scholarly journals Source apportionment of atmospheric PM<sub>10</sub> oxidative potential: synthesis of 15 year-round urban datasets in France

2021 ◽  
Vol 21 (14) ◽  
pp. 11353-11378
Author(s):  
Samuël Weber ◽  
Gaëlle Uzu ◽  
Olivier Favez ◽  
Lucille Joanna S. Borlaza ◽  
Aude Calas ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Health Risks ◽  
Biomass Burning ◽  
Large Scale ◽  
Road Traffic ◽  
Urban Traffic ◽  
Redox Activity ◽  
Significant Activity ◽  
Oxidative Potential

Abstract. Reactive oxygen species (ROS) carried or induced by particulate matter (PM) are suspected of inducing oxidative stress in vivo, leading to adverse health impacts such as respiratory or cardiovascular diseases. The oxidative potential (OP) of PM, displaying the ability of PM to oxidize the lung environment, is gaining strong interest in examining health risks associated with PM exposure. In this study, OP was measured by two different acellular assays (dithiothreitol, DTT, and ascorbic acid, AA) on PM10 filter samples from 15 yearly time series of filters collected at 14 different locations in France between 2013 and 2018, including urban, traffic and Alpine valley site typologies. A detailed chemical speciation was also performed on the same samples, allowing the source apportionment of PM using positive matrix factorization (PMF) for each series, for a total number of more than 1700 samples. This study then provides a large-scale synthesis of the source apportionment of OP using coupled PMF and multiple linear regression (MLR) models. The primary road traffic, biomass burning, dust, MSA-rich, and primary biogenic sources had distinct positive redox activity towards the OPDTT assay, whereas biomass burning and road traffic sources only display significant activity for the OPAA assay. The daily median source contribution to the total OPDTT highlighted the dominant influence of the primary road traffic source. Both the biomass burning and the road traffic sources contributed evenly to the observed OPAA. Therefore, it appears clear that residential wood burning and road traffic are the two main target sources to be prioritized in order to decrease significantly the OP in western Europe and, if the OP is a good proxy of human health impact, to lower the health risks from PM exposure.

scholarly journals Source apportionment of atmospheric PM<sub>10</sub> Oxidative Potential: synthesis of 15 year-round urban datasets in France

2021 ◽  
Author(s):  
Samuël Weber ◽  
Gaëlle Uzu ◽  
Olivier Favez ◽  
Lucille Joanna Borlaza ◽  
Aude Calas ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Health Risks ◽  
Biomass Burning ◽  
Large Scale ◽  
Road Traffic ◽  
Urban Traffic ◽  
Redox Activity ◽  
Significant Activity ◽  
Oxidative Potential

Abstract. Reactive oxygen species (ROS) carried or induced by particulate matter (PM) are suspected to induce oxidative stress in vivo, leading to adverse health impacts, such as respiratory or cardiovascular diseases. The oxidative potential (OP) of PM, displaying the ability of PM to oxidize the lung environment, is gaining a strong interest to examine health risks associated to PM exposure. In this study, OP was measured by two different acellular assays (dithiothreitol, DTT and ascorbic acid, AA) on PM10 filter samples from 15 yearly time series of filters collected at 14 different locations in France between 2013 and 2018, including urban, traffic and Alpine valley site typologies. A detailed chemical speciation was also performed on the same samples allowing the source-apportionment of PM using positive matrix factorization (PMF) for each series, for a total number of more than 1700 samples. This study provides then a large-scale synthesis on the source-apportionment of OP using coupled PMF and multiple linear regression (MLR) models. The primary road traffic, biomass burning, dust, MSA-rich, and primary biogenic sources had distinct positive redox-activity towards the OPDTT assay, whereas biomass burning and road traffic sources only display significant activity for the OPAA assay. The daily median source contribution to the total OPDTT highlighted the dominant influence of the primary road traffic source. Both the biomass burning and the road traffic sources contributed evenly to the observed OPAA. Therefore, it appears clearly that residential wood burning and road traffic are the two main target sources to prioritized in order to decrease significantly the OP in Western Europe and, would the OP being a good proxy of human health impact, to lower the health risks from PM exposure.

