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•Comparison of heated tobacco product (HTP), e-cig and cigarette toxicity is lacking.•HTP emits lesser carbonyls and PAHs than cigarette but more than e-cig.•Cytotoxicity of HTP is ...lower than that of cigarette but stronger than that of e-cig.•Increasing e-cig power impacts toxic compound levels and related oxidative stress.•All devices have the potential to induce oxidative stress and inflammatory response.
The electronic cigarettes (e-cigs) and more recently the heated tobacco products (HTP) provide alternatives for smokers as they are generally perceived to be less harmful than conventional cigarettes. However, it is crucial to compare the health risks of these different emergent devices, in order to determine which product should be preferred to substitute cigarette. The present study aimed to compare the composition of emissions from HTP, e-cigs and conventional cigarettes, regarding selected harmful or potentially harmful compounds, and their toxic impacts on the human bronchial epithelial BEAS-2B cells. The HTP emitted less polycyclic aromatic hydrocarbons and carbonyls than the conventional cigarette. However, amounts of these compounds in HTP aerosols were still higher than in e-cig vapours. Concordantly, HTP aerosol showed reduced cytotoxicity compared to cigarette smoke but higher than e-cig vapours. HTP and e-cig had the potential to increase oxidative stress and inflammatory response, in a manner similar to that of cigarette smoke, but after more intensive exposures. In addition, increasing e-cig power impacted levels of certain toxic compounds and related oxidative stress. This study provides important data necessary for risk assessment by demonstrating that HTP might be less harmful than tobacco cigarette but considerably more harmful than e-cig.
Terpenoids have long been known to originate from natural sources. However, there is growing evidence for emissions from anthropogenic activities in cities, in particular from the production, ...manufacturing, and use of household solvents. Here, as part of the DATAbASE (Do Anthropogenic Terpenoids mAtter in AtmoSpheric chEmistry?) project, we investigate for the first time the potential role of industrial activities on the terpenoid burden in the urban atmosphere. This study is based on continuous VOC observations from an intensive field campaign conducted in July 2014 at an industrial-urban background site located in Dunkirk, Northern France. More than 80 VOCs including oxygenated and terpenoid compounds were measured by on-line Thermal Desorption Gas Chromatography with a Flame Ionization Detection (TD-GC-FID) and Proton Transfer Reaction-Time of Flight Mass Spectrometry (PTR-ToFMS). Isoprene, α-pinene, limonene and the sum of monoterpenes were the terpenoids detected at average mixing ratios of 0.02 ± 0.02 ppbv, 0.02 ± 0.02 ppbv, 0.01 ± 0.01 ppbv and 0.03 ± 0.05 ppbv, respectively. Like other anthropogenic VOCs, the mixing ratios of terpenoids significantly increase downwind the industrial plumes by one order of magnitude. Positive Matrix Factorization (PMF) was performed to identify the different emission sources of VOCs and their contribution. Six factors out of the eight factors extracted (r2 = 0.95) are related to industrial emissions such as solvent use, chemical and agrochemical storage, metallurgy, petrochemical, and coal-fired industrial activities. From the correlations between the industrial-type PMF factors, sulfur dioxide, and terpenoids, we determined their emissions ratios and we quantified for the first time their industrial emissions. The highest emission ratio is related to the alkene-dominated factor and is related to petrochemical, metallurgical and coal-fired industrial activities. The industrial emissions of monoterpenes equal 8.1 ± 4.3 tons/year. Those emissions are as significant as the non-industrialized anthropogenic ones estimated for the Paris megacity.
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•PMF source- apportionment is performed on VOC in an urban-industrial area, Dunkirk.•6 out of 8 PMF factors are associated to mixed industrial sources.•Terpenoids correlate with mixed industrial factors downwind the industrial sector.•The industrial emission ratios of terpenoids are determined.•The industrial emissions of monoterpenes are quantified: they are significant.
