This study investigates the secondary organic aerosol (SOA) formation potential of carburetor motorcycles exhaust. This type of two-wheeler is a popular means of transport in many Asian cities. A volatility-based numerical model was employed to predict SOA formation from a fleet of motorcycles in Tehran, capital of Iran. The fleet was a combination of four-stroke, gasoline-powered motorcycles with different engine displacement volumes. Total hydrocarbon (THC) emission factors of all motorcycles were previously measured in a chassis dynamometer laboratory according to cold start Eum-3 emissions certification test procedures. Due to incomplete combustion and lack of control on exhaust emissions, unburned fuel was assumed to be a good surrogate for the exhaust of carburetor motorcycles, regarding SOA formation. 150 cc engine and 200 cc engine motorcycles had the highest SOA formation potential, under atmospheric oxidant concentration, while 125 cc engine motorcycles had the highest SOA emission factor (travel- and fuel-based). It was found out that SOA emission factor of 125 cc engine motorcycles could increase up to 20%, three to five years after production. Average SOA formation from carburetor motorcycles in the present study was 4 times higher than Eum-4 passenger cars and 20 times higher than direct emission of particles from Euro-2 motorcycles and on (according to EMEP/EEA levels for PM2.5 emission factors). Carburetor motorcycles with 180 cc engine volume in the present study, had the lowest SOA formation potential.
Industrial metalworking facilities emit a variety of air toxics including volatile organic compounds, polycyclic aromatic hydrocarbons (PAHs) and heavy metals. In order to investigate these emissions, a 1-month multi-instrument field campaign was undertaken at an industrial site in Grande-Synthe, Dunkirk (France), in May and June 2012. One of the main objectives of the study was to provide new information on the chemical composition of particulate matter with aerodynamic diameters smaller than 2.5 μm (PM2.5) in the vicinity of metalworking facilities. An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed to provide size-resolved chemical mixing state measurements of ambient single particles at high temporal resolution. This mixing state information was then used to apportion PM2.5 to local metalworking facilities influencing the receptor site. Periods when the site was influenced by metalworking sources were characterised by a pronounced increase in particles containing toxic metals (manganese, iron, lead) and polycyclic aromatic hydrocarbons (PAHs) with a variety of chemical mixing states. The association of specific particle classes with a nearby ferromanganese alloy manufacturing plant was confirmed through comparison with previous analysis of raw materials (ores) and chimney filter particle samples collected at the facility. Particles associated with emissions from a nearby steelworks were also identified. The contribution of local metalworking activities to PM2.5 at the receptor site for the period when the ATOFMS was deployed ranged from 1 to 65% with an average contribution of 17%, while the remaining mass was attributed to other local and regional sources. These findings demonstrate the impact of metalworking facilities on air quality downwind and provide useful single particle signatures for future source apportionment studies in communities impacted by metalworking emissions.
Abstract While the importance of supermicron particles on human health and climate is well recognized, knowledge of their size‐related properties remains elusive. Many routine near‐surface in situ measurements of aerosol properties include size spectra of submicron particles and aerosol total scattering coefficient at three visible wavelengths and two size cutoffs. These properties are collected, for example, at the U.S. Department of Energy's Atmospheric Radiation Measurement (ARM) user facility. Our study illustrates how these conventional measurements can be used to predict total particle volume (particle size <10 μm). The well‐known fact that small and large particles scatter sunlight very differently forms the basis of a new method. Our study demonstrates a good agreement between estimated and measured total volumes for five climate‐important locations. The agreement suggests that the new method can be used to predict the total particle volume from the routine data collected at numerous sites around the world.