scholarly journals A semi-automated system for quantifying the oxidative potential of ambient particles in aqueous extracts using the dithiothreitol (DTT) assay: results from the Southeastern Center for Air Pollution and Epidemiology (SCAPE)

2014 ◽  
Vol 7 (7) ◽  
pp. 7245-7279 ◽  
Author(s):  
T. Fang ◽  
V. Verma ◽  
H. Guo ◽  
L. E. King ◽  
E. S. Edgerton ◽  
...  
Keyword(s):  
Air Pollution ◽  
Large Scale ◽  
Limit Of Detection ◽  
Water Soluble ◽  
Automated System ◽  
Oxidative Potential ◽  
Data Set ◽  
Ambient Particles ◽  
Southeastern Us

Abstract. A variety of methods are used to measure the capability of particulate matter (PM) to catalytically generate reactive oxygen species (ROS) in vivo, also defined as the aerosol oxidative potential. A widely used measure of aerosol oxidative potential is the dithiothreitol (DTT) assay, which monitors the depletion of DTT (a surrogate for cellular antioxidants) as catalyzed by the redox-active species in PM. However, a major constraint in the routine use of the DTT assay for integrating it with the large-scale health studies is its labor-intensive and time-consuming protocol. To specifically address this concern, we have developed a semi-automated system for quantifying the oxidative potential of aerosol liquid extracts using the DTT assay. The system, capable of unattended analysis at one sample per hour, has a high analytical precision (Coefficient of Variation of 12% for standards, 4% for ambient samples), and reasonably low limit of detection (0.31 nmol min−1). Comparison of the automated approach with the manual method conducted on ambient samples yielded good agreement (slope = 1.08 ± 0.12, r2 = 0.92, N = 9). The system was utilized for the Southeastern Center for Air Pollution and Epidemiology (SCAPE) to generate an extensive data set on DTT activity of ambient particles collected from contrasting environments (urban, road-side, and rural) in the southeastern US. We find that water-soluble PM2.5 DTT activity on a per air volume basis was spatially uniform and often well correlated with PM2.5 mass (r = 0.49 to 0.88), suggesting regional sources contributing to the PM oxidative potential in southeast US. However, the greater heterogeneity in the intrinsic DTT activity (per PM mass basis) across seasons indicates variability in the DTT activity associated with aerosols from sources that vary with season. Although developed for the DTT assay, the instrument can also be used to determine oxidative potential with other acellular assays.

scholarly journals Airborne particles in the Brazilian city of São Paulo: One-year investigation for the chemical composition and source apportionment

2017 ◽  
Author(s):  
Guilherme Martins Pereira ◽  
Kimmo Teinilä ◽  
Danilo Custódio ◽  
Aldenor Gomes Santos ◽  
Huang Xian ◽  
...  
Keyword(s):  
Air Pollution ◽  
Particulate Matter ◽  
Source Apportionment ◽  
Health Risks ◽  
Biomass Burning ◽  
Sao Paulo ◽  
Airborne Particles ◽  
São Paulo ◽  
Carbonaceous Species ◽  
Local Sources