•In situ DRIFT spectroscopy was employed to monitor the dust surface.•XRF, XRD and ICP-MS analyses were used for the chemical characterization of dusts.•Particles Size and the Ca/Si ratio could ...determine water adsorption onto dust.•At ambient relative humidity, natural mineral samples are always covered with water.
The adsorption of water molecules on natural mineral dusts was investigated employing in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). The natural dust samples originated from North and West Africa, Saudi Arabia and Gobi desert regions. Furthermore, the hygroscopicity of commercially available Arizona Test Dusts (ATDs) and Icelandic volcanic ash were examined. N2 sorption measurements, X-ray fluorescence and diffraction (XRF and XRD), as well as Inductively Coupled Plasma Mass Spectrometry (ICP-MS) analyses were performed to determine the physicochemical properties of the particles. The water adsorption experiments were conducted in an optical cell, at room temperature under the relative humidity (RH) range of 1.9–95%. Results were simulated using a modified three-parameter Brunauer-Emmett-Teller (BET) equation. Water monolayer (ML) was formed in the RH range of 15–25%, while additional water layers were formed at higher RH. Besides, the standard adsorption enthalpies of water onto natural mineral dust samples were determined. A thorough comparison of two commercially available ATD samples indicated that size distribution and/or porosity should play a key role in particle hygroscopicity. Regarding the natural mineral particles, Ca/Si ratios, and to a lesser extent Al/Si, Na/Si, Mg/Si ratios, were found to impact the minimum RH level required for water monolayer formation. These results suggest that the hygroscopic properties of investigated African dusts are quite similar over the whole investigated RH range. Furthermore, one of the major conclusions is that under most atmospheric relative humidity conditions, natural mineral samples are always covered with at least one layer of adsorbed water.
This study presents the first long-term online measurements of submicron (PM1) particles at the ATOLL (ATmospheric Observations in liLLe) platform, in northern France. The ongoing measurements using ...an Aerosol Chemical Speciation Monitor (ACSM) started at the end of 2016 and the analysis presented here spans through December 2020. At this site, the mean PM1 concentration is 10.6 μg m−3, dominated by organic aerosols (OA, 42.3%) and followed by nitrate (28.9%), ammonium (12.3%), sulfate (8.6%), and black carbon (BC, 8.0%). Large seasonal variations of PM1 concentrations are observed, with high concentrations during cold seasons, associated with pollution episodes (e.g. over 100 μg m−3 in January 2017). To study OA origins over this multiannual dataset we performed source apportionment analysis using rolling positive matrix factorization (PMF), yielding two primary OA factors, a traffic-related hydrocarbon-like OA (HOA) and biomass-burning OA (BBOA), and two oxygenated OA (OOA) factors. HOA showed a homogeneous contribution to OA throughout the seasons (11.8%), while BBOA varied from 8.1% (summer) to 18.5% (winter), the latter associated with residential wood combustion. The OOA factors were distinguished between their less and more oxidized fractions (LO-OOA and MO-OOA, on average contributing 32% and 42%, respectively). During winter, LO-OOA is identified as aged biomass burning, so at least half of OA is associated with wood combustion during this season. Furthermore, ammonium nitrate is also a predominant aerosol component during cold-weather pollution episodes – associated with fertilizer usage and traffic emissions. This study provides a comprehensive analysis of submicron aerosol sources at the recently established ATOLL site in northern France from multiannual observations, depicting a complex interaction between anthropogenic and natural sources, leading to different mechanisms of air quality degradation in the region across different seasons.
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•Pollution episodes at ATOLL are dominated by organics (OA) and nitrate in the PM1.•Multiannual source apportionment of OA yields high dominance of oxidized OA (74%).•During winter, primary and aged wood combustion dominates OA (>50%).•Pollution levels are strongly enhanced by continental air masses from Central Europe.
