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Sample records for aerosol source apportionment

  1. Source apportionment of carbonaceous aerosol in southern Sweden

    NASA Astrophysics Data System (ADS)

    Genberg, J.; Hyder, M.; Stenström, K.; Bergström, R.; Simpson, D.; Fors, E.; Jönsson, J. Å.; Swietlicki, E.

    2011-05-01

    A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (14C) and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (82 %), which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (38 %) and fossil fuel combustion (33 %) were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 8.2 compared to the measurements.

  2. Source apportionment of carbonaceous aerosol in southern Sweden

    NASA Astrophysics Data System (ADS)

    Genberg, J.; Hyder, M.; Stenström, K.; Bergström, R.; Simpson, D.; Fors, E. O.; Jönsson, J. Å.; Swietlicki, E.

    2011-11-01

    A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (14C) and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (80%), which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (32%) and fossil fuel combustion (28%) were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP MSC-W chemical transport model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 2.2 compared to the measurements.

  3. Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

    EPA Science Inventory

    ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

  4. Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

    EPA Science Inventory

    ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

  5. Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Daellenbach, K. R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J. G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; Prévôt, A. S. H.; El Haddad, I.

    2015-08-01

    Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make impractical its deployment at sufficient sites to determine regional characteristics. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, PM10) collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g. AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91 %) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon, oxygen containing and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g. filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially-resolved long-term datasets.

  6. Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Daellenbach, K. R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J. G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; El Haddad, I.; Prévôt, A. S. H.

    2016-01-01

    Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 µm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91 %) achieved using this technique, together with low detection limits (0.8 µg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.

  7. Carbon isotope based aerosol source apportionment in Eastern European city Vilnius

    NASA Astrophysics Data System (ADS)

    Garbaras, Andrius; Sapolaite, Justina; Garbariene, Inga; Ezerinskis, Zilvinas; Pocevicius, Matas; Krikscikas, Laurynas; Jacevicius, Sarunas; Plukis, Arturas; Remeikis, Vidmantas

    2016-04-01

    We present carbonaceous aerosol source apportionment results in Eastern European city Vilnius (capital of Lithuania) using stable carbon isotope ratio (δ13C) and radiocarbon (14C) methods. The aerosol sampling campaigns were performed in 2014-2016 winter seasons in Vilnius. PM1 particles were collected on quartz fiber filters using high volume sampler, while PM10 and size segregated aerosol particles were collected using low volume and MOUDI 128 cascade impactor respectively. δ13C values were measured with EA-IRMS system while radiocarbon analysis was performed using Single Stage Accelerator Mass Spectrometer (SSAMS). For the AMS analysis, filters (or aluminium foils from cascade impactor) were graphitized using Automated Graphitization Equipment. It was estimated that dominant carbonaceous aerosol source in Vilnius was of biogenic/biomass origin (60-90 %). Fossil fuel sources accounted for up to 23 % of total carbon fraction. Combining stable carbon and radiocarbon isotope analysis we were able to quantify the amount of coal derived aerosol particles. The contribution of coal burning emissions were up to 14 %. We will present the applicability of dual carbon (13C and 14C) isotope ratio method for the aerosol source apportionment in different regions of Europe, also the perspectives of using MOUDI cascade impactors to make source apportionment in size segregated aerosol particles.

  8. PIXE and receptor models applied to remote aerosol source apportionment in Brazil

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Orsini, Celso

    1987-03-01

    We have used PIXE together with receptor modeling for quantiative source apportionment of remote aerosols. The Sao Paulo PIXE system uses an 8 MeV alpha particle beam, and it can detect elements with Z > 11 with a detection limit between 1 and 30 ng m 3 . We sampled atmospheric aerosols in six remote sites: Amazon Basin. Atlantic Forest, Arembepe, Fernando de Noronha, Firminopolis and Itaherai. Sampling was performed using stacked filter units, cascade impactors with 6 or 10 stages and linear streakers. Source apportionment of the coarse mode aerosols was done using three receptor models: chemical mass balance, principal factor analysis and stepwise multiple regression analysis. Three sources of aerosols were quantiatively distinguished: marine aerosols, soil dust and aerosols released by plants. The emission of aerosols by vegetation is very clear for all sampling sites and with all three receptor models. In the Amazon Basin and Atlantic Forest the aerosol released by plants is the major source and accounts for 60-80% of airborne concentrations.

  9. Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Nøjgaard, J. K.; Kristensen, K.; Genberg, J.; Stenström, K.; Swietlicki, E.; Hillamo, R.; Aurela, M.; Bauer, H.; Offenberg, J. H.; Jaoui, M.; Dye, C.; Eckhardt, S.; Burkhart, J. F.; Stohl, A.; Glasius, M.

    2011-06-01

    In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 collected at four Nordic rural background sites (Birkenes (Norway), Hyytiälä (Finland) Vavihill (Sweden), Lille Valby (Denmark)) during late summer (5 August-2 September 2009). Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the 14C/12C ratio of total carbon (TC), have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TCp; i.e. particulate TC) was totally dominated by natural sources (69-86 %), with biogenic secondary organic aerosol (BSOA) being the single most important source (48-57 %). Interestingly, primary biological aerosol particles (PBAP) were the second most important source (20-32 %). The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff (10-24 %), whereas no more than 3-7 % was explained by combustion of biomass (OCbb and ECbb in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, accounting for 4-12 % of TCp, whereas <1.5 % was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources. Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural background environment are reported for the first time in the present study. The most abundant organosulphate compounds were an organosulphate of isoprene and nitrooxy

  10. Secondary organic aerosol formation and source apportionment in Southeast Texas

    NASA Astrophysics Data System (ADS)

    Zhang, Hongliang; Ying, Qi

    2011-06-01

    The latest version of US EPA's Community Multi-scale Air Quality (CMAQ v4.7) model with the most recent update on secondary organic aerosol (SOA) formation pathways was adapted into a source-oriented modeling framework to determine the contributions of different emission sources to SOA concentrations from a carbon source perspective in Southeast Texas during the 2000 Texas Air Quality Study (TexAQS 2000) from August 25 to September 5, 2000. A comparison of the VOC and SOA predictions with observations shows that anthropogenic emissions of long chain alkanes and aromatics are likely underestimated in the EPA's Clean Air Interstate Rule (CAIR) inventory and the current SOA mechanism in CMAQ still under-predicts SOA. The peak SOA concentrations measured at La Porte are more accurately predicted by increasing the emissions of the anthropogenic SOA precursors by a factor of 5 although the overall precursor concentrations are better predicted by increasing the emissions by a factor of 2. A linear correlation between SOA and odd oxygen (ΔSOA/ΔOx = 23.0-28.4 μg m-3/ppm Ox) can be found when they are formed simultaneously in the air masses passing the urban Houston area on high SOA days. Based on the adjusted emissions (a factor of 2 increase in the alkane and aromatics precursor emissions), approximately 20% of the total SOA in the Houston-Galveston Bay area is due to anthropogenic sources. Solvent utilization and gasoline engines are the main anthropogenic sources. SOA from alkanes and aromatics accounts for approximately 2-4% and 5-9% of total SOA, respectively. The predicted overall anthropogenic SOA concentrations are not sensitive to the half-life time used to calculate the conversion rate of semi-volatile organic compounds to non-volatile oligomers in the particle phase. The main precursors of biogenic SOA are sesquiterpenes, which contribute to approximately 12-35% of total SOA. Monoterpenes contribute to 3-14% and isoprene accounts for approximately 6-9% of the

  11. Quantification and radiocarbon source apportionment of black carbon in atmospheric aerosols using the CTO-375 method

    NASA Astrophysics Data System (ADS)

    Zencak, Zdenek; Elmquist, Marie; Gustafsson, Örjan

    To make progress towards linking the atmosphere and biogeosphere parts of the black carbon (BC) cycle, a chemothermal oxidation method (CTO-375), commonly applied for isolating BC from complex geomatrices such as soils, sediments and aquatic particles, was applied to investigate the BC also in atmospheric particles. Concentrations and 14C-based source apportionment of CTO-375 based BC was established for a reference aerosol (NIST RM-8785) and for wintertime aerosols collected in Stockholm and in a Swedish background area. The results were compared with thermal-optical (OC/EC) measurements. For NIST RM-8785, a good agreement was found between the BC CTO-375 concentration and the reported elemental carbon (EC) concentration measured by the "Speciation Trends Network—National Institute of Occupational Safety and Health" method (EC NIOSH) with BC CTO-375 of 0.054±0.002 g g -1 and EC NIOSH of 0.067±0.008 g g -1. In contrast, there was an average factor of ca. 20 difference between BC CTO-375 and EC NIOSH for the ambient Scandinavian wintertime aerosols, presumably reflecting a combination of BC CTO-375 isolating only the recalcitrant soot-BC portion of the BC continuum and the EC NIOSH metric inadvertently including some intrinsically non-pyrogenic organic matter. Isolation of BC CTO-375 with subsequent off-line radiocarbon analysis yielded fraction modern values (fM) for total organic carbon (TOC) of 0.93 (aerosols from a Swedish background area), and 0.58 (aerosols collected in Stockholm); whereas the fM for BC CTO-375 isolates were 1.08 (aerosols from a Swedish background area), and 0.87 (aerosols collected in Stockholm). This radiocarbon-based source apportionment suggests that contribution from biomass combustion to cold-season atmospheric BC CTO-375 in Stockholm was 70% and in the background area 88%.

  12. Relevance of aerosol size spectrum analysis as support to qualitative source apportionment studies.

    PubMed

    Manigrasso, M; Febo, A; Guglielmi, F; Ciambottini, V; Avino, P

    2012-11-01

    This work presents a diagnostic methodology in support to source apportionment studies to identify remote and local pollution sources. It is based on the temporal analysis of both PM size distributions and PM size fraction correlation along with natural radioactivity measurements as index of Planetary Boundary Layer dynamic. A correlation drop is indicative of changing aerosol sources. When this observation is coupled with decreasing level of natural radioactivity and increasing aerosol concentration, be it coarse or fine, it is indicative of the inflow of remote polluted air masses. The methodology defines in which size range operates the contribution of remote pollution sources. It was applied to two PM10 pollution episodes: the first involved the advection of coarse PM, the second entailed the inflow of two air masses, one transporting coarse dust and the other fine PM. Dust models and backward trajectories analysis confirmed such results, indicating the air mass provenience.

  13. Advances in the Use of Molecular Markers for Source Apportionment of Atmospheric Organic Aerosols

    NASA Astrophysics Data System (ADS)

    Schauer, J. J.; Sheesley, R. J.; Jaeckels, J. M.

    2006-12-01

    Over the past decade, there has been significant effort directed at measuring particle-phase organic compounds in air pollution emission sources and in the atmosphere. A subset of these organic compounds are relatively unique to the emissions from specific air pollution source categories and are believed to be stable enough in the atmosphere to be used as source tracers. To date, studies have been conducted in North America, Asia and Europe in both remote and urbanized locations that have used these organic compound tracers, also called molecular markers, for source attribution studies. The major short-comings of these studies are the uncertainties associated with developing site and season specific molecular marker source profiles and the absence of source fingerprints for secondary organic aerosol. Recent advances in molecular marker chemical analysis methods has lead to two key advances for molecular marker source apportionment efforts: 1) sufficiently large data sets of molecular marker measures have been generated that now allow multivariate receptor models to be used in parallel with chemical mass balance (CMB) models, and 2) compounds that are believed to be predominately associated with secondary organic aerosol (SOA) have been identified and can be routinely analyzed in organic aerosol samples. Given these advances, data sets have been generated that can be used to apportion atmospheric organic aerosols to both primary and secondary organic aerosols without the use of source profiles. Background on molecular markers will be presented along with recent organic aerosol source apportionment results that were obtained using multivariate receptor models to analyze molecular marker data sets obtained in the Midwestern United States. These data sets include a daily time series of molecular marker concentration data from the Midwest Supersite in East St. Louis that spans two years and a monthly average tracer data for a year that were simultaneously obtained in St

  14. Volatility-resolved source apportionment of primary and secondary organic aerosol over Europe

    NASA Astrophysics Data System (ADS)

    Skyllakou, Ksakousti; Fountoukis, Christos; Charalampidis, Panagiotis; Pandis, Spyros N.