Abstract. São Paulo in Brazil has relatively relaxed regulations for ambient air pollution standards and often experiences high air pollution levels due to emissions of airborne particles from local sources and long-range transport of biomass burning-impacted air masses. In order to evaluate the sources of particulate air pollution (PM) and related health risks, a year-round sampling was performed for PM2.5 (&amp;leq; 2.5 μm) and PM10 (&amp;leq; 10 μm) in 2014 through intensive (every day sampling in wintertime) and extensive campaigns (once a week for the whole year) with 24 h of sampling. This year was characterized to have lower average precipitation comparing to meteorological data, and high pollution episodes were observed all year round, with a significant increase of pollution level in the intensive campaign, which was performed during wintertime. Different chemical constituents, such as carbonaceous species, polycyclic aromatic hydrocarbons (PAHs) and derivatives, water-soluble ions and biomass burning tracers were identified in order to evaluate health risks and to apportion sources. The species such as PAHs, inorganic and organic ions and monosaccharides were determined by chromatographic techniques and carbonaceous species by thermal-optical analysis. The associated risks to particulate matter exposure based on PAH concentrations were also assessed, along with indexes such as the benzo[a]pyrene equivalent (BaPE) and lung cancer risk (LCR). High BaPE and LCR were observed in most of the samples, rising to critical values in the wintertime. Also, biomass burning tracers and PAHs were higher in this season, while secondarily formed ions presented low variation throughout the year. Meanwhile, vehicular tracer species were also higher in the intensive campaign suggesting the influence of lower dispersion conditions in that period. Source apportionment was done by Positive Matrix Factorization (PMF), which indicated five different factors: road dust, industrial emissions, vehicular exhaust, biomass burning and secondary processes. The results highlighted the contribution of vehicular emissions and the significant input from biomass combustion in wintertime, suggesting that most of the particulate matter is due to local sources, besides the influence of pre-harvest sugarcane burning.

scholarly journals An apportionment method for the Oxydative Potential to the atmospheric PM sources: application to a one-year study in Chamonix, France

2018 ◽  
Author(s):  
Samuël Weber ◽  
Uzu Gaëlle ◽  
Aude Calas ◽  
Florie Chevrier ◽  
Jean-Luc Besombes ◽  
...  
Keyword(s):  
Health Impact ◽  
Redox Activity ◽  
Coupled Analysis ◽  
Oxidative Potential ◽  
Lung Fluid ◽  
One Year ◽  
The Impact ◽  
Linear Regressions ◽  
Detailed Chemical

Abstract. The particulate matter (PM) induces cellular oxidative stress in vivo and so lead to adverse health outcome. The oxidative potential (OP) of the PM appears to be a more relevant proxy of the health impact of the aerosol rather than the total mass concentration. However, the relative contributions of the emission’s sources of aerosols to the OP are still poorly known. In order to better quantify the impact of each PM source to the air quality, we sampled aerosols in a French city for one year (year 2014, 115 samples). A coupled analysis with detailed chemical speciation (more than 100 species, including organic and carbonaceous compounds, ions, metals and aethalomether measurements) and two OP assays (ascorbic acid (AA) and dithiothreitiol (DTT)) in a simulated lung fluid (SLF) were performed in these samples. We developed in this study a new statistical model using a coupled approach with Positive Matrix Factorisation (PMF) and multiple linear regressions to attribute a redox-activity per PM sources. Our results highlight the importance of the Biomass burning and Vehicular sources to explain the observed OP for both assays. In general, we see a different contribution of the sources when considering the OP AA, OP DTT or the mass of the PM10. Moreover, some significant differences are observed between the DTT and AA tests that emphasized the chemical specificities of the two tests and the need of a standardized approach for the future studies on epidemiology or toxicology of the PM.

scholarly journals Nitrogen isotope fractionation during gas-particle conversion of NO<sub>x</sub> to NO<sub>3</sub><sup>−</sup> in the atmosphere – implications for isotope-based NO<sub>x</sub> source apportionment

2018 ◽  
Author(s):  
Yunhua Chang ◽  
Yanlin Zhang ◽  
Chongguo Tian ◽  
Shichun Zhang ◽  
Xiaoyan Ma ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Isotope Effect ◽  
Biomass Burning ◽  
Coal Combustion ◽  
Isotope Fractionation ◽  
Road Traffic ◽  
Eastern China ◽  
Rural Site ◽  
Urban Site ◽  
Exchange Reactions