Abstract Introduction There are fundamental differences between electronic cigarettes (e-cigarettes) and conventional cigarette product categories with regards to potential environmental exposures, notably that e-cigarettes do not contain tobacco or generate side-stream emissions. Here we assess the spatial and temporal patterns of exhaled e-cigarette aerosol at a bystander’s position, and compare it with conventional cigarette smoke emissions. Methods Smokers were asked to use e-cigarettes or smoke conventional cigarettes in a room-simulating chamber. Volunteers used the products at different distances from a heated mannequin, representing a bystander, and under different room ventilation rates. Aerosol particle concentrations and size distributions at the bystander’s position were measured. Results For both product categories, the particle concentrations registered following each puff were in the same order of magnitude. However, for e-cigarettes the particle concentration returned rapidly to background values within seconds; for conventional cigarettes it increased with successive puffs, returning to background levels after 30–45 minutes. Unlike for the e-cigarette devices tested, such temporal variation was dependent on the room ventilation rate. Particle size measurements showed that exhaled e-cigarette particles were smaller than those emitted during smoking conventional cigarettes and evaporated almost immediately after exhalation, thus affecting the removal of particles through evaporation rather than displacement by ventilation. Conclusions Significant differences between emissions from the tested e- and conventional cigarettes are reported. Exhaled e-cigarette particles are liquid droplets evaporating rapidly; conventional cigarette smoke particles are far more stable and linger. Implications • Several factors potentially influencing particle behavior after exhalation of e-cigarette aerosols or emitted during smoking conventional cigarettes were studied. • Differences in particle size between those exhaled following use of e-cigarettes and those emitted during smoking of conventional cigarettes were observed. • E-cigarette particle concentrations decreased rapidly following exhalation due to evaporation. • The removal of particles following smoking conventional cigarettes was much slower and was dependent on the room ventilation rate.
In a context where a significant fraction of the population lives near industrial areas, the main objectives of this study are to provide (a) new data on PM2.5 chemical compositions, heavy-metal concentrations and trace gases released by metalworking activities and (b) new information on the near-field evolution (up to about a thousand meters) of such industrial plumes in terms of particle chemical composition and size distribution. For that purpose, a one-month field campaign was performed in an industrial area near the city of Dunkirk (Northern France), combining measurements of atmospheric dynamics and physico-chemical characterization of air masses. Comparisons between several elemental ratios (mainly Mn/Fe), particle size distributions and volatile organic compound (VOC) concentrations at the stacks and at a near-field site suggest that plumes of a ferromanganese alloy plant were quickly mixed with pollutants emitted by other sources (mainly other industries, possibly traffic and sea spray), in particular a neighboring steelworks, before reaching the sampling site. This led to the emergence of secondary particles related to condensation and/or aggregation phenomena inside the plumes. Metalworking emissions were also identified as a source of new particle formation, formed through the emission of gaseous precursors and their fast transformation and condensation, over a timescale of minutes before reaching the near-field site 800 m downwind. Ultrafine particles emitted at the stacks also quickly agglomerated to form larger particles before reaching the near-field site. These results show that, even over short distances, the chemical composition and size distribution of metalworking plumes may evolve rapidly and the characteristics of particles at the boundary of an industrial area (especially in contiguous urban areas) may differ from those emitted directly at the stacks.
PM2.5 pollution has become a global health concern, however its size-resolved health impact remains to be poorly elucidated. Here, ambient particulate matter (PM) were collected into 13 different size ranges (10 nm to 18 μm) and the mass, metal, endotoxin distributions, and related oxidative potential were investigated in two regions (Zürich, Switzerland and Beijing, China). Results showed that the two regions had remarkably different PM distribution patterns. Swiss urban samples had a mode around 40 nm with 23.3% of total PM mass, while Chinese samples featured two modes around 0.75 and 4.23 μm with 13.8-18.6% and 13.7-20.4% of total PM mass, respectively. Two peaks for endotoxin at 40-100 nm and 1-4 μm were observed in different regions. For PM-borne metals, Chinese samples had 67.6-100% of total Cd, As, and Pb in the size range of 0.1-1 μm, and Swiss samples had similar distributions of Cd and Pb but much lower total metals than Chinese samples. The PM oxidative potential varied greatly with sizes for different regions. Accordingly, the current practice, i.e., sole use of the mass concentration, could lead to inadequate health protection for one region, but unnecessary economic costs for another without achieving significant extra health benefits.