    2017-10-01

    A three-dimensional regional chemical transport model (Particulate Matter Comprehensive Air Quality Model with Extensions, PMCAMx) was applied over Europe combined with a source apportionment algorithm, the Particulate Source Apportionment Technology (PSAT), in order to quantify the sources which contribute to the primary and secondary organic aerosol (OA) during different seasons. The PSAT algorithm was first extended to allow the quantification of the sources of OA as a function of volatility. The most significant OA sources during May were biogenic, while during February residential wood combustion and during September wildfires dominated. The contributions of the various sources have strong spatial dependence. Wildfires were significant OA sources (38% of the OA) for Russia during September, but had a much lower impact (5%) in Scandinavia. The above results are in general consistent with the findings of the CARBOSOL project for selected sites in Europe. For remote sites such as Finokalia in Crete, more than 90% of the OA has undergone two or more generations of oxidation for all seasons. This highly processed oxidized OA is predicted to also dominate over much of Europe during the summer and fall. The first generation SOA is predicted to represent 20-30% of the OA in central and northern Europe during these photochemically active periods.

  15. Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Nøjgaard, J. K.; Kristensen, K.; Genberg, J.; Stenström, K.; Swietlicki, E.; Hillamo, R.; Aurela, M.; Bauer, H.; Offenberg, J. H.; Jaoui, M.; Dye, C.; Eckhardt, S.; Burkhart, J. F.; Stohl, A.; Glasius, M.

    2011-12-01

    In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter <10 μm) collected at four Nordic rural background sites [Birkenes (Norway), Hyytiälä (Finland), Vavihill (Sweden), Lille Valby, (Denmark)] during late summer (5 August-2 September 2009). Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the 14C/12C ratio of total carbon (TC), have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TCp; i.e. particulate TC) was totally dominated by natural sources (69-86%), with biogenic secondary organic aerosol (BSOA) being the single most important source (48-57%). Interestingly, primary biological aerosol particles (PBAP) were the second most important source (20-32%). The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff) (10-24%), whereas no more than 3-7% was explained by combustion of biomass (OCbb and ECbb) in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, which accounted for 4-12% of TCp, whereas <1.5% of EC was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources. Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural background environment are reported for the first time in the present study. The most abundant organosulphate compounds were an

  16. Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

    NASA Astrophysics Data System (ADS)

    Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

    2016-04-01

    The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle

  17. Aerosol source apportionment from 1-year measurements at the CESAR tower in Cabauw, the Netherlands

    NASA Astrophysics Data System (ADS)

    Schlag, Patrick; Kiendler-Scharr, Astrid; Blom, Marcus Johannes; Canonaco, Francesco; Sebastiaan Henzing, Jeroen; Moerman, Marcel; Prévôt, André Stephan Henry; Holzinger, Rupert

    2016-07-01

    Intensive measurements of submicron aerosol particles and their chemical composition were performed with an Aerosol Chemical Speciation Monitor (ACSM) at the Cabauw Experimental Site for Atmospheric Research (CESAR) in Cabauw, the Netherlands, sampling at 5 m height above ground. The campaign lasted nearly 1 year from July 2012 to June 2013 as part of the EU-FP7-ACTRIS project (Q-ACSM Network). Including equivalent black carbon an average particulate mass concentration of 9.50 µg m-3 was obtained during the whole campaign with dominant contributions from ammonium nitrate (45 %), organic aerosol (OA, 29 %), and ammonium sulfate (19 %). There were 12 exceedances of the World Health Organization (WHO) PM2.5 daily mean limit (25 µg m-3) observed at this rural site using PM1 instrumentation only. Ammonium nitrate and OA represented the largest contributors to total particulate matter during periods of exceedance. Source apportionment of OA was performed season-wise by positive matrix factorization (PMF) using the multilinear engine 2 (ME-2) controlled via the source finder (SoFi). Primary organic aerosols were attributed mainly to traffic (8-16 % contribution to total OA, averaged season-wise) and biomass burning (0-23 %). Secondary organic aerosols (SOAs, 61-84 %) dominated the organic fraction during the whole campaign, particularly on days with high mass loadings. A SOA factor which is attributed to humic-like substances (HULIS) was identified as a highly oxidized background aerosol in Cabauw. This shows the importance of atmospheric aging processes for aerosol concentration at this rural site. Due to the large secondary fraction, the reduction of particulate mass at this rural site is challenging on a local scale.

  18. Aerosol source apportionment from 1 year measurements at the CESAR tower at Cabauw, NL

    NASA Astrophysics Data System (ADS)

    Schlag, P.; Kiendler-Scharr, A.; Blom, M. J.; Canonaco, F.; Henzing, J. S.; Moerman, M. M.; Prévôt, A. S. H.; Holzinger, R.

    2015-12-01

    Intensive measurements of submicron aerosol particles and their chemical composition were performed with an Aerosol Chemical Speciation Monitor (ACSM) at the Cabauw Experimental Site for Atmospheric Research (CESAR) in Cabauw, NL. The campaign lasted nearly one year from July 2012 to June 2013 as part of the ACTRIS project. Including black carbon data an average particulate mass concentration of 9.50 μg m-3 was obtained during the whole campaign with dominant contributions from ammonium nitrate (45 %), organic aerosol (OA, 29 %), and ammonium sulfate (19 %). 12 exceedances of the World Health Organization (WHO) PM2.5 daily mean limit (25 μg m-3) were observed at this rural site using PM1 instrumentation only. Ammonium nitrate and OA represented the largest contributors to total particulate matter during periods of exceedance. Source apportionment of OA was performed season-wise by Positive Matrix Factorization (PMF) using the Multilinear Engine 2 (ME-2) controlled via the source finder (SoFi). Primary organic aerosols were attributed mainly to traffic (8-16 % contribution to total OA, averaged season-wise) and biomass burning (0-23 %). Secondary organic aerosols (SOA, 61-84 %) dominated the organic fraction during the whole campaign, particularly on days with high mass loadings. A SOA factor which is attributed to humic-like substances (HULIS) was identified as a highly oxidized background aerosol in Cabauw. This shows the importance of atmospheric ageing processes for aerosol concentration at this rural site. Due to the large secondary fraction, the reduction of particulate mass at this rural site is challenging on a local scale.

  19. Source apportionment of carbonaceous aerosols over South and East Asia using dual carbon isotopes

    NASA Astrophysics Data System (ADS)

    Gustafsson, O.; Kirillova, E. N.; Andersson, A.-; Kruså, M.; Sheesley, R. J.; Tiwari, S.-; Lee, M.; Chen, B.; Du, K.

    2012-12-01

    Emissions of black carbon (BC) and other components of carbonaceous aerosols affect both climate and health in South and East Asia, yet substantial uncertainties exist regarding their sources. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain both to direct mitigation and as their different properties make their effects on climate forcing and respiratory health different. This study approached the sourcing challenge by applying microscale radiocarbon measurements to aerosol particles collected in both source regions and at regional receptor observatories of both S Asia (New Delhi and the Maldives Climate Observatory) and of E Asia (Beijing, Shanghai, South China Coastal Observatory and the Korea Climate Observatory - Gosan, KCO-G, Jeju Island). The radiocarbon approach is ideally suited to this task as fossil sources are void of 14C whereas biomass combustion products hold a contemporary 14C signal. For S Asia, the 14C-based observations suggest that biomass combustion contributes half to two-thirds of the BC loading. In contrast, for E Asia, fossil fuel combustion account for four-fifths of the BC emitted from China. This source-diagnostic radiocarbon signal in the ambient aerosol over East Asia establishes a much larger role for fossil fuel combustion than suggested by all fifteen BC emission inventory models. There are also poor constraints on the sources of water-soluble organic carbon (WSOC), a large hydrophilic component of carbonaceous aerosols that enhances the propensity of aerosols to form clouds. In a 15-mo continuous campaign in S Asia, radiocarbon-based source apportionment of WSOC shows the dominance of biogenic/biomass combustion sources but also a substantial anthropogenic fossil-fuel contribution (about 20%). WSOC in E Asia reaching KCO-G were 50% from fossil sources. Aerosols reaching the Maldives after long-range over-ocean transport were enriched by 3-4‰ in δ13C-WSOC. This is

  20. Radiocarbon source apportionment of urban and wildfire black and organic carbon aerosols

    NASA Astrophysics Data System (ADS)

    Mouteva, G.; Fahrni, S. M.; Santos, G.; Randerson, J. T.; Czimczik, C. I.

    2013-12-01

    Fossil and non-fossil sources of black carbon (BC) and organic carbon (OC) in carbonaceous aerosols can be quantified unambiguously by radiocarbon (14C) measurements. However, accurate 14C-based source apportionment requires a clear and reproducible physical separation of OC and BC, as well as minimal sample contaminations with non-sample carbon. To achieve a clear separation, we used a thermo-optical aerosol analyzer (Sunset Laboratory Inc, USA) with a newly established protocol (Swiss_4S protocol, Zhang et al., 2012), specifically optimized to completely separate the OC and BC fractions with minimal charring and maximum BC recovery. A simple and efficient vacuum line was coupled to the analyzer to trap produced CO2 with high yields and low carbon blanks. Upon trapping, CO2 samples sealed into glass ampoules were converted to graphite and measured for their radiocarbon content at the Keck Carbon Cycle Accelerator Mass Spectrometry Laboratory at the University of California, Irvine. Here, we present the results from the radiocarbon analysis of a set of 14C reference materials, blanks and inter-comparison samples for both OC and BC with sample sizes as small as 5 μg C. We will also present initial results from a set of urban aerosol samples from Salt Lake City, collected throughout 2012 and 2013, and from interior Alaska, collected during the summer of 2013 near the Stuart Creek 2 wildfire.