Abstract. Atmospheric fine-particle (PM2.5) pollution is frequently associated with the formation of particulate nitrate (pNO3−), the end product of the oxidation of NOx gases (= NO + NO2) in the upper troposphere. The application of stable nitrogen (N) (and oxygen) isotope analyses of pNO3− to constrain NOx source partitioning in the atmosphere requires the knowledge of the isotope fractionation during the reactions leading to NO3− formation. Here we determined the δ15N values of fresh pNO3− (δ15N-pNO3−) in PM2.5 at a rural site in Northern China, where atmospheric pNO3− can be attributed exclusively to biomass burning. The observed δ15N-pNO3− (12.17 ± 1.55 ‰; n = 8) was much higher than the N isotopic source signature of NOx from biomass burning (1.04 ± 4.13 ‰). The large difference between δ15N-pNO3− and δ15N-NOx (Δ(δ15N)) can be reconciled by the net N isotope effect (ԑN) associated with the gas-particle conversion from NOx to NO3−. For the biomass-burning site, a mean ԑN (≈ Δ(δ15N)) of 10.99 ± 0.74 ‰ was assessed through a newly-developed computational quantum chemistry (CQC) module. ԑN depends on the relative importance of the two dominant N isotope exchange reactions involved (NO2 reaction with OH versus hydrolysis of dinitrogen pentoxide (N2O5) with H2O), and varies between regions, and on a diurnal basis. A second, slightly higher CQC-based mean value for ԑN (15.33 ± 4.90 ‰) was estimated for an urban site with intense traffic in Eastern China, and integrated in a Bayesian isotope mixing model to make isotope-based source apportionment estimates for NOx at this site. Based on the δ15N values (10.93 ± 3.32 ‰, n = 43) of ambient pNO3− determined for the urban site, and considering the location-specific estimate for ԑN, our results reveal that the relative contribution of coal combustion and road traffic to urban NOx are 32 ± 11 % and 68 ± 11 %, respectively. This finding agrees well with a regional bottom-up emission inventory of NOx. Moreover, the variation pattern of OH contribution to ambient pNO3− formation calculated by the CQC module is consistent with that simulated by the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), further confirming the robustness of our estimates. Our investigations also show that, without the consideration of the N isotope effect during pNO3− formation, the observed δ15N-pNO3− at the study site would erroneously imply that NOx is derived almost entirely from coal combustion. Similarly, reanalysis of reported δ15N-NO3− data throughout China suggests that, nationwide, NOx emissions from coal combustion may be substantively overestimated (by > 30 %) when the N isotope fractionation during atmospheric pNO3− formation is neglected.

scholarly journals A semi-automated system for quantifying the oxidative potential of ambient particles in aqueous extracts using the dithiothreitol (DTT) assay: results from the Southeastern Center for Air Pollution and Epidemiology (SCAPE)

2015 ◽  
Vol 8 (1) ◽  
pp. 471-482 ◽  
Author(s):  
T. Fang ◽  
V. Verma ◽  
H. Guo ◽  
L. E. King ◽  
E. S. Edgerton ◽  
...  
Keyword(s):  
Air Pollution ◽  
Large Scale ◽  
Limit Of Detection ◽  
Water Soluble ◽  
Automated System ◽  
Oxidative Potential ◽  
Data Set ◽  
Ambient Particles ◽  
Southeastern Us

Abstract. A variety of methods are used to measure the capability of particulate matter (PM) to catalytically generate reactive oxygen species (ROS) in vivo, also defined as the aerosol oxidative potential. A widely used measure of aerosol oxidative potential is the dithiothreitol (DTT) assay, which monitors the depletion of DTT (a surrogate for cellular antioxidants) as catalyzed by the redox-active species in PM. However, a major constraint in the routine use of the DTT assay for integrating it with large-scale health studies is its labor-intensive and time-consuming protocol. To specifically address this concern, we have developed a semi-automated system for quantifying the oxidative potential of aerosol liquid extracts using the DTT assay. The system, capable of unattended analysis at one sample per hour, has a high analytical precision (coefficient of variation of 15% for positive control, 4% for ambient samples) and reasonably low limit of detection (0.31 nmol min−1). Comparison of the automated approach with the manual method conducted on ambient samples yielded good agreement (slope = 1.08 ± 0.12, r2 = 0.92, N = 9). The system was utilized for the Southeastern Center for Air Pollution &amp; Epidemiology (SCAPE) to generate an extensive data set on DTT activity of ambient particles collected from contrasting environments (urban, roadside, and rural) in the southeastern US. We find that water-soluble PM2.5 DTT activity on a per-air-volume basis was spatially uniform and often well correlated with PM2.5 mass (r = 0.49 to 0.88), suggesting regional sources contributing to the PM oxidative potential in the southeastern US. The correlation may also suggest a mechanistic explanation (oxidative stress) for observed PM2.5 mass-health associations. The heterogeneity in the intrinsic DTT activity (per-PM-mass basis) across seasons indicates variability in the DTT activity associated with aerosols from sources that vary with season. Although developed for the DTT assay, the instrument can also be used to determine oxidative potential with other acellular assays.