Multi-wavelength in situ aerosol extinction, absorption and scattering measurements made at two ground sites during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) are analyzed using a spectral deconvolution method that allows extraction of particle-size-related information, including the fraction of extinction produced by the fine-mode particles and the effective radius of the fine mode. The spectral deconvolution method is typically applied to analysis of remote sensing measurements. Here, its application to in situ measurements allows for comparison with more direct measurement methods and validation of the retrieval approach. Overall, the retrieved fine-mode fraction and effective radius compare well with other in situ measurements, including size distribution measurements and scattering and absorption measurements made separately for PM1 and PM10, although there were some periods during which the different methods yielded different results. One key contributor to differences between the results obtained is the alternative, spectrally based definitions of fine and coarse modes from the optical methods, relative to instruments that use a physically defined cut point. These results indicate that for campaigns where size, composition and multi-wavelength optical property measurements are made, comparison of the results can result in closure or can identify unusual circumstances. The comparison here also demonstrates that in situ multi-wavelength optical property measurements can be used to determine information about particle size distributions in situations where direct size distribution measurements are not available.
Mounting evidence from field and laboratory observations coupled with atmospheric model analyses shows that primary combustion emissions of organic compounds dynamically partition between the vapor and particulate phases, especially as near-source emissions dilute and cool to ambient conditions. The most recent version of the Community Multiscale Air Quality model version 5.2 (CMAQv5.2) accounts for the semivolatile partitioning and gas-phase aging of these primary organic aerosol (POA) compounds consistent with experimentally derived parameterizations. We also include a new surrogate species, potential secondary organic aerosol from combustion emissions (pcSOA), which provides a representation of the secondary organic aerosol (SOA) from anthropogenic combustion sources that could be missing from current chemical transport model predictions. The reasons for this missing mass likely include the following: (1) unspeciated semivolatile and intermediate volatility organic compound (SVOC and IVOC, respectively) emissions missing from current inventories, (2) multigenerational aging of organic vapor products from known SOA precursors (e.g., toluene, alkanes), (3) underestimation of SOA yields due to vapor wall losses in smog chamber experiments, and (4) reversible organic compounds-water interactions and/or aqueous-phase processing of known organic vapor emissions. CMAQ predicts the spatially averaged contribution of pcSOA to OA surface concentrations in the continental United States to be 38.6 and 23.6 % in the 2011 winter and summer, respectively. Whereas many past modeling studies focused on a particular measurement campaign, season, location, or model configuration, we endeavor to evaluate the model and important uncertain parameters with a comprehensive set of United States-based model runs using multiple horizontal scales (4 and 12 km), gas-phase chemical mechanisms, and seasons and years. The model with representation of semivolatile POA improves predictions of hourly OA observations over the traditional nonvolatile model at sites during field campaigns in southern California (CalNex, May-June 2010), northern California (CARES, June 2010), the southeast US (SOAS, June 2013; SEARCH, January and July, 2011). Model improvements manifest better correlations (e.g., the correlation coefficient at Pasadena at night increases from 0.38 to 0.62) and reductions in underprediction during the photochemically active afternoon period (e.g., bias at Pasadena from -5.62 to -2.42 μg m-3). Daily averaged predictions of observations at routine-monitoring networks from simulations over the continental US (CONUS) in 2011 show modest improvement during winter, with mean biases reducing from 1.14 to 0.73μg m-3, but less change in the summer when the decreases from POA evaporation were similar to the magnitude of added SOA mass. Because the model-performance improvement realized by including the relatively simple pcSOA approach is similar to that of more-complicated parameterizations of OA formation and aging, we recommend caution when applying these more-complicated approaches as they currently rely on numerous uncertain parameters. The pcSOA parameters optimized for performance at the southern and northern California sites lead to higher OA formation than is observed in the CONUS evaluation. This may be due to any of the following: variations in real pcSOA in different regions or time periods, too-high concentrations of other OA sources in the model that are important over the larger domain, or other model issues such as loss processes. This discrepancy is likely regionally and temporally dependent and driven by interferences from factors like varying emissions and chemical regimes.