  1. Organic aerosol source apportionment by offline-AMS over a full year in Marseille

    NASA Astrophysics Data System (ADS)

    Bozzetti, Carlo; El Haddad, Imad; Salameh, Dalia; Daellenbach, Kaspar Rudolf; Fermo, Paola; Gonzalez, Raquel; Cruz Minguillón, María; Iinuma, Yoshiteru; Poulain, Laurent; Elser, Miriam; Müller, Emanuel; Gates Slowik, Jay; Jaffrezo, Jean-Luc; Baltensperger, Urs; Marchand, Nicolas; Prévôt, André Stephan Henry

    2017-07-01

    We investigated the seasonal trends of OA sources affecting the air quality of Marseille (France), which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). In total 216 PM2. 5 (particulate matter with an aerodynamic diameter < 2.5 µm) filter samples were collected over 1 year from August 2011 to July 2012. These filters were used to create 54 composite samples which were analyzed by offline-AMS. The same samples were also analyzed for major water-soluble ions, metals, elemental and organic carbon (EC / OC), and organic markers, including n-alkanes, hopanes, polycyclic aromatic hydrocarbons (PAHs), lignin and cellulose pyrolysis products, and nitrocatechols. The application of positive matrix factorization (PMF) to the water-soluble AMS spectra enabled the extraction of five factors, related to hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), oxygenated OA (OOA), and an industry-related OA (INDOA). Seasonal trends and relative contributions of OA sources were compared with the source apportionment of OA spectra collected from the AMS field deployment at the same station but in different years and for shorter monitoring periods (February 2011 and July 2008). Online- and offline-AMS source apportionment revealed comparable seasonal contribution of the different OA sources. Results revealed that BBOA was the dominant source during winter, representing on average 48 % of the OA, while during summer the main OA component was OOA (63 % of OA mass on average). HOA related to traffic emissions contributed on a yearly average 17 % to the OA mass, while COA was a minor source contributing 4 %. The contribution of INDOA was enhanced during winter (17 % during winter and 11 % during summer), consistent with an increased contribution from light alkanes, light PAHs (fluoranthene, pyrene, phenanthrene), and selenium, which is commonly considered as

  2. Biomass burning in the Amazon region: Aerosol source apportionment and associated health risk assessment

    NASA Astrophysics Data System (ADS)

    de Oliveira Alves, Nilmara; Brito, Joel; Caumo, Sofia; Arana, Andrea; de Souza Hacon, Sandra; Artaxo, Paulo; Hillamo, Risto; Teinilä, Kimmo; Batistuzzo de Medeiros, Silvia Regina; de Castro Vasconcellos, Pérola

    2015-11-01

    The Brazilian Amazon represents about 40% of the world's remaining tropical rainforest. However, human activities have become important drivers of disturbance in that region. The majority of forest fire hotspots in the Amazon arc due to deforestation are impacting the health of the local population of over 10 million inhabitants. In this study we characterize western Amazonia biomass burning emissions through the quantification of 14 Polycyclic Aromatic Hydrocarbons (PAHs), Organic Carbon, Elemental Carbon and unique tracers of biomass burning such as levoglucosan. From the PAHs dataset a toxic equivalence factor is calculated estimating the carcinogenic and mutagenic potential of biomass burning emissions during the studied period. Peak concentration of PM10 during the dry seasons was observed to reach 60 μg m-3 on the 24 h average. Conversely, PM10 was relatively constant throughout the wet season indicating an overall stable balance between aerosol sources and sinks within the filter sampling resolution. Similar behavior is identified for OC and EC components. Levoglucosan was found in significant concentrations (up to 4 μg m-3) during the dry season. Correspondingly, the estimated lung cancer risk calculated during the dry seasons largely exceeded the WHO health-based guideline. A source apportionment study was carried out through the use of Absolute Principal Factor Analysis (APFA), identifying a three-factor solution. The biomass burning factor is found to be the dominating aerosol source, having 75.4% of PM10 loading. The second factor depicts an important contribution of several PAHs without a single source class and therefore was considered as mixed sources factor, contributing to 6.3% of PM10. The third factor was mainly associated with fossil fuel combustion emissions, contributing to 18.4% of PM10. This work enhances the knowledge of aerosol sources and its impact on climate variability and local population, on a site representative of the

  3. Aerosol source apportionment based on multi-wavelength photoacoustic light absorption measurements: a simulation method for system's optimisation

    NASA Astrophysics Data System (ADS)

    Simon, Károly; Ajtai, Tibor; Kiss-Albert, Gergely; Utry, Noémi; Pintér, Máté; Szabó, Gábor; Bozóki, Zoltán

    2017-04-01

    Aerosol source apportionment is currently one of the outstanding challenges for environmental monitoring. In most cases atmospheric aerosol is a heterogeneous mixture as it typically originates from various sources. Consequently, each aerosol type has distinct chemical and physical properties. Contrary to chemical properties, optical absorption and size distribution of airborne particles can be measured in real time with high time resolution i.e. their measurement facilitates real time source apportionment (Favez et al (2009), Ajtai et al (2011), Favez et al (2010)). The wavelength dependency of the optical absorption coefficient (OAC) is usually characterised by the Absorption Angström Exponent (AAE). So far, the selection of light sources (lasers) into a photoacoustic aerosol measuring system was based on rule of thumb type estimations only. Recently, we proposed a simulation method that can be used to estimate the accuracy of aerosol source apportionment in case of a dual wavelength photoacoustic system (Simon et al., (2017)). This simulation is based on the assumption that the atmospheric aerosol load is dominated by two distinct sources and each of them is strongly light absorbing with specific AAE values. This is a typical scenario e.g. for urban measurements under wintry conditions when dominating aerosol sources are fossil fuel and wood burning with characteristic AAE 1 and 2, respectively. The wavelength pair of 405 and 1064 nm was found to be optimal for source apportionment in this case. In the presented study we investigated the situation when there are aerosol components with only slightly different AAE values and searched for a photoacoustic system which is optimal for distinguishing these components. Ajtai, T.; Filep, Á.; Utry, N.; Schnaiter, M.; Linke, C.; Bozóki, Z.; Szabó, G. and Leisner T. (2011) Journal of Aerosol Science 42, 859-866. Favez, O.; Cachier, H.; Sciare, J.; Sarda-Estève, R. and Martinon, L. (2009) Atmospheric Environment 43

  4. Source apportionment of PM2.5 carbonaceous aerosol in Baghdad, Iraq

    NASA Astrophysics Data System (ADS)

    Hamad, Samera Hussein; Schauer, James Jay; Heo, Jongbae; Kadhim, Ahmed K. H.

    2015-04-01

    Baghdad is the second largest city in the Middle East and suffers from severe air quality degradation due to the high levels of the atmospheric particulate matter (PM). Limited information exists regarding the sources of PM in Baghdad, and the lack of information on sources inhibits the development of control strategies to reduce air pollution. To better understand the nature of fine particulate matter (PM2.5) in Baghdad and the Middle East, a one year sampling campaign to collect PM2.5 was conducted from September 2012 through September 2013, missing August 2013 samples due to the security situation. 24-hour integrated samples collected on a 1-in-6 day schedule were analyzed for the major components, and monthly average samples were analyzed by gas chromatography mass spectrometry (GCMS) methods to measure particle-phase organic molecular markers. The results of organic molecular markers were used in a chemical mass balance (CMB) model to quantify the sources of PM2.5 organic carbon (OC) and PM2.5 mass. Primary sources accounted for 44% of the measured PM2.5, and secondary sources were estimated to make up 28% of the measured PM2.5. Picene, a tracer of coal combustion detected in Baghdad where there is no evidence for coal combustion, can be attributed to burning crude oil and other low quality fuels in Baghdad. Source apportionment results showed that the dominant sources of the carbonaceous aerosols in Baghdad are gasoline (37 ± 6%) and diesel engines (17 ± 3%) which can be attributed to the extensive use of gasoline and diesel powered generators in Baghdad. Wood burning and residual oil combustion contributed to 5 ± 0.4 and 1 ± 0.2% respectively of OC. The unresolved sources contributed to 42 ± 19% of the OC which represented the secondary organic aerosol (SOA) and the unidentified sources.

  5. Source apportionment of carbonaceous aerosol in Sao Paulo using 13C and 14C measurements

    NASA Astrophysics Data System (ADS)

    Oyama, Beatriz; Andrade, Maria de Fatima; Holzinger, Rupert; Röckmann, Thomas; Meijer, Harro A. J.; Dusek, Ulrike

    2016-04-01

    The Metropolitan Area of Sao Paulo is affected by high aerosol concentrations, which contain a large fraction of organic material. Up to date, not much is known about the composition and origin of the organic aerosol in this city. We present the first source apportionment of the carbonaceous aerosol fraction in Sao Paulo, using stable (13C) and radioactive carbon isotopes (14C). 14C provides a clear-cut distinction between fossil sources, which contain no 14C, and contemporary sources such as biofuels, biomass burning, or biogenic sources, which contain a typical contemporary 14C/12C ratio. 13C can be used to distinguish C3 plants, such as maize and sugarcane, from C4 plants. This can help to identify a possible impact of sugarcane field burning in the rural areas of Sao Paulo State on the aerosol carbon in the city. In the first part of the study, we compare two tunnel studies: Tunnel 1 is frequented only by light duty vehicles, which run mainly on mixtures of gasoline with ethanol (gasohol, 25% ethanol and 85% gasoline) or hydrated ethanol (5% water and 95% ethanol). Tunnel 2 contains a significant fraction of heavy-duty diesel vehicles, and therefore the fraction of biofuels in the average fleet is lower. Comparison of 14C in organic and elemental carbon (OC and EC) shows that in both tunnels there is no significant contribution of biofuels to EC. Combusting ethanol-gasoline fuels in a vehicle engine does apparently not result in significant EC formation from ethanol. Biofuels contribute around 45% to OC in Tunnel 1 an only 20% in Tunnel 2, reflecting a strong impact of diesel vehicles in Tunnel 2. In the second part of the study we conduct a source apportionment of ambient aerosol carbon collected in a field study during winter (July-August) 2012. Ambient EC has two main sources, vehicular emissions and biomass burning. We estimate a contribution of vehicular sources to EC of roughly 90% during weekdays and 80% during weekends, using the 14C values measured in

  6. Source Apportionment of Carbonaceous Aerosols at Two Sites on the North Slope of Alaska

    NASA Astrophysics Data System (ADS)

    Moffett, C. E.; Barrett, T. E.; Gunsch, M.; Pratt, K.; Sheesley, R. J.

    2016-12-01

    Aerosols both directly and indirectly affect the Earth's albedo by scattering or absorbing solar radiation and acting as cloud and ice condensation nuclei. In order to better understand the variability of aerosol sources in the Alaskan Arctic, this study utilizes radiocarbon analysis for the apportionment of total organic carbon to fossil and contemporary carbon sources. Fossil sources include fossil fuel combustion and secondary organic aerosol (SOA) from fossil precursors while contemporary sources include biomass combustion, primary biogenic emissions, and SOA produced from biogenic and biomass combustion-derived precursors. Total suspended particulate (TSP) samples were collected in August/September 2015 at two Department of Energy Atmospheric Radiation Measurement climate research facilities. Barrow, AK, is located on the northern most point of the United States; the site is 7.4 km north of the village of Barrow (population 4,581). Research shows the site receives minimal aerosol contribution from the village with dominant contributions from long range transport. Oliktok Point, AK, is 300 km south east of Barrow in a region of intense petroleum development. It receives contributions from the petroleum industry surrounding it as well as from long range transport. The proximity of the two sites allows for a finer spatial analysis of Arctic carbonaceous aerosol source contributions. Samples were analyzed for organic carbon (OC), elemental carbon (EC), and radiocarbon (14C) abundance. Preliminary results show Barrow had OC concentrations from 0.05 to 0.16 µg/m3, while Oliktok had concentrations of OC from 0.11 to 0.27 µg/m3. EC concentrations ranged from 0.002 to 0.013 µg/m3 in Barrow, 0.002 to 0.088 µg/m3 in Oliktok. In Barrow, 14C abundance shows the contribution of fossil sources remained in the range of 21% to 28%. At Oliktok, analysis reveals an increase from 30% contribution from fossil sources in August to a 70% contribution at the end of September.

  7. Source apportionment of aerosol particles near a steel plant by electron microscopy.

    PubMed

    Ebert, Martin; Müller-Ebert, Dörthe; Benker, Nathalie; Weinbruch, Stephan

    2012-12-01

    The size, morphology and chemical composition of 37,715 individual particles collected over 22 sampling days in the vicinity of a large integrated steel production were studied by scanning and transmission electron microscopy. Based on the morphology, chemistry and beam stability the particles were classified into the following fourteen groups: silicates, sea salt, calcium sulfates, calcium carbonates, carbonate-silicate mixtures, sulfate-silicate mixtures, iron oxides, iron mixtures, metal oxide-metals, complex secondary particles, soot, Cl-rich particles, P-rich particles, and other particles. The majority of iron oxide (≈85%) and metal oxide-metal (≈70%) particles as well as ≈20% of the silicate particles are fly ashes from high temperature processes. The emissions from the steel work are dominated by iron oxide particles. For source apportionment, seven source categories and two sectors of local wind direction (industrial and urban background) were distinguished. In both sectors PM₁₀ consists of four major source categories: 35% secondary, 20% industrial, 17% soil and 16% soot in the urban background sector compared to 45% industrial, 20% secondary, 13% soil, and 9% soot in the industrial sector. As the secondary and the soot components are higher in the urban background sector than in the industrial sector, it is concluded that both components predominantly originate from urban background sources (traffic, coal burning, and domestic heating). Abatement measures should not only focus on the steel work but should also include the urban background aerosol.

