclusive. Restructuring of the soot agglomerates and filling of the voids that accompany the condensation of water‐soluble materials and subsequent water absorption lead to little or no observable changes in particle mobility size at subsaturated RH even for particles that contain aqueous coatings. Extrapolation of our experimental results to the urban atmosphere indicates that initially hydrophobic soot particles acquire sufficient sulfate coating to become efficient CCN (cloud condensation nuclei) within a time period ranging from a few hours to a few days, dependent on the ambient H2SO4 level. The results imply that internal mixing with sulfuric acid through H2SO4 vapor condensation likely represents a common aging process for a variety of atmospheric aerosols. The variations in the size and hygroscopicity of soot particles during atmospheric processing influence their optical properties, cloud‐forming potential, and human health effects.
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