Seasonal variability of non-refractory PM1 (NR-PM1) was studied at a rural background site (National Atmospheric Observatory Košetice – NAOK) in the Czech Republic to investigate the effect of ...regional and long-range atmospheric transport in central Europe. NR-PM1 measurements were performed by compact time-of-flight aerosol mass spectrometry (C-ToF-AMS), and the chemically speciated mass size distributions, density, shape, and origin were discussed. Average PM1 concentrations, calculated as the sum of the NR-PM1 and the equivalent black carbon (eBC) concentrations measured by an aethalometer (AE), were 8.58 ± 3.70 µg m-3 in summer and 10.08 ± 8.04 µg m-3 in winter. Organics were dominant during both campaigns (summer/winter: 4.97 ± 2.92/4.55 ± 4.40 µg m-3), followed by SO42-in summer (1.68 ± 0.81/1.36 ± 1.38 µg m-3) and NO3- in winter (0.67 ± 0.38/2.03 ± 1.71 µg m-3). The accumulation mode dominated the average mass size distribution during both seasons, with larger particles of all species measured in winter (mode diameters: Org: 334/413 nm, NO3-: 377/501 nm, SO42-: 400/547 nm, and NH4+: 489/515 nm) indicating regional and long-range transport. However, since the winter aerosols were less oxidized than the summer aerosols (comparing fragments f44 and f43), the importance of local sources in the cold part of the year was still enough to be considered. Although aged continental air masses from the south-east (SE) were rare in summer (7 %), they were related to the highest concentrations of PM1, eBC, and all NR-PM1 species, especially SO42- and NH4+. In winter, slow continental air masses from the south-west (SW) (44 %) were linked to inversion conditions over central Europe and were associated with the highest concentrations among all NR-PM1 species as well as PM1 and eBC. Average PM1 material density (ρm) corresponded to higher inorganic contents in both seasons (summer: ∼ 1.30 g cm-3 and winter: ∼ 1.40 g cm-3). During episodes of higher mass concentrations ρm ranged from 1.30–1.40 g cm-3 in summer and from 1.30–1.50 g cm-3 in winter. The dynamic shape factors (χ) decreased slightly with particle mobility diameter (Dm) in both seasons. This study provides insights into the seasonal effects and air mass variability on aerosol particles, focusing on episodes of high mass and number concentrations measured at a central European rural background site.
A growing number of studies are using specific primary sugar species, such as sugar alcohols or primary saccharides, as marker compounds to characterize and apportion primary biogenic organic ...aerosols (PBOAs) in the atmosphere. To better understand their annual cycles, as well as their spatiotemporal abundance in terms of concentrations and sources, we conducted a large study focusing on three major atmospheric primary sugar compounds (i.e., arabitol, mannitol, and glucose) measured in various environmental conditions for about 5300 filter samples collected at 28 sites in France. Our results show significant atmospheric concentrations of polyols (defined here as the sum of arabitol and mannitol) and glucose at each sampling location, highlighting their ubiquity. Results also confirm that polyols and glucose are mainly associated with the coarse rather than the fine aerosol mode. At nearly all sites, atmospheric concentrations of polyols and glucose display a well-marked seasonal pattern, with maximum concentrations from late spring to early autumn, followed by an abrupt decrease in late autumn, and a minimum concentration during wintertime. Such seasonal patterns support biogenic emissions associated with higher biological metabolic activities (sporulation, growth, etc.) during warmer periods. Results from a previous comprehensive study using positive matrix factorization (PMF) based on an extended aerosol chemical composition dataset of up to 130 species for 16 of the same sample series have also been used in the present work. The polyols-to-PMPBOA ratio is 0.024±0.010 on average for all sites, with no clear distinction between traffic, urban, or rural typology. Overall, even if the exact origin of the PBOA source is still under investigation, it appears to be an important source of particulate matter (PM), especially during summertime. Results also show that PBOAs are significant sources of total organic matter (OM) in PM10 (13±4 % on a yearly average, and up to 40 % in some environments in summer) at most of the investigated sites. The mean PBOA chemical profile is clearly dominated by contribution from OM (78±9 % of the mass of the PBOA PMF on average), and only a minor contribution from the dust class (3±4 %), suggesting that ambient polyols are most likely associated with biological particle emissions (e.g., active spore discharge) rather than soil dust resuspension.