  8. Source apportionment of secondary organic aerosol during a severe photochemical smog episode

    NASA Astrophysics Data System (ADS)

    Kleeman, Michael J.; Ying, Qi; Lu, Jin; Mysliwiec, Mitchel J.; Griffin, Robert J.; Chen, Jianjun; Clegg, Simon

    The UCD/CIT air quality model was modified to predict source contributions to secondary organic aerosol (SOA) by expanding the Caltech Atmospheric Chemistry Mechanism to separately track source apportionment information through the chemical reaction system as precursor species react to form condensable products. The model was used to predict source contributions to SOA in Los Angeles from catalyst-equipped gasoline vehicles, non-catalyst equipped gasoline vehicles, diesel vehicles, combustion of high sulfur fuel, other anthropogenic sources, biogenic sources, and initial/boundary conditions during the severe photochemical smog episode that occurred on 9 September 1993. Gasoline engines (catalyst+non-catalyst equipped) were found to be the single-largest anthropogenic source of SOA averaged over the entire model domain. The region-wide 24-h average concentration of SOA produced by gasoline engines was predicted to be 0.34 μg m -3 with a maximum 24-h average concentration of 1.81 μg m -3 downwind of central Los Angeles. The region-wide 24-h average concentration of SOA produced by diesel engines was predicted to be 0.02 μg m -3, with a maximum 24-h average concentration of 0.12 μg m -3 downwind of central Los Angeles. Biogenic sources are predicted to produce a region-wide 24-h average SOA value of 0.16 μg m -3, with a maximum 24-h average concentration of 1.37 μg m -3 in the less-heavily populated regions at the northern and southern edges of the air basin (close to the biogenic emissions sources). SOA concentrations associated with anthropogenic sources were weakly diurnal, with slightly lower concentrations during the day as mixing depth increased. SOA concentrations associated with biogenic sources were strongly diurnal, with higher concentrations of aqueous biogenic SOA at night when relative humidity (RH) peaked and little biogenic SOA formation during the day when RH decreased.

  9. Chemical characterization and source apportionment of submicron aerosols measured in Senegal during the 2015 SHADOW campaign

    NASA Astrophysics Data System (ADS)

    Rivellini, Laura-Hélèna; Chiapello, Isabelle; Tison, Emmanuel; Fourmentin, Marc; Féron, Anaïs; Diallo, Aboubacry; N'Diaye, Thierno; Goloub, Philippe; Canonaco, Francesco; Prévôt, André Stephan Henry; Riffault, Véronique

    2017-09-01

    The present study offers the first chemical characterization of the submicron (PM1) fraction in western Africa at a high time resolution, thanks to collocated measurements of nonrefractory (NR) species with an Aerosol Chemical Speciation Monitor (ACSM), black carbon and iron concentrations derived from absorption coefficient measurements with a 7-wavelength Aethalometer, and total PM1 determined by a TEOM-FDMS (tapered element oscillating microbalance-filtered dynamic measurement system) for mass closure. The field campaign was carried out over 3 months (March to June 2015) as part of the SHADOW (SaHAran Dust Over West Africa) project at a coastal site located in the outskirts of the city of Mbour, Senegal. With an averaged mass concentration of 5.4 µg m-3, levels of NR PM1 in Mbour were 3 to 10 times lower than those generally measured in urban and suburban polluted environments. Nonetheless the first half of the observation period was marked by intense but short pollution events (NR PM1 concentrations higher than 15 µg m-3), sea breeze phenomena and Saharan desert dust outbreaks (PM10 up to 900 µg m-3). During the second half of the campaign, the sampling site was mainly under the influence of marine air masses. The air masses on days under continental and sea breeze influences were dominated by organics (36-40 %), whereas sulfate particles were predominant (40 %) for days under oceanic influence. Overall, measurements showed that about three-quarters of the total PM1 were explained by NR PM1, BC (black carbon) and Fe (a proxy for dust) concentrations, leaving approximately one-quarter for other refractory species. A mean value of 4.6 % for the Fe / PM1 ratio was obtained. Source apportionment of the organic fraction, using positive matrix factorization (PMF), highlighted the impact of local combustion sources, such as traffic and residential activities, which contribute on average to 52 % of the total organic fraction. A new organic aerosol (OA) source

  10. Measurement of Organic and Inorganic Chemical Tracers for Source Apportionment of Tropospheric Aerosols Collected During the ACE-Asia Experiment

    NASA Astrophysics Data System (ADS)

    Schauer, J. J.; Park, J.; Duvall, R.; Bae, M.; Shafer, M. M.; Chuang, P.; Chuang, P.; Kim, Y. J.

    2001-12-01

    Naturally occurring dust and anthropogenic air pollutants are important contributors to tropospheric aerosols and impact air quality and the radiative balance of the Earth's atmosphere. In order to better understand the relationship between the origin, chemical composition and ultimate impact of Asian aerosols on climate forcing, aerosol samples were collected as part of the ACE-Asia experiment for detailed chemical analysis. Atmospheric particulate matter samples were collected from March 27, 2001 through May 6, 2001 at the ACE-Asia ground station located on Cheju Island, Korea. During this period, this region is impacted by anthropogenic air pollution emissions from highly urbanized region of Asia and by desert dust originating from northeastern Asia. As part of the experiment, atmospheric particulate matter samplers were also collected in urban and desert locations in Asia that represent regional sources of particulate matter in Asia. Size resolved aerosol samples were analyzed for trace metals by using microwave assisted-acid digestion and ICP-MS analysis, speciated organic compounds using solvent extraction and GC-MS analysis, as well as soluble ions and elemental and organic carbon (ECOC). These measurements provide fingerprints for source apportionment of the atmospheric particulate matter samples collected at the Cheju Island sampling site. The use of these chemical tracers for apportionment of wind-driven long range transported desert dust, local crustal derived dust, biogenically and anthropogenically derived sulfate, specific urban combustion source, and fossil fuel combustion will be presented.

  11. Atmospheric aerosol compositions over the South China Sea: temporal variability and source apportionment

    NASA Astrophysics Data System (ADS)

    Xiao, Hong-Wei; Xiao, Hua-Yun; Luo, Li; Shen, Chun-Yan; Long, Ai-Min; Chen, Lin; Long, Zhen-Hua; Li, Da-Ning

    2017-03-01

    In order to evaluate impacts of different source emission on marine atmospheric particles over the South China Sea (SCS), major inorganic ionic concentrations (Na+, Cl-, SO42-, Ca2+, Mg2+, K+, NH4+ and NO3-) were determined in total suspended particulates (TSPs) at Yongxing Island, from March 2014 to February 2015. The annual average concentration of TSPs was 89.6 ± 68.0 µg m-3, with 114.7 ± 82.1, 60.4 ± 27.0 and 59.5 ± 25.6 µg m-3 in cool, warm and transition seasons, respectively. Cl- had the highest concentration, with an annual average of 7.73 ± 5.99 µg m-3, followed by SO42- (5.54 ± 3.65 µg m-3), Na+ (4.00 ± 1.88 µg m-3), Ca2+ (2.15 ± 1.54 µg m-3), NO3- (1.95 ± 1.34 µg m-3), Mg2+ (0.44 ± 0.33 µg m-3), K+ (0.33 ± 0.22 µg m-3) and NH4+ (0.07 ± 0.07 µg m-3). Concentrations of TSPs and the major ions showed seasonal variations, which were higher in the cool season and lower in the warm and transition seasons. Factors of influence were wind speed, temperature, relatively humidity, rain and air mass source region. Back trajectories, concentration-weighted trajectories (CWTs), and positive matrix factorization (PMF) of chemical compositions were analyzed for source apportionment, source contribution and spatiotemporal variation of major ions. Back trajectories and CWTs showed that air masses at Yongxing Island were mainly from the northeast, southwest and southeast in the cool, warm and transition seasons, respectively. The PMF results showed that 77.4 % of Na+ and 99.3 % of Cl- were from sea salt; 60.5 % of NH4+ was from oceanic emission. Anthropogenic sources were very important for atmospheric aerosols over the island. Secondary inorganic aerosol of SO2 and NOx from fossil fuel combustion (especially coal in Chinese coastal regions) was the dominant source of NO3- (69.5 %) and SO42- (57.5 %).

  12. Source apportionment of organic aerosol across Houston, TX during DISCOVER-AQ

    NASA Astrophysics Data System (ADS)

    Yoon, S.; Clark, A. E.; Ortiz, S. M.; Usenko, S.; Sheesley, R. J.

    2015-12-01

    As part of the ground-based sampling efforts during DISCOVER-AQ's Houston month-long campaign in September 2013, atmospheric particulate matter (PM) samples were collected at four sites: Moody Tower (urban), Manvel Croix (southern suburb), Conroe (northern suburb), and La Porte (urban industrial). The Houston metropolitan area, especially the Houston Ship Channel, is a densely industrialized urban city with large concentrations of petroleum refining, petrochemical manufacturing, and heavy traffic during peak hours. Due to these and other emission sources, the area is heavily impacted by ambient PM. This study will be looking at fine PM (diameter less than 2.5µm, PM2.5) from all four sites. PM2.5fraction is relevant for understanding fate and transport of organic contaminants and is widely known to negatively impact human health. Chemical analysis including radiocarbon (14C) and organic tracer measurements (polycyclic aromatic hydrocarbons, alkanes, hopanes, steranes, and levoglucosan) were used for source apportionment. The 14C measurements constrained CMB results to estimate both primary and secondary contributions to total organic carbon (TOC). Results indicate that Moody Tower had consistent primary motor vehicle exhaust contribution (18-27%) and a fossil secondary organic aerosol (SOA) contribution from 5-33% depending on atmospheric conditions. Conroe had a lower contribution of motor vehicle exhaust (5-10%) and similarly variable fraction of fossil SOA (4-25%). Manvel Croix had an interim motor vehicle contribution (9-15%) with a variable fossil SOA (5-30%). For contemporary OC, there was minimal contribution of wood smoke during examined weeks (0-9%) but larger contributor of biogenic SOA ranging from 40-75% at Moody Tower, 56-81% at Manvel Croix and 60-79% at Conroe. Overall, the motor vehicle contribution was consistent at each site during the analysis week, biogenic SOA was consistently high, while fossil SOA showed the most variability.

  13. Organic composition and source apportionment of fine aerosol at Monterrey, Mexico, based on organic markers

    NASA Astrophysics Data System (ADS)

    Mancilla, Y.; Mendoza, A.; Fraser, M. P.; Herckes, P.

    2016-01-01

    attribution results obtained using the CMB (chemical mass balance) model indicate that emissions from motor vehicle exhausts are the most important, accounting for the 64 % of the PM2.5, followed by meat-cooking operations with 31 % The vegetative detritus and biomass burning had the smallest contribution (2.2 % of the PM2.5). To our knowledge, this is only the second study to explore the organic composition and source apportionment of fine organic aerosol based on molecular markers in Mexico and the first for the MMA. Particularly molecular marker were quantified by solvent extraction with dichloromethane, derivatization, and gas chromatography with mass spectrometry (GC/MS).

  14. Characterization of emissions from South Asian biofuels and application to source apportionment of carbonaceous aerosol in the Himalayas

    NASA Astrophysics Data System (ADS)

    Stone, Elizabeth A.; Schauer, James J.; Pradhan, Bidya Banmali; Dangol, Pradeep Man; Habib, Gazala; Venkataraman, Chandra; Ramanathan, V.