scholarly journals Source Apportionment of PM2.5 and of its Oxidative Potential in an Industrial Suburban Site in South Italy

Atmosphere ◽  
2019 ◽  
Vol 10 (12) ◽  
pp. 758 ◽  
Author(s):  
Daniela Cesari ◽  
Eva Merico ◽  
Fabio Massimo Grasso ◽  
Stefano Decesari ◽  
Franco Belosi ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Environmental Protection Agency ◽  
Biogas Production ◽  
Atmospheric Particulate Matter ◽  
Industrial Emissions ◽  
Oxidative Potential ◽  
Vehicle Traffic ◽  
Receptor Models ◽  
Source Contributions

Some studies suggested a role of the atmospheric particulate matter (PM) and of its oxidative potential (OP) in determining adverse health effects. Several works have focused on characterisation of source contributions to PM OP, mainly using three approaches: correlation between OP and chemical markers of specific sources; use of OP as input variable in source apportionment with receptor models; and multi-linear regression (MLR) between OP and source contributions to PM obtained from receptor models. Up to now, comparison of results obtained with different approaches on the same dataset is scarce. This work aims to perform a OP study of PM2.5 collected in an industrial site, located near a biogas production and combustion plant (in southern Italy), comparing different approaches to investigate the contributions of the different sources to OP. The PM2.5 samples were analysed for determining ions, metals, carbonaceous components, and OP activity with the DTT (dithiotreitol) assay. Results showed that OP normalised in volume (DTTV) is correlated with carbonaceous components and some ions (NO3−, and Ca2+) indicating that PM of combustion, secondary, and crustal origin could contribute to the OP activity. The source apportionment, done with the Environmental Protection Agency (EPA)—Positive Matrix Factorization (PMF5.0) model, identified six sources: secondary sulphate; biomass burning; industrial emissions; crustal; vehicle traffic and secondary nitrate; and sea spray. A MLR analysis between the source’s daily contributions and the daily DTTV values showed a reasonable agreement of the two approaches (PMF and MLR), identifying the biomass burning and the vehicle traffic and secondary nitrate as the main sources contributing to DTTV activity.

scholarly journals Source apportionment of carbonaceous chemical species to fossil fuel combustion, biomass burning and biogenic emissions by a coupled radiocarbon–levoglucosan marker method

2017 ◽  
Vol 17 (22) ◽  
pp. 13767-13781 ◽  
Author(s):  
Imre Salma ◽  
Zoltán Németh ◽  
Tamás Weidinger ◽  
Willy Maenhaut ◽  
Magda Claeys ◽  
...  
Keyword(s):  
Source Apportionment ◽  
Biomass Burning ◽  
Fossil Fuel ◽  
Road Traffic ◽  
Size Fraction ◽  
Chemical Species ◽  
Control Measures ◽  
Total Carbon ◽  
Relative Uncertainty ◽  
Atmospheric Concentrations