Composite materials with fibrous reinforcement often provide superior mechanical, thermal, electrical and optical properties than the matrix. Asbestos, carbon fibers and carbon nanotubes (CNTs) have been widely used in composites with profound impacts not only on technology and economy but also on human health and environment. A large number of studies have been dedicated to the release of fibrous particles from composites. Here we focus on the transformation of the fibrous fillers after their release, especially the change of the properties essential for the health impacts. Asbestos fibers exist in a large number of products and the end-of-the-life treatment of asbestos-containing materials poses potential risks. Thermal treatment can transform asbestos to non-hazardous phase which provides opportunities of safe disposal of asbestos-containing materials by incineration, but challenges still exist. Carbon fibers with diameters in the range of 5–10 μm are not considered to be respirable, however, during the release process from composites, the carbon fibers may be split along the fiber axis, generating smaller and respirable fibers. CNTs may be exposed on the surface of the composites or released as free standing fibers, which have lengths shorter than the original ones. CNTs have high thermal stability and may be exposed after thermal treatment of the composites and still keep their structural integrity. Due to the transformation of the fibrous fillers during the release process, their toxicity may be significantly different from the virgin fibers, which should be taken into account in the risk assessment of fiber-containing composites.
We present the evolution of multispectral optical properties through urban aerosols that have aged and interacted with biogenic emissions, resulting in stronger short wavelength absorption and the formation of moderately brown secondary organic aerosols. Ground-based aerosol measurements were made in June 2010 within the Sacramento urban area (site T0) and at a 40-km downwind location (site T1) in the forested Sierra Nevada foothills area. Data on black carbon (BC) and non-refractory aerosol mass and composition were collected at both sites. In addition, photoacoustic (PA) instruments with integrating nephelometers were used to measure spectral absorption and scattering coefficients for wavelengths ranging from 355 to 870 nm. The daytime absorption Ångström exponent (AAE) indicated a modest wavelength-dependent enhancement of absorption at both sites throughout the study. From 22 to 28 June 2010, secondary organic aerosol mass increased significantly at both sites, which was due to increased biogenic emissions coupled with intense photochemical activity and air mass recirculation in the area. During this period, the median BC mass-normalized absorption cross-section (MAC) values for 405 nm and 532 nm at T1 increased by ~23% and ~35%, respectively, compared with the relatively less aged urban emissions at the T0 site. In contrast, the average MAC values for the 870 nm wavelength were similar for both sites. These results suggest the formation of moderately brown secondary organic aerosols in biogenically-influenced urban air.
Aviation is a substantial and a fast growing emissions source. Besides greenhouse gases, aircraft engines emit black carbon (BC), a climate forcer and air pollutant. Aviation BC emissions have been regulated and estimated through exhaust smoke visibility (smoke number). Their impacts are poorly understood because emission inventories lack representative data. Here, we measured BC mass and number-based emissions of the most popular airliner's engines according to a new emission standard. We used a calibrated engine performance model to determine the emissions on the ground, at cruise altitude, and over entire flight missions. Compared to previous estimates, we found up to a factor of 4 less BC mass emitted from the standardized landing and takeoff cycle and up to a factor of 40 less during taxiing. However, the taxi phase accounted for up to 30% of the total BC number emissions. Depending on the fuel composition and flight distance, the mass and number-based emission indices (/kg fuel burned) were 6.2-14.7 mg and 2.8 × 1014 - 8.7 × 1014, respectively. The BC mass emissions per passenger-km were similar to gasoline vehicles, but the number-based emissions were relatively higher, comparable to old diesel vehicles. This study provides representative data for models and will lead to more accurate assessments of environmental impacts of aviation.