    2010-03-01

    This study focuses on improving source apportionment of carbonaceous aerosol in South Asia and consists of three parts: (1) development of novel molecular marker-based profiles for real-world biofuel combustion, (2) application of these profiles to a year-long data set, and (3) evaluation of profiles by an in-depth sensitivity analysis. Emissions profiles for biomass fuels were developed through source testing of a residential stove commonly used in South Asia. Wood fuels were combusted at high and low rates, which corresponded to source profiles high in organic carbon (OC) or high in elemental carbon (EC), respectively. Crop wastes common to the region, including rice straw, mustard stalk, jute stalk, soybean stalk, and animal residue burnings, were also characterized. Biofuel profiles were used in a source apportionment study of OC and EC in Godavari, Nepal. This site is located in the foothills of the Himalayas and was selected for its well-mixed and regionally impacted air masses. At Godavari, daily samples of fine particulate matter (PM2.5) were collected throughout the year of 2006, and the annual trends in particulate mass, OC, and EC followed the occurrence of a regional haze in South Asia. Maximum concentrations occurred during the dry winter season and minimum concentrations occurred during the summer monsoon season. Specific organic compounds unique to aerosol sources, molecular markers, were measured in monthly composite samples. These markers implicated motor vehicles, coal combustion, biomass burning, cow dung burning, vegetative detritus, and secondary organic aerosol as sources of carbonaceous aerosol. A molecular marker-based chemical mass balance (CMB) model provided a quantitative assessment of primary source contributions to carbonaceous aerosol. The new profiles were compared to widely used biomass burning profiles from the literature in a sensitivity analysis. This analysis indicated a high degree of stability in estimates of source

  15. Studying organic aerosols during bonfire night in Manchester: ME-2 source apportionment

    NASA Astrophysics Data System (ADS)

    Reyes Villegas, Ernesto; Allan, James

    2016-04-01

    Over the past decade, there has been an increasing interest in short-term events that negatively affect air quality (Zhao et al. 2014) such as bonfires and fireworks. In general, during these episodes, high particulate matter concentrations drop within 24 hrs; however, it is the fine fraction that dominates the emissions, known to have a potentially negative impact on air quality, thus the impact of bonfires/fireworks on air quality must be considered. Aerosols and gases were measured using a variety of instruments at The University of Manchester, sampling atmospheric emissions on Bonfire night, 5 November, one week before and one week later, in 2013 and 2014. The Multilinear Engine (ME-2) factorization tool was used through the recently developed source finder interface (SoFi, Canonaco et al. 2013) to identify sources of organic aerosols (OA) sampled with an Aerosol Mass Spectrometer (AMS). ME-2 identified five sources: solid fuel OA (SFOA), hydrocarbon like OA (HOA), cooking OA (COA), semi-volatile (SVOOA) and low volatility (LVOOA) during both years. In 2014, air pollutant concentrations were particularly high, with the highest SFOA concentrations being 20 μgm-3 at 20:30 hrs. when fireworks from different parks in Manchester were launched. Black carbon (BC) concentrations started increasing before the fireworks, around 18:00 hrs; these concentrations are representative of bonfire emissions. However, traffic emissions may be contributing to BC here; further work will be done to differentiate traffic emissions from solid fuel emissions. By analysing daily aerosol concentrations according to DEFRA's Daily Air Quality Index, it is possible to observe that in 2014, PM2.5 concentrations were considered to be high (65 μgm-3) while in 2013, PM2.5 concentrations were considered low (12 μgm-3); in the case of BBOA, concentrations ranged from 2.9 μgm-3 in 2014 to 0.65 μgm-3 in 2013. The discrepancy between these studies is mainly a result of different meteorological

  16. 14C-based Source Apportionment of Carbonaceous Aerosols in Switzerland for 2008 - 2012

    NASA Astrophysics Data System (ADS)

    Zotter, Peter; Ciobanu, Gabriela; Zhang, Yanlin; El-Haddad, Imad; Szidat, Sönke; Wacker, Lukas; Baltensperger, Urs; Prévôt, André

    2013-04-01

    Carbonaceous particles (total carbon, TC) are a major fraction of the fine aerosol and affect climate and human health. TC is classified into the sub-fractions elemental carbon (EC) and organic carbon (OC). EC originates only from fossil fuel combustion and biomass burning. OC can be emitted directly as primary organic aerosol from biogenic emissions, wood burning and fossil fuel combustion or can be formed in-situ in the atmosphere (secondary organic aerosol) (Szidat et al. 2006). Radiocarbon (14C) analysis is a direct and quantitative tool for distinguishing fossil and non-fossil sources, since 14C in fossil fuels is completely depleted whereas other sources have a contemporary 14C level. This study presents source apportionment results from the winter season over a time period of 5 years (2007/2008-2011/2012) using 14C measurements on aerosol filters collected simultaneously at 16 air quality monitoring stations across Switzerland. For every year 5 winter smog episode days were selected from which filters from all stations were analyzed. To resolve a good spatial variability 11 stations north and 5 stations south of the Alps were selected. This 14C data set is unique around the world concerning the number of analyzed filters and the duration. The filter sampling was conducted using high volume samplers with PM10 inlets and a time resolution of 24h. Separation of OC and EC was carried out using the THEODORE system (Szidat et al. 2004) and a Sunset EC/OC analyzer (Zhang et al. 2012), respectively. The resulting CO2 was cryo-trapped and sealed in glass ampoules for 14C measurements, performed with the Mini Carbon Dating System MICADAS (Ruff et al. 2007) at the Swiss Federal Institute of Technology (ETH) Zürich. The results for non-fossil (NF) OC (5 year average) are 81% ± 10% for north and 85% ± 8% for south of the Alps. ECNF values range from 31% to 53% north and from 36% to 66% south of the Alps. Both, the OCNF and ECNF show higher values south of the Alps

  17. Year-round radiocarbon-based source apportionment of carbonaceous aerosols at two background sites in South Asia

    NASA Astrophysics Data System (ADS)

    Sheesley, Rebecca J.; Kirillova, Elena; Andersson, August; Krusâ, Martin; Praveen, P. S.; Budhavant, Krishnakant; Safai, P. D.; Rao, P. S. P.; Gustafsson, Örjan

    2012-05-01

    Atmospheric Brown Clouds (ABC), regional-scale haze events, are a significant concern for both human cardiopulmonary health and regional climate impacts. In order to effectively mitigate this pollution-based phenomenon, it is imperative to understand the magnitude, scope and source of ABC in regions such as South Asia. Two sites in S. Asia were chosen for a 15-month field campaign focused on isotope-based source apportionment of carbonaceous aerosols in 2008-2009. Both the Maldives Climate Observatory in Hanimaadhoo (MCOH) and a mountaintop site in Sinhagad, India (SINH) act as regionally mixed receptor sites. Annual radiocarbon-based source apportionment for soot elemental carbon (SEC) at MCOH and SINH revealed 73 ± 6% and 59 ± 5% contribution from biomass combustion, respectively (remainder from fossil fuel). The contributions from biogenic/biomass combustion to total organic carbon were similar between MCOH and SINH (69 ± 5% and 64 ± 5, respectively). The biomass combustion contribution for SEC in the current study, especially the results from MCOH, shows good agreement with published black carbon emissions inventories for India. Geographic source assessment, including clustered back trajectory analysis and carbon contribution by source region, indicated that the highest SEC/TOC loads originated from the W. Indian coastal margin, including the coastal city of Mumbai, India. The winter dry season 14C-based source apportionment of the BC-tracing SEC fraction for 2006, 2008, 2009 were not statistically different (p = 0.7) and point to a near-constant two-thirds contribution from biomass combustion practices, including wood and other biofuels as well as burning of agricultural crop residues.

  18. Chinese province-scale source apportionments for sulfate aerosol in 2005 evaluated by the tagged tracer method.

    PubMed

    Itahashi, Syuichi; Hayami, Hiroshi; Yumimoto, Keiya; Uno, Itsushi

    2017-01-01

    Appropriate policies to improve air quality by reducing anthropogenic emissions are urgently needed. This is typified by the particulate matter (PM) problem and it is well known that one type of PM, sulfate aerosol (SO4(2-)), has a large-scale impact due to long range transport. In this study we evaluate the source-receptor relationships of SO4(2-) over East Asia for 2005, when anthropogenic sulfur dioxide (SO2) emissions from China peaked. SO2 emissions from China have been declining since 2005-2006, so the possible maximum impact of Chinese contributions of SO4(2-) is evaluated. This kind of information provides a foundation for policy making and the estimation of control effects. The tagged tracer method was applied to estimate the source apportionment of SO4(2-) for 31 Chinese province-scale regions. In addition, overall one-year source apportionments were evaluated to clarify the seasonal dependency. Model performance was confirmed by comparing with ground-based observations over mainland China, Taiwan, Korea, and Japan, and the model results fully satisfied the performance goal for PM. We found the following results. Shandong and Hebei provinces, which were the largest and second largest SO2 sources in China, had the greatest impact over the whole of East Asia with apportionments of around 10-30% locally and around 5-15% in downwind receptor regions during the year. Despite large SO2 emissions, the impact of south China (e.g., Guizhou, Guangdong, and Sichuan provinces) was limited to local impact. These results suggest that the reduction policy in south China contributes to improving the local air quality, whereas policies in north and central China are beneficial for both the whole of China and downwind regions. Over Taiwan, Korea, and Japan, the impact of China was dominant; however, local contributions were important during summer. Copyright © 2016 The Authors. Published by Elsevier Ltd.. All rights reserved.

  19. Size-segregated aerosol in a hot-spot pollution urban area: Chemical composition and three-way source apportionment.

    PubMed

    Bernardoni, V; Elser, M; Valli, G; Valentini, S; Bigi, A; Fermo, P; Piazzalunga, A; Vecchi, R

    2017-08-24

    In this work, a comprehensive characterisation and source apportionment of size-segregated aerosol collected using a multistage cascade impactor was performed. The samples were collected during wintertime in Milan (Italy), which is located in the Po Valley, one of the main pollution hot-spot areas in Europe. For every sampling, size-segregated mass concentration, elemental and ionic composition, and levoglucosan concentration were determined. Size-segregated data were inverted using the program MICRON to identify and quantify modal contributions of all the measured components. The detailed chemical characterisation allowed the application of a three-way (3-D) receptor model (implemented using Multilinear Engine) for size-segregated source apportionment and chemical profiles identification. It is noteworthy that - as far as we know - this is the first time that three-way source apportionment is attempted using data of aerosol collected by traditional cascade impactors. Seven factors were identified: wood burning, industry, resuspended dust, regional aerosol, construction works, traffic 1, and traffic 2. Further insights into size-segregated factor profiles suggested that the traffic 1 factor can be associated to diesel vehicles and traffic 2 to gasoline vehicles. The regional aerosol factor resulted to be the main contributor (nearly 50%) to the droplet mode (accumulation sub-mode with modal diameter in the range 0.5-1 μm), whereas the overall contribution from the two factors related to traffic was the most important one in the other size modes (34-41%). The results showed that applying a 3-D receptor model to size-segregated samples allows identifying factors of local and regional origin while receptor modelling on integrated PM fractions usually singles out factors characterised by primary (e.g. industry, traffic, soil dust) and secondary (e.g. ammonium sulphate and nitrate) origin. Furthermore, the results suggested that the information on size

  20. On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, Y. L.; Perron, N.; Ciobanu, V. G.; Zotter, P.; Minguillón, M. C.; Wacker, L.; Prévôt, A. S. H.; Baltensperger, U.; Szidat, S.