Abstract. An intensive aerosol measurement and sample collection campaign was conducted in central Budapest in a mild winter for 2 weeks. The online instruments included an FDMS-TEOM, RT-OC/EC analyser, DMPS, gas pollutant analysers and meteorological sensors. The aerosol samples were collected on quartz fibre filters by a low-volume sampler using the tandem filter method. Elemental carbon (EC), organic carbon (OC), levoglucosan, mannosan, galactosan, arabitol and mannitol were determined, and radiocarbon analysis was performed on the aerosol samples. Median atmospheric concentrations of EC, OC and PM2.5 mass were 0.97, 4.9 and 25 µg m−3, respectively. The EC and organic matter (1.6  ×  OC) accounted for 4.8 and 37 %, respectively, of the PM2.5 mass. Fossil fuel (FF) combustion represented 36 % of the total carbon (TC  =  EC + OC) in the PM2.5 size fraction. Biomass burning (BB) was a major source (40 %) for the OC in the PM2.5 size fraction, and a substantial source (11 %) for the PM10 mass. We propose and apply here a novel, straightforward, coupled radiocarbon–levoglucosan marker method for source apportionment of the major carbonaceous chemical species. The contributions of EC and OC from FF combustion (ECFF and OCFF) to the TC were 11.0 and 25 %, respectively, EC and OC from BB (ECBB and OCBB) were responsible for 5.8 and 34 %, respectively, of the TC, while the OC from biogenic sources (OCBIO) made up 24 % of the TC. The overall relative uncertainty of the OCBIO and OCBB contributions was assessed to be up to 30 %, while the relative uncertainty for the other apportioned species is expected to be below 20 %. Evaluation of the apportioned atmospheric concentrations revealed some of their important properties and relationships among them. ECFF and OCFF were associated with different FF combustion sources. Most ECFF was emitted by vehicular road traffic, while the contribution of non-vehicular sources such as domestic and industrial heating or cooking using gas, oil or coal to OCFF was substantial. The mean contribution of BB to EC particles was smaller by a factor of approximately 2 than that of road traffic. The main formation processes of OCFF, OCBB and OCBIO from volatile organic compounds were jointly influenced by a common factor, which is most likely the atmospheric photochemistry, while primary organic emissions can also be important. Technological improvements and control measures for various BB appliances, together with efficient education and training of their users, in particular on the admissible fuel types, offer an important potential for improving the air quality in Budapest, and likely in other cities as well.

scholarly journals An apportionment method for the oxidative potential of atmospheric particulate matter sources: application to a one-year study in Chamonix, France

2018 ◽  
Vol 18 (13) ◽  
pp. 9617-9629 ◽  
Author(s):  
Samuël Weber ◽  
Gaëlle Uzu ◽  
Aude Calas ◽  
Florie Chevrier ◽  
Jean-Luc Besombes ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Health Impact ◽  
Atmospheric Particulate Matter ◽  
Redox Activity ◽  
Coupled Analysis ◽  
Oxidative Potential ◽  
Adverse Health Outcomes ◽  
One Year ◽  
The Impact

Abstract. Inhaled aerosolized particulate matter (PM) induces cellular oxidative stress in vivo, leading to adverse health outcomes. The oxidative potential (OP) of PM appears to be a more relevant proxy of the health impact of the aerosol rather than the total mass concentration. However, the relative contributions of the aerosol sources to the OP are still poorly known. In order to better quantify the impact of different PM sources, we sampled aerosols in a French city for one year (2014, 115 samples). A coupled analysis with detailed chemical speciation (more than 100 species, including organic and carbonaceous compounds, ions, metals and aethalometer measurements) and two OP assays (ascorbic acid, AA, and dithiothreitiol, DTT) in a simulated lung fluid (SLF) were performed in these samples. We present in this study a statistical framework using a coupled approach with positive matrix factorization (PMF) and multiple linear regression to attribute a redox-activity to PM sources. Our results highlight the importance of the biomass burning and vehicular sources to explain the observed OP for both assays. In general, we see a different contribution of the sources when considering the OP AA, OP DTT or the mass of the PM10. Moreover, significant differences are observed between the DTT and AA tests which emphasized chemical specificities of the two tests and the need of a standardized approach for the future studies on epidemiology or toxicology of the PM.

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