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.
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•Particles assigned to a ferromanganese facility and a steelworks based on composition.•Metalworking particle composition and mixing state is complex and diverse.•Metalworking emissions contributed 17% to PM2.5 on average at the receptor site.•Metalworking is the dominant source of metals and polycyclic aromatic hydrocarbons.
According to the literature, tiny amounts of transition metals in airborne fine particles (PM2.5) may induce proinflammatory cell response through reactive oxygen species production. The solubility ...of particle-bound metals in physiological fluids, i.e. the metal bioaccessibility is driven by factors such as the solution chemical composition, the contact time with the particles, and the solid-to-liquid phase ratio (S/L). In this work, PM2.5-bound metal bioaccessibility was assessed in various physiological-like solutions including cell culture media in order to evidence the potential impact on normal human bronchial epithelial cells (NHBE) when studying the cytotoxicity and inflammatory responses of PM2.5 towards the target bronchial compartment. Different fluids (H2O, PBS, LHC-9 culture medium, Gamble and human respiratory mucus collected from COPD patients), various S/L conditions (from 1/6000 to 1/100,000) and exposure times (6, 24 and 72h) were tested on urban PM2.5 samples. In addition, metals’ total, soluble and insoluble fractions from PM2.5 in LHC-9 were deposited on NHBE cells (BEAS-2B) to measure their cytotoxicity and inflammatory potential (i.e., G6PDH activity, secretion of IL-6 and IL-8). The bioaccessibility is solution-dependent. A higher salinity or organic content may increase or inhibit the bioaccessibiliy according to the element, as observed in the complex mucus matrix. Decreasing the S/L ratio also affect the bioaccessibility depending on the solution tested while the exposure time appears less critical. The LHC-9 culture medium appears to be a good physiological proxy as it induces metal bioaccessibilities close to the mucus values and is little affected by S/L ratios or exposure time. Only the insoluble fraction can be linked to the PM2.5-induced cytotoxicity. By contrast, both soluble and insoluble fractions can be related to the secretion of cytokines. The metal bioaccessibility in LHC-9 of the total, soluble, and insoluble fractions of the PM2.5 under study did not explain alone, the cytotoxicity nor the inflammatory response observed in BEAS-2B cells. These findings confirm the urgent need to perform further toxicological studies to better evaluate the synergistic effect of both bioaccessible particle-bound metals and organic species.
•Bioaccessibility of atmospheric particle-bond metals in cell culture media.•First bioaccessible test in pulmonary mucus from actual patients.•Soluble and insoluble fractions of PM2.5 are linked to cytotoxicity and inflammation.•Needs for organic and metal bioaccessibility assays to assess soluble toxicology.
Here we report results of a detailed analysis of the urban and non-urban
contributions to particulate matter (PM) concentrations and source contributions in five European
cities, namely Schiedam (the ...Netherlands, NL), Lens (France, FR), Leipzig
(Germany, DE), Zurich (Switzerland, CH) and Barcelona (Spain, ES). PM
chemically speciated data from 12 European paired monitoring sites (one
traffic, five urban, five regional and one continental background) were analysed by
positive matrix factorisation (PMF) and Lenschow's approach to assign
measured PM and source contributions to the different spatial levels. Five
common sources were obtained at the 12 sites: sulfate-rich (SSA) and nitrate-rich (NSA) aerosols,
road traffic (RT), mineral matter (MM), and aged sea salt (SS). These sources explained from 55 % to 88 % of PM
mass at urban low-traffic-impact sites (UB) depending on the country. Three
additional common sources were identified at a subset of sites/countries,
namely biomass burning (BB) (FR, CH and DE), explaining an additional 9 %–13 % of PM
mass, and residual oil combustion (V–Ni) and primary industrial (IND) (NL and ES), together explaining an additional
11 %–15 % of PM mass. In all countries, the majority of PM measured at UB
sites was of a regional+continental (R+C) nature (64 %–74 %). The R+C PM
increments due to anthropogenic emissions in DE, NL, CH, ES and FR
represented around 66 %, 62 %, 52 %, 32 % and 23 %, respectively,
of UB PM mass. Overall, the R+C PM increments due to natural and
anthropogenic sources showed opposite seasonal profiles with the former
increasing in summer and the latter increasing in winter, even if exceptions
were observed. In ES, the anthropogenic R+C PM increment was higher in
summer due to high contributions from regional SSA and V–Ni sources, both
being mostly related to maritime shipping emissions at the Spanish sites.