    2012-07-01

    Radiocarbon (14C) measurements of elemental carbon (EC) and organic carbon (OC) separately (as opposed to only total carbon, TC) allow an unambiguous quantification of their non-fossil and fossil sources and represent an improvement in carbonaceous aerosol source apportionment. Isolation of OC and EC for accurate 14C determination requires complete removal of interfering fractions with maximum recovery. To evaluate the extent of positive and negative artefacts during OC and EC separation, we performed sample preparation with a commercial Thermo-Optical OC/EC Analyser (TOA) by monitoring the optical properties of the sample during the thermal treatments. Extensive attention has been devoted to the set-up of TOA conditions, in particular, heating program and choice of carrier gas. Based on different types of carbonaceous aerosols samples, an optimised TOA protocol (Swiss_4S) with four steps is developed to minimise the charring of OC, the premature combustion of EC and thus artefacts of 14C-based source apportionment of EC. For the isolation of EC for 14C analysis, the water-extraction treatment on the filter prior to any thermal treatment is an essential prerequisite for subsequent radiocarbon; otherwise the non-fossil contribution may be overestimated due to the positive bias from charring. The Swiss_4S protocol involves the following consecutive four steps (S1, S2, S3 and S4): (1) S1 in pure oxygen (O2) at 375 °C for separation of OC for untreated filters, and water-insoluble organic carbon (WINSOC) for water-extracted filters; (2) S2 in O2 at 475 °C, followed by (3) S3 in helium (He) at 650 °C, aiming at complete OC removal before EC isolation and leading to better consistency with thermal-optical protocols like EUSAAR_2, compared to pure oxygen methods; and (4) S4 in O2 at 760 °C for recovery of the remaining EC. WINSOC was found to have a significantly higher fossil contribution than the water-soluble OC (WSOC). Moreover, the experimental results

  1. On the isolation of OC and EC and the optimal strategy of radiocarbon-based source apportionment of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Zhang, Y. L.; Perron, N.; Ciobanu, V. G.; Zotter, P.; Minguillón, M. C.; Wacker, L.; Prévôt, A. S. H.; Baltensperger, U.; Szidat, S.

    2012-11-01

    Radiocarbon (14C) measurements of elemental carbon (EC) and organic carbon (OC) separately (as opposed to only total carbon, TC) allow an unambiguous quantification of their non-fossil and fossil sources and represent an improvement in carbonaceous aerosol source apportionment. Isolation of OC and EC for accurate 14C determination requires complete removal of interfering fractions with maximum recovery. The optimal strategy for 14C-based source apportionment of carbonaceous aerosols should follow an approach to subdivide TC into different carbonaceous aerosol fractions for individual 14C analyses, as these fractions may differ in their origins. To evaluate the extent of positive and negative artefacts during OC and EC separation, we performed sample preparation with a commercial Thermo-Optical OC/EC Analyser (TOA) by monitoring the optical properties of the sample during the thermal treatments. Extensive attention has been devoted to the set-up of TOA conditions, in particular, heating program and choice of carrier gas. Based on different types of carbonaceous aerosols samples, an optimised TOA protocol (Swiss_4S) with four steps is developed to minimise the charring of OC, the premature combustion of EC and thus artefacts of 14C-based source apportionment of EC. For the isolation of EC for 14C analysis, the water-extraction treatment on the filter prior to any thermal treatment is an essential prerequisite for subsequent radiocarbon measurements; otherwise the non-fossil contribution may be overestimated due to the positive bias from charring. The Swiss_4S protocol involves the following consecutive four steps (S1, S2, S3 and S4): (1) S1 in pure oxygen (O2) at 375 °C for separation of OC for untreated filters and water-insoluble organic carbon (WINSOC) for water-extracted filters; (2) S2 in O2 at 475 °C followed by (3) S3 in helium (He) at 650 °C, aiming at complete OC removal before EC isolation and leading to better consistency with thermal-optical protocols

  2. Source apportionment of absorbing aerosols in the central Indo-Gangetic Plain

    NASA Astrophysics Data System (ADS)

    Vaishya, Aditya; Singh, Prayagraj; Rastogi, Shantanu; Babu, S. Suresh

    2016-05-01

    Atmospheric aerosols in the Indo-Gangetic Plain (IGP) depicts high spatial and temporal heterogeneity in their radiative properties. Despite the fact that significant advancement in terms of characterizing aerosols radiative and physiochemical properties in the IGP have been made, information regarding the organic content towards total absorbing aerosol budget is lacking. In the present study we have analyzed two years of aerosol spectral light absorption measurements from the central-IGP, Gorakhpur (26.75°N, 83.38°E, 85m amsl), in order to study their seasonal behavior and to quantify their magnitude in terms of absorbing aerosols loading and source speciation. Remote sensing data in the form of 'Cloud corrected Fire Count' from MODIS Terra and 'Absorption Aerosol Index' from OMI satellites platform have been used to identify absorbing aerosol source regions. Spectral absorption analysis reveals a four-fold enhancement in absorption in the winter (W) and the post-monsoon (PoM) seasons at UV wavelengths as compared to 880 nm on account of increased biomass aerosol contribution to total absorbing aerosol load. Despite having higher fire events and absorption aerosol index, both indicating high biomass burning activities, in the pre-monsoon (PM) season, aerosols from the biomass sources contribute ~ 27% during the W and the PoM seasons as against ~17% in the PM season to the total absorbing aerosol content. This is due to near stagnant wind conditions and shallow height of air masses travelling to the central IGP in the W and the PoM seasons.

  3. Aerosol black carbon quantification in the central Indo-Gangetic Plain: Seasonal heterogeneity and source apportionment

    NASA Astrophysics Data System (ADS)

    Vaishya, Aditya; Singh, Prayagraj; Rastogi, Shantanu; Babu, S. Suresh

    2017-03-01

    Two years of aerosol spectral light absorption measurements, using filter based technique, from the central Indo-Gangetic plain (IGP), Gorakhpur (26.75°N, 83.38°E, 85 m amsl), are analyzed to study their seasonal behavior and to quantify their magnitude in terms of absorbing aerosols loading and source speciation. Spectral absorption analysis reveals a four-fold enhancement in absorption in winter (W) and post-monsoon (PoM) seasons at UV wavelengths as compared to IR wavelengths on account of increased biomass burning aerosol contribution to total absorbing aerosol load. Aerosols from the biomass sources contribute 28% during W and PoM seasons as against 16% in pre-monsoon (PM) and monsoon (M) seasons to the total absorbing aerosol content. A Mode shift in the distribution of the Absorption Ångström exponent (α) from 1.3 to 1.6 from PM-M seasons to PoM-W seasons signifies change in source type of absorbing aerosols from fossil fuel to biomass burning and their relative source strength. Due to near stagnant wind conditions combined with shallow boundary layer height, where air masses travelling to the central IGP are confined to a smaller volume, in W and PoM seasons, local sources assume more prominence rather than long-range transport of aerosols. Long-term measurements of aerosols physicochemical and radiative properties from this measurement location will enhance our understanding of the complex aerosol system over the IGP and its climatic implications.

  4. A two year's source apportionment study of wood burning and traffic aerosols for urban and rural sites in Switzerland

    NASA Astrophysics Data System (ADS)

    Herich, H.; Hueglin, C.; Buchmann, B.

    2010-11-01

    The contributions of fossil fuel (FF) and wood burning (WB) emissions to black carbon (BC) have been investigated in the past by analysis of multi-wavelength aethalometer data. This approach utilize the stronger light absorption of WB aerosols in the near ultraviolet compared to the light absorption of aerosols from FF combustion. Here we present two years of seven-wavelength aethalometer data from one urban and two rural background sites in Switzerland measured from 2008-2010. The contribution of WB and FF to BC was directly determined from the absorption coefficients of FF and WB aerosols which were calculated by using confirmed absorption exponents and aerosol light absorption cross-sections that were determined for all sites. Reasonable separation of total BC into contributions from FF and WB was achieved for all sites and seasons. The obtained WB contributions to BC are well correlated with measured concentrations of levoglucosan and potassium while FF contributions to BC correlate nicely with NOx. These findings support our approach and show that the applied source apportionment of BC is well applicable for long-term data sets. During winter, we found that BC from WB contributes on average 24-29% to total BC at the considered measurement sites. This is a noticeable high fraction as the contribution of wood burning to the total final energy consumption is in Switzerland less than 4%.

  5. Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

    PubMed

    Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

    2014-09-15

    The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic

  6. SOURCE APPORTIONMENT OF PHOENIX PM2.5 AEROSOL WITH THE UNMIX RECEPTOR MODEL

    EPA Science Inventory

    The multivariate receptor model Unmix has been used to analyze a 3-yr PM2.5 ambient aerosol data set collected in Phoenix, AZ, beginning in 1995. The analysis generated source profiles and overall percentage source contribution estimates (SCE) for five source categories: ga...

  7. SOURCE APPORTIONMENT OF PHOENIX PM2.5 AEROSOL WITH THE UNMIX RECEPTOR MODEL

    EPA Science Inventory

    The multivariate receptor model Unmix has been used to analyze a 3-yr PM2.5 ambient aerosol data set collected in Phoenix, AZ, beginning in 1995. The analysis generated source profiles and overall percentage source contribution estimates (SCE) for five source categories: ga...

  8. European isotopic signatures for lead in atmospheric aerosols: a source apportionment based upon 206Pb/207Pb ratios.

    PubMed

    Flament, Pascal; Bertho, Marie-Laure; Deboudt, Karine; Véron, Alain; Puskaric, Emile

    2002-09-16

    To investigate the capability of the lead isotope signature technique to support a source apportionment study at a Continental scale, atmospheric particulate matter was collected at Cap Gris-Nez (Eastern Channel, northern France), over one year (1995-1996). Four days retrospective trajectories of air masses were available during each sampling experiment. Twenty-eight samples, for which the origin of aerosols was unambiguously determined, were selected for isotopic measurements. Considering the Enrichment Factors, EF(Crust) of lead and its size distribution, we show that lead is mostly from anthropogenic origin and mainly associated with [0.4 < diameter < 0.9 microm] particles. The extent to which various Continental sources influence the lead abundance in aerosols is exhibited by considering both the lead concentration and the origin of air masses. Lead concentration is higher by a factor of approximately seven, when air masses are derived from Continental Europe, by comparison with marine air masses. Taking into account these concentrations and the vertical movements of air masses, we compare the different isotopic compositions using a statistical non-parametric test (Kolmogorov-Smirnov). We produce evidence that, for most of the cases, air masses originating from Continental Europe exhibit a more radiogenic composition (1.134 < 206Pb/207Pb < 1.172) than air masses coming from the United Kingdom (1.106 < 206Pb/207Pb < 1.124). Generally, lead isotopic compositions in aerosols are clearly distinct from the gasoline signatures in European countries, strongly suggesting that automotive lead is no longer the major component of this metal in the air. Gasoline and industrial isotopic signatures could explain the origin of lead in our aerosol samples. A source apportionment based upon 206Pb/207Pb ratios, suggests that the difference between British (206Pb/207Pb = 1.122 +/- 0.038) and Continental (206Pb/207Pb = 1.155 +/- 0.022) signatures may be largely explained by

  9. The AIRPARIF-AEROSOL project: A comprehensive source apportionment study of fine aerosols (PM2.5) in the region of Paris (France)

    NASA Astrophysics Data System (ADS)

    Sciare, Jean; Ghersi, Veronique; Bressi, Michael; Lameloise, Philippe; Bonnaire, Nicolas; Rosso, Amandine; Nicolas, Jose; Moukhtar, Sophie; Ferron, Anais; Baumier, Dominique

    2010-05-01

    With a population of about 12 millions inhabitants (20% of the French population), Greater Paris (France) is one of the most populated megacity in Europe and among the few located in developed countries. Due to its favorable geographical situation (far from other big European cities and influenced very often by clean oceanic air masses), it may be considered as a good candidate for investigating the build-up of urban air pollution from temperate industrialized countries. Particulate mass of fine aerosols with aerodynamic diameter below 2.5μm (PM2.5) is continuously monitored at several stations from great Paris for almost 8 years by the local air quality network (AIRPARIF), using a conventional on-line automatic system (R&P TEOM; see Patashnik and Rupprecht, 1991). During the period 2000-2006, levels of PM2.5 in the region of Paris have shown rather stable yearly mean values ranging 13 to 16?g/m3 whereas most of the other pollutants monitored by AIRPARIF have shown a net decrease during this period (http:\\www.airparif.asso.fr). Since the year 2007, this situation has becoming worse for particulate pollution with a net increase of the yearly mean concentration of PM2.5 (up to 21?g/m3), which increase is partly due to the use of a new PM2.5 measurement technique (R&P TEOM-FDMS instrument) enabling a proper determination of the semi-volatile fraction of fine aerosols. Although this new method greatly improves the determination of PM2.5, it has also brought PM2.5 levels in the region of Paris closer to the 25?g/m3 yearly mean targeted value recommended by Europe for 2010 (limit value for 2015). Efficient abatement policies aiming at reducing levels of PM2.5 in the region of Paris will have to be fed by preliminary PM2.5 source apportionment studies and exhaustive aerosol chemistry studies (chemical mass balance) allowing a better separation between regional to continental aerosol sources. The objective of the AIRPARIF-AEROSOL project aims to perform a spatially- and

  10. Source apportionment of PM 2.5 and PM 10 aerosols in Brisbane (Australia) by receptor modelling

    NASA Astrophysics Data System (ADS)

    Chan, Y. C.; Simpson, R. W.; Mctainsh, G. H.; Vowles, P. D.; Cohen, D. D.; Bailey, G. M.