Nonmethane organic gas emissions (NMOGs) from in-service aircraft turbine engines were investigated using a proton transfer reaction time-of-flight mass spectrometer (PTR-ToF-MS) at an engine test facility at Zurich Airport, Switzerland. Experiments consisted of 60 exhaust samples for seven engine types (used in commercial aviation) from two manufacturers at thrust levels ranging from idle to takeoff. Emission indices (EIs) for more than 200 NMOGs were quantified, and the functional group fractions (including acids, carbonyls, aromatics, and aliphatics) were calculated to characterize the exhaust chemical composition at different engine operation modes. Total NMOG emissions were highest at idling with an average EI of 7.8 g/kg fuel and were a factor of ∼40 lower at takeoff thrust. The relative contribution of pure hydrocarbons (particularly aromatics and aliphatics) of the engine exhaust decreased with increasing thrust while the fraction of oxidized compounds, for example, acids and carbonyls increased. Exhaust chemical composition at idle was also affected by engine technology. Older engines emitted a higher fraction of nonoxidized NMOGs compared to newer ones. Idling conditions dominated ground level organic gas emissions. Based on the EI determined here, we estimate that reducing idle emissions could substantially improve air quality near airports.
A field campaign has been performed in two municipal solid waste incineration (MSWI) plants in Switzerland, at Hinwil (ZH) and Giubiasco (TI). The aim was to measure airborne pollutants at different locations of the abatement systems (including those released from the stacks into the atmosphere) and at a near-field (similar to 1 km) downwind site, in order to assess the efficiency of the abatement systems and the environmental impact of these plants.During this study, we measured the particle number concentration with a condensation particle counter (CPC), and the size distribution with a scanning mobility particle sizer (SMPS) and an aerodynamic particle sizer (APS). We also sampled particles on filters for subsequent analyses of the morphology, size and elemental composition with a scanning electron microscope coupled to an energy dispersive X-ray spectroscope (SEM/EDX), and of water soluble ions by ion chromatography (IC). Finally, volatile organic compounds (VOCs) were sampled on adsorbing cartridges and analyzed by thermal desorption-gas chromatography/mass spectrometry (TD-GC/MS), and a portable gas analyzer was used to monitor NO, SO2, CO, CO2, and O-2.The particle concentration decreased significantly at two locations of the plants: at the electrostatic precipitator and the bag-house filter. The particle concentrations measured at the stacks were very low (<100 #/cm(3)), stressing the efficiency of the abatement system of the two plants. At Hinwil, particles sampled at the stack were mainly constituted of NaCI and KCI, two salts known to be involved in the corrosion process in incinerators. At Giubiasco, no significant differences were observed for the morphology and chemical composition of the particles collected in the ambient background and at the downwind site, suggesting that the incineration plant released very limited amounts of particles to the surrounding areas. (C) 2017 Elsevier Ltd. All rights reserved.
Particulate matter emissions from aircraft gas turbines are a concern for human health, environmental degradation and climate change. Understanding the effect of aromatics in the fuel on non-volatile particle matter (nvPM) emissions is important for establishing future regulations and for assessing potential emission abatement strategies that intend to change fuel feedstock. This work presents non-volatile PM mass and number emission indices (EIs, mass or number nvPM/ mass fuel) as a function of fuel aromatic content for two measurement campaigns (Aircraft Particulate Regulatory Instrumentation Demonstration Experiments (A-PRIDE) 7 and 8 with an aircraft gas turbine source run in the test cell of SR Technics, Zurich airport. The nvPM sampling system and system operation corresponded to the recommended practice (SAE International, 2013). The fuel (JET A-1) total aromatics level was changed by a controlled injection of two aromatic solvents into the fuel supply line to the engine. The two aromatic solvents were Solvesso 150 and Solvesso 150ND, of which the first one contained 6 % by volume naphthalenes and the second one was naphthalenes depleted (< 0.3%). Besides the unmixed fuel that had a total aromatic content of 17.8% by volume, three fuel blending ratios ranging from 22.5% to 24.7% by volume in total aromatic content were tested for each solvent at various engine thrust points ranging from idle to take-off. The results show an increase in nvPM mass and number EIs with increasing fuel aromatics content (Figure 1).