Conversely, in the other countries, higher anthropogenic R+C PM increments
in winter were mostly due to high contributions from NSA and BB regional
sources during the cold season. On annual average, the sources showing
higher R+C increments were SSA (77 %–91 % of SSA source contribution at the
urban level), NSA (51 %–94 %), MM (58 %–80 %), BB (42 %–78 %) and IND (91 %
in NL). Other sources showing high R+C increments were photochemistry and coal combustion (97 %–99 %;
identified only in DE). The highest regional SSA increment was observed in
ES, especially in summer, and was related to ship emissions, enhanced
photochemistry and peculiar meteorological patterns of the Western
Mediterranean. The highest R+C and urban NSA increments were observed in
NL and associated with high availability of precursors such as NOx and
NH3. Conversely, on average, the sources showing higher local
increments were RT (62 %–90 % at all sites) and V–Ni (65 %–80 % in ES and
NL). The relationship between SSA and V–Ni indicated that the contribution
of ship emissions to the local sulfate concentrations in NL has strongly
decreased since 2007 thanks to the shift from high-sulfur- to low-sulfur-content fuel used by ships. An improvement of air quality in the five cities
included here could be achieved by further reducing local (urban) emissions
of PM, NOx and NH3 (from both traffic and non-traffic sources) but
also SO2 and PM (from maritime ships and ports) and giving high
relevance to non-urban contributions by further reducing emissions of
SO2 (maritime shipping) and NH3 (agriculture) and those from
industry, regional BB sources and coal combustion.
Trajectory-based statistical models (TMs) are widely used to locate source areas responsible for atmospheric pollution at receptor sites. In order to study the influence of long, medium and ...short-range back-trajectories (BTs) on geographical sources location, an original approach was applied to daily PM10 concentrations measured for 5 years (2009–2013) at 12 receptor sites in the Hauts-de-France (HdF) region bounded on the south by the Paris megacity and on the north by the Benelux countries. The methodology used was based on two complementary TMs, Concentration Field (CF) and Potential Source Contribution Function (PSCF), and included several meaningful constraints in order to improve the spatial representativeness and the statistical significance of the potential source maps. The selection of BTs depending on the occurrence of scavenging precipitations (>1 mm h−1) during the transport of air masses and altitude limitations with respect to the planetary boundary layer height led to more realistic maps. The variability of the density of BT endpoints was accounted for by a weighting function which highlighted medium-distant yet recurring (e.g. Benelux and West of Germany) potential sources of PM10. Investigating the effect of short-range BTs (75% of endpoints within a radius of 500 km from the receptor sites) pointed out at nearby large conurbations (Lille and Paris areas). Comparing our potential source maps with European PM10 emission inventory maps as well as PM10 measurements at European background monitoring stations for similar periods confirmed our results for Central Europe, the Benelux and the East of Germany. This study showed how the combination of several receptor sites enables the determination of potential source areas impacting a whole region. It pointed out also that the fine-tuned parametrization of the CF and PSCF TMs may considerably help improving the knowledge on geographical location of sources related to long, medium and short-range BTs and could be easily implemented for other regions of interest.
•Use of constrained multisite trajectory-based CF and PSCF statistical models for PM10 source localization.•Identification of potential sources from regional to continental scales depending on model constraining.•Realization of CF and PSCF maps of PM10 potential sources impacting North of France over a 5-year period.
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