    Aerosol samples for PM 2.5 and PM 10 (particulate matter with aerodynamic diameters less than 2.5 and 10 μm, respectively) were collected from 1993 to 1995 at five sites in Brisbane, a subtropical coastal city in Australia. This paper investigates the contributions of emission sources to PM 2.5 and PM 10 aerosol mass in Brisbane. Source apportionment results derived from the chemical mass balance (CMB), target transformation factor analysis (TTFA) and multiple linear regression (MLR) methods agree well with each other. The contributions from emission sources exhibit large variations in particle size with temporal and spatial differences. On average, the major contributors of PM 10 aerosol mass in Brisbane include: soil/road side dusts (25% by mass), motor vehicle exhausts (13%, not including the secondary products), sea salt (12%), Ca-rich and Ti-rich compounds (11%, from cement works and mineral processing industries), biomass burning (7%), and elemental carbon and secondary products contribute to around 15% of the aerosol mass on average. The major sources of PM 2.5 aerosols at the Griffith University (GU) site (a suburban site surrounded by forest area) are: elemental carbon (24% by mass), secondary organics (21%), biomass burning (15%) and secondary sulphate (14%). Most of the secondary products are related to motor vehicle exhausts, so, although motor vehicle exhausts contribute directly to only 6% of the PM 2.5 aerosol mass, their total contribution (including their secondary products) could be substantial. This pattern of source contribution is similar to the results for Rozelle (Sydney) among the major Australian studies, and is less in contributions from industrial and motor vehicular exhausts than the other cities. An attempt was made to estimate the contribution of rural dust and road side dust. The results show that road side dusts could contribute more than half of the crustal matter. More than 80% of the contribution of vehicle exhausts arises from

  11. Isotope-Based Source Apportionment of EC Aerosol Particles during Winter High-Pollution Events at the Zeppelin Observatory, Svalbard.

    PubMed

    Winiger, Patrik; Andersson, August; Yttri, Karl E; Tunved, Peter; Gustafsson, Örjan

    2015-10-06

    Black carbon (BC) aerosol particles contribute to climate warming of the Arctic, yet both the sources and the source-related effects are currently poorly constrained. Bottom-up emission inventory (EI) approaches are challenged for BC in general and the Arctic in particular. For example, estimates from three different EI models on the fractional contribution to BC from biomass burning (north of 60° N) vary between 11% and 68%, each acknowledging large uncertainties. Here we present the first dual-carbon isotope-based (Δ(14)C and δ(13)C) source apportionment of elemental carbon (EC), the mass-based correspondent to optically defined BC, in the Arctic atmosphere. It targeted 14 high-loading and high-pollution events during January through March of 2009 at the Zeppelin Observatory (79° N; Svalbard, Norway), with these representing one-third of the total sampling period that was yet responsible for three-quarters of the total EC loading. The top-down source-diagnostic (14)C fingerprint constrained that 52 ± 15% (n = 12) of the EC stemmed from biomass burning. Including also two samples with 95% and 98% biomass contribution yield 57 ± 21% of EC from biomass burning. Significant variability in the stable carbon isotope signature indicated temporally shifting emissions between different fossil sources, likely including liquid fossil and gas flaring. Improved source constraints of Arctic BC both aids better understanding of effects and guides policy actions to mitigate emissions.

  12. Organic aerosol source apportionment in London 2013 with ME-2: exploring the solution space with annual and seasonal analysis

    NASA Astrophysics Data System (ADS)

    Reyes-Villegas, Ernesto; Green, David C.; Priestman, Max; Canonaco, Francesco; Coe, Hugh; Prévôt, André S. H.; Allan, James D.

    2016-12-01

    The multilinear engine (ME-2) factorization tool is being widely used following the recent development of the Source Finder (SoFi) interface at the Paul Scherrer Institute. However, the success of this tool, when using the a value approach, largely depends on the inputs (i.e. target profiles) applied as well as the experience of the user. A strategy to explore the solution space is proposed, in which the solution that best describes the organic aerosol (OA) sources is determined according to the systematic application of predefined statistical tests. This includes trilinear regression, which proves to be a useful tool for comparing different ME-2 solutions. Aerosol Chemical Speciation Monitor (ACSM) measurements were carried out at the urban background site of North Kensington, London from March to December 2013, where for the first time the behaviour of OA sources and their possible environmental implications were studied using an ACSM. Five OA sources were identified: biomass burning OA (BBOA), hydrocarbon-like OA (HOA), cooking OA (COA), semivolatile oxygenated OA (SVOOA) and low-volatility oxygenated OA (LVOOA). ME-2 analysis of the seasonal data sets (spring, summer and autumn) showed a higher variability in the OA sources that was not detected in the combined March-December data set; this variability was explored with the triangle plots f44 : f43 f44 : f60, in which a high variation of SVOOA relative to LVOOA was observed in the f44 : f43 analysis. Hence, it was possible to conclude that, when performing source apportionment to long-term measurements, important information may be lost and this analysis should be done to short periods of time, such as seasonally. Further analysis on the atmospheric implications of these OA sources was carried out, identifying evidence of the possible contribution of heavy-duty diesel vehicles to air pollution during weekdays compared to those fuelled by petrol.

  13. Carbonaceous aerosol source apportionment using the Aethalometer model - evaluation by radiocarbon and levoglucosan analysis at a rural background site in southern Sweden

    NASA Astrophysics Data System (ADS)

    Martinsson, Johan; Azeem, Hafiz Abdul; Sporre, Moa K.; Bergström, Robert; Ahlberg, Erik; Öström, Emilie; Kristensson, Adam; Swietlicki, Erik; Eriksson Stenström, Kristina

    2017-03-01

    With the present demand on fast and inexpensive aerosol source apportionment methods, the Aethalometer model was evaluated for a full seasonal cycle (June 2014-June 2015) at a rural atmospheric measurement station in southern Sweden by using radiocarbon and levoglucosan measurements. By utilizing differences in absorption of UV and IR, the Aethalometer model apportions carbon mass into wood burning (WB) and fossil fuel combustion (FF) aerosol. In this study, a small modification in the model in conjunction with carbon measurements from thermal-optical analysis allowed apportioned non-light-absorbing biogenic aerosol to vary in time. The absorption differences between WB and FF can be quantified by the absorption Ångström exponent (AAE). In this study AAEWB was set to 1.81 and AAEFF to 1.0. Our observations show that the AAE was elevated during winter (1.36 ± 0.07) compared to summer (1.12 ± 0.07). Quantified WB aerosol showed good agreement with levoglucosan concentrations, both in terms of correlation (R2 = 0. 70) and in comparison to reference emission inventories. WB aerosol showed strong seasonal variation with high concentrations during winter (0.65 µg m-3, 56 % of total carbon) and low concentrations during summer (0.07 µg m-3, 6 % of total carbon). FF aerosol showed less seasonal dependence; however, black carbon (BC) FF showed clear diurnal patterns corresponding to traffic rush hour peaks. The presumed non-light-absorbing biogenic carbonaceous aerosol concentration was high during summer (1.04 µg m-3, 72 % of total carbon) and low during winter (0.13 µg m-3, 8 % of total carbon). Aethalometer model results were further compared to radiocarbon and levoglucosan source apportionment results. The comparison showed good agreement for apportioned mass of WB and biogenic carbonaceous aerosol, but discrepancies were found for FF aerosol mass. The Aethalometer model overestimated FF aerosol mass by a factor of 1.3 compared to radiocarbon and levoglucosan

  14. Source apportionment of the carbonaceous aerosol - Quantitative estimates based on 14C- and organic tracer analysis

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Svendby, T. M.; Simpson, D.; Puxbaum, H.; Stenström, K.

    2009-04-01

    The World Health Organization (WHO) points towards combustion derived primary particles when ascribing the negative health effects that ambient particles have on human health. These particles consist mainly of carbonaceous material. Further, great uncertainties are associated with the contribution from natural sources to the ambient carbonaceous aerosol concentration. Until recently there has been no way of separating such particles from particles from other sources in the ambient air. By the combined effort of thermal optical, 14C-, and organic tracer analysis this is now possible. When treating such data statistically using Latin Hypercube Sampling (LHS), we are able to apportion the ambient aerosol carbonaceous material to a total of seven different sources, i.e. Elemental carbon from combustion of biomass (ECbb) and fossil fuel (ECff), organic carbon from combustion of biomass (OCbb) and fossil fuel (OCff), primary biogenics (OCpb), and secondary organic aerosols from anthropogenic and (ASOA) and biogenic (BSOA) precursors. The current approach makes it possible to separate not only primary versus secondary aerosols, but also to separate between natural and anthropogenic sources, which is highly important in order to sort out abatement strategies for reducing man-made emissions of combustion derived primary particles. The carbonaceous aerosol originating from the above mentioned seven sources has been examined with respect to size fraction (PM10 and PM1), time of the day and season for one rural background site (Hurdal) and one urban background site (Oslo) in Norway. Briefly, the results show that combustion derived primary particles (ECbb, ECff, OCbb, OCff) accounted for 45% of the carbonaceous material in PM10 in Oslo in summer, whereas 46% of the carbonaceous material came from natural sources (OCpb, BSOA). For PM1, combustion derived primary particles accounted for 47% of the carbonaceous material, whereas 36% originated from natural sources. The major

  15. Online coupling of pure O2 thermo-optical methods - 14C AMS for source apportionment of carbonaceous aerosols

    NASA Astrophysics Data System (ADS)

    Agrios, Konstantinos; Salazar, Gary; Zhang, Yan-Lin; Uglietti, Chiara; Battaglia, Michael; Luginbühl, Marc; Ciobanu, Viorela Gabriela; Vonwiller, Matthias; Szidat, Sönke

    2015-10-01

    This paper reports on novel separation methods developed for the direct determination of 14C in organic carbon (OC) and elemental carbon (EC), two sub-fractions of total carbon (TC) of atmospheric air particulate matter. Until recently, separation of OC and EC has been performed off-line by manual and time-consuming techniques that relied on the collection of massive CO2 fractions. We present here two on-line hyphenated techniques between a Sunset OC/EC analyzer and a MICADAS (MIni radioCArbon DAting System) accelerator mass spectrometer (AMS) equipped with a gas ion source. The first implementation facilitates the direct measurement in the low sample size range (<10 μg C) with high throughput on a routine basis, while the second explores the potential for a continuous-flow real-time CO2 gas feed into the ion source. The performance achieved with reference materials and real atmospheric samples will be discussed to draw conclusions on the improvement offered in the field of 14C aerosol source apportionment.