The chemical composition of single particles deposited on industrial filters located in three different chimneys of an iron-manganese (Fe-Mn) alloy manufacturing plant have been compared using aerosol time-of-flight mass spectrometry (ATOFMS) and scanning electron microscopy-energy dispersive X-ray spectrometry (SEM-EDX). Very similar types of particles were observed using both analytical techniques. Calcium-containing particles dominated in the firing area of the sintering unit, Mn and/or Al-bearing particles were observed at the cooling area of the sintering unit, while Mn-containing particles were dominant at the smelting unit. SEM-EDX analysis of particles collected downstream of the industrial filters showed that the composition of the particles emitted from the chimneys is very similar to those collected on the filters. ATOFMS analysis of ore samples was also performed to identify particulate emissions that could be generated by wind erosion and manual activities. Specific particle types have been identified for each emission source (chimneys and ore piles) and can be used as tracers for source apportionment of ambient PM measured in the vicinity of the industrial site.
A field campaign has been performed in two municipal solid waste incineration plants in Switzerland, at Giubiasco (TI) and Hinwil (ZH). The aim was to measure airborne pollutants at different locations of the abatement systems and those released from the stacks into the atmosphere, in order to assess the efficiency of the abatement systems and the environmental impact of these plants. Both incineration plants were equipped with an electrostatic precipitator, a DeNOx system based on the selective catalytic reduction (SCR) technology, and a bag-house filter. The main differences between the two plants were 1) the presence of a dry scrubber at Hinwil and a wet scrubber at Giubiasco, and 2) the location of the bag-house filters within the abatement system (last step of abatement at Giubiasco, between the dry scrubber and the DeNOx at Hinwil). Measurements were performed at different locations of the abatement system of the two plants, and additional measurements were undertaken at a near-field (~ 1 km) downwind site at Giubiasco. During this study, we deployed a large set of instruments to measure the particle number concentration and size distribution. We also sampled particles on filters for subsequent analyses of the morphology, size, elemental composition, and water soluble anions. Finally, volatile organic compounds (VOCs) and trace gases (NO, SO2, CO, CO2, and O2) were also measured. The particle concentration decreased significantly at two locations of the plants: at the electrostatic precipitator and the bag-house filter, while the DeNOx system removed up to 97% of the nitrogen oxides. The particle concentrations measured at the stacks were very low (< 100 #/cm), stressing the efficiency of the abatement system of the two plants. Particles released from the stacks had a relatively uniform shape and size, and were possibly constituted of ammonium chloride salts. We did not see considerable amount of this type of particles at the near-field downwind site of Giubiasco, and the concentrations of chloride were rather low there, suggesting that the incineration plants released very limited amounts of particles to the surrounding areas.
Measurements of the effect of water uptake on particulate light extinction or scattering made at two locations during the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES) study around Sacramento, CA are reported. The observed influence of water uptake, characterized through the dimensionless optical hygroscopicity parameter γ, is compared with calculations constrained by observed particle size distributions and size-dependent particle composition. A closure assessment has been carried out that allowed for determination of the average hygroscopic growth factors (GFs) at 85% relative humidity and the dimensionless hygroscopicity parameter κ for oxygenated organic aerosol (OA) and for supermicron particles (defined here as particles with aerodynamic diameters between 1 and 2.5 microns), yielding κ = 0.1–0.15 and 0.9–1.0, respectively. The derived range of oxygenated OA κ values are in line with previous observations. The relatively large values for supermicron particles is consistent with substantial contributions of sea-salt-containing particles in this size range. Analysis of time-dependent variations in the supermicron particle hygroscopicity suggest that atmospheric processing, specifically chloride displacement by nitrate and the accumulation of secondary organics on supermicron particles, can lead to substantial depression of the observed GF.