  16. Chemical characterization of PM1.0 aerosol in Delhi and source apportionment using positive matrix factorization.

    PubMed

    Jaiprakash; Singhai, Amrita; Habib, Gazala; Raman, Ramya Sunder; Gupta, Tarun

    2017-01-01

    Fine aerosol fraction (particulate matter with aerodynamic diameter <= 1.0 μm (PM)1.0) over the Indian Institute of Technology Delhi campus was monitored day and night (10 h each) at 30 m height from November 2009 to March 2010. The samples were analyzed for 5 ions (NH4(+), NO3(-), SO4(2-), F(-), and Cl(-)) and 12 trace elements (Na, K, Mg, Ca, Pb, Zn, Fe, Mn, Cu, Cd, Cr, and Ni). Importantly, secondary aerosol (sulfate and nitrate) formation was observed during dense foggy events, supporting the fog-smog-fog cycle. A total of 76 samples were used for source apportionment of PM mass. Six factors were resolved by PMF analyses and were identified as secondary aerosol, secondary chloride, biomass burning, soil dust, iron-rich source, and vehicular emission. The geographical location of the sources and/or preferred transport pathways was identified by conditional probability function (for local sources) and potential source contribution function (for regional sources) analyses. Medium- and small-scale metal processing (e.g. steel sheet rolling) industries in Haryana and National Capital Region (NCR) Delhi, coke and petroleum refining in Punjab, and thermal power plants in Pakistan, Punjab, and NCR Delhi were likely contributors to secondary sulfate, nitrate, and secondary chloride at the receptor site. The agricultural residue burning after harvesting season (Sept-Dec and Feb-Apr) in Punjab, and Haryana contributed to potassium at receptor site during November-December and March 2010. The soil dust from North and East Pakistan, and Rajasthan, North-East Punjab, and Haryana along with the local dust contributed to soil dust at the receptor site, during February and March 2010. A combination of temporal behavior and air parcel trajectory ensemble analyses indicated that the iron-rich source was most likely a local source attributed to emissions from metal processing facilities. Further, as expected, the vehicular emissions source did not show any seasonality and was

  17. Source apportionment of carbonaceous aerosols in a megacity of northwest China: insights from radiocarbon measurement

    NASA Astrophysics Data System (ADS)

    Ni, Haiyan; Huang, Rujin; Dusek, Ulrike

    2017-04-01

    Fine particulate matter (PM2.5) samples were collected from 5 July 2008 to 27 June 2009 at Xi'an, a very polluted megacity in Northwest China. The 24 h averaged PM2.5concentrations (ranged from 32 μg m-3 to 339 μg m-3) were 1-14 times higher than the WHO guideline for 24 h PM2.5(25 μg m-3). In this work, we unambiguously quantify fossil (e.g., vehicle emissions, coal burning etc.) and non-fossil (e.g., biomass burning, cooking, biogenic emissions etc.) contributions to organic carbon (OC) and elemental carbon (EC) of PM2.5using radiocarbon (14C) measurement. In addition, we measured PM2.5 major components and source markers, including OC and EC, ions, trace elements, polycyclic aromatic hydrocarbons (PAHs), oxygenated PAHs (o-PAHs), anhydrous sugars and hopanes. The preliminary results of radiocarbon measurements in OC and EC show that the annual mean contributions from fossil-fuel combustion to EC was 76 ± 8% (6 ± 2 μg m-3). The remaining 24 ± 8% (2 ± 1 μg m-3) was attributed to biomass burning, with higher contribution in the cold period (˜33%) compared to the warm period (˜21%), due to enhanced emissions from local biomass burning activities in winter. In contrast with EC, OC was dominated by non-fossil sources, with an annual average of 54 ± 8 % (13 ± 10 μg m-3). Clear seasonal variations were seen in OC concentrations both from fossil fuel (OCff), and from non-fossil sources (OCnf), with maxima in the cold period and minima in the warm period, because of enhanced fossil and non-fossil activities in winter, mainly biomass burning and domestic coal burning. Further source apportionment of OC, including primary/secondary fossil OC, primary/secondary non-fossil OC, will be conducted by combining 14C results with positive matrix factorization (PMF) analysis of organic matter (OM).

  18. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    NASA Astrophysics Data System (ADS)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-01-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the Southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8±8.4 μg m-3 and 13.5±8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva)~200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  19. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    NASA Astrophysics Data System (ADS)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-07-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m-3 and 13.5 ± 8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva) ∼200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  20. Source apportionment of major and trace elements in aerosols during smog episodes in large cities in China

    NASA Astrophysics Data System (ADS)

    Furger, Markus; Rai, Pragati; Visser, Suzanne; Elser, Miriam; Canonaco, Francesco; Slowik, Jay G.; Huang, Ru-Jin; Prévôt, André S. H.; Baltensperger, Urs

    2017-04-01

    Air pollution in Chinese cities is one of the environmental problems China has to address to mitigate the impacts on human health, air quality and climate. Average concentrations of particulate matter exceed 100 μg m-3 in many places in China, and the government is developing and implementing strategies to reduce the load of pollutants by various measures. A characterization of airborne particulate matter (PM), especially its composition and sources, will help in optimizing reduction and mitigation strategies for air pollution. We collected PM10 aerosols with a rotating drum impactor (RDI) in Xi'an in December 2013 and in Beijing in January 2014 with 30-min time resolution and for three size ranges (cut-off sizes 10, 2.5 and 1 μm). Each campaign encompassed one or more high pollution episodes in the respective city. Elements from Na to Pb were analyzed with synchrotron radiation induced X-ray fluorescence spectrometry (SR-XRF), and the resulting time series were used for source apportionment performed with the Multilinear-Engine 2 (ME-2) implementation of the Positive Matrix Factorization algorithm. The preliminary computations yielded 5 factors for Beijing, namely road dust, sea salt, traffic-related, industrial, coal combustion. For Xi'an an additional desert dust factor was found. Further refinement could be expected from including the smaller size fractions, e.g. a sulfur-rich factor for secondary sulfate or a reacted chlorine factor in the fine mode fraction.

  1. Source apportionment of elevated BaP concentrations in PM10 aerosols in an alpine valley in Austria

    NASA Astrophysics Data System (ADS)

    Bauer, Heidi; Puxbaum, Hans; Jankowski, Nicole; Sampaio Cordeiro Wagner, Lylian

    2010-05-01

    INTRODUCTION: In a village situated at 1215 m a.s.l. in a natural preserve in an Austrian alpine valley elevated BaP concentrations have been measured in the last years. A highly frequented highway leading from Italy to Germany passes near the village. Monthly means of particulate BaP concentrations show a clear seasonal trend with values below 1 ng/m³ during the warmer months and with concentrations up to 9 ng/m³ in the cold season. Annual averages in the years 2000 - 2005 ranged between 1.4 and 2.8 ng/m³ - much higher than the EU target value of 1 ng/m³. We used a macrotracer model developed at the Vienna University of Technology to determine the contributions of the sources for BaP emissions, which were mainly space heating with wood and traffic from the highway. EXPERIMENTAL: The macrotracer concept is a nine component model to derive source contribution and explains 80-100% of PM10 aerosols in Austria. The amount of traffic exhaust is derived by using EC as tracer, whereas EC produced by wood burning is subtracted, the amount of wood smoke is derived by the anhydro-sugar levoglucosan and the ratio between the anhydro-sugars levoglucosan and mannosan. For the source apportionment of BaP the applied factors reflect on the one hand the composition of the automotive fleet in Austria and on the other hand the composition of the fire wood in the region. Filter samples collected with a high volume sampler in winter were analyzed for PM10 aerosol mass, total, organic, elemental and carbonate carbon, HULIS, anhydro-sugars, polyols and ions (major ions and organic acids) and PAHs. In the same way emission samples taken at a motor test stand and at a test stand for wood combustion were analyzed (Schmidl et al. 2008). The saccharides were determined using high pH anion exchange and pulsed amperometry (HPAE-PAD). Details of the analytical method are given in Iinuma et al., 2009. Elemental and organic carbon were determined with a thermal-optical instrument (Sunset lab

  2. A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

    NASA Astrophysics Data System (ADS)

    Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, Jose L.

    2016-11-01

    We present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography-mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level resolution on

  3. A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

    SciTech Connect

    Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; Docherty, Kenneth S.; Jimenez, Jose L.

    2016-11-25

    Here, we present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography–mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arranged into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level

  4. A technique for rapid source apportionment applied to ambient organic aerosol measurements from a thermal desorption aerosol gas chromatograph (TAG)

    DOE PAGES

    Zhang, Yaping; Williams, Brent J.; Goldstein, Allen H.; ...

    2016-11-25

    Here, we present a rapid method for apportioning the sources of atmospheric organic aerosol composition measured by gas chromatography–mass spectrometry methods. Here, we specifically apply this new analysis method to data acquired on a thermal desorption aerosol gas chromatograph (TAG) system. Gas chromatograms are divided by retention time into evenly spaced bins, within which the mass spectra are summed. A previous chromatogram binning method was introduced for the purpose of chromatogram structure deconvolution (e.g., major compound classes) (Zhang et al., 2014). Here we extend the method development for the specific purpose of determining aerosol samples' sources. Chromatogram bins are arrangedmore » into an input data matrix for positive matrix factorization (PMF), where the sample number is the row dimension and the mass-spectra-resolved eluting time intervals (bins) are the column dimension. Then two-dimensional PMF can effectively do three-dimensional factorization on the three-dimensional TAG mass spectra data. The retention time shift of the chromatogram is corrected by applying the median values of the different peaks' shifts. Bin width affects chemical resolution but does not affect PMF retrieval of the sources' time variations for low-factor solutions. A bin width smaller than the maximum retention shift among all samples requires retention time shift correction. A six-factor PMF comparison among aerosol mass spectrometry (AMS), TAG binning, and conventional TAG compound integration methods shows that the TAG binning method performs similarly to the integration method. However, the new binning method incorporates the entirety of the data set and requires significantly less pre-processing of the data than conventional single compound identification and integration. In addition, while a fraction of the most oxygenated aerosol does not elute through an underivatized TAG analysis, the TAG binning method does have the ability to achieve molecular level

  5. Receptor modeling of source apportionment of Hong Kong aerosols and the implication of urban and regional contribution

    NASA Astrophysics Data System (ADS)

    Guo, H.; Ding, A. J.; So, K. L.; Ayoko, G.; Li, Y. S.; Hung, W. T.

    Understanding the spatial-temporal variations of source apportionment of PM 2.5 is critical to the effective control of particulate pollution. In this study, two one-year studies of PM 2.5 composition were conducted at three contrasting sites in Hong Kong from November 2000 to October 2001, and from November 2004 to October 2005, respectively. A receptor model, principal component analysis (PCA) with absolute principal component scores (APCS) technique, was applied to the PM 2.5 data for the identification and quantification of pollution sources at the rural, urban and roadside sites. The receptor modeling results identified that the major sources of PM 2.5 in Hong Kong were vehicular emissions/road erosion, secondary sulfate, residual oil combustion, soil suspension and sea salt regardless of sampling sites and sampling periods. The secondary sulfate aerosols made the most significant contribution to the PM 2.5 composition at the rural (HT) (44 ± 3%, mean ± 1 σ standard error) and urban (TW) (28 ± 2%) sites, followed by vehicular emission (20 ± 3% for HT and 23 ± 4% for TW) and residual oil combustion (17 ± 2% for HT and 19 ± 1% for TW). However, at the roadside site (MK), vehicular emissions especially diesel vehicle emissions were the major source of PM 2.5 composition (33 ± 1% for diesel vehicle plus 18 ± 2% for other vehicles), followed by secondary sulfate aerosols (24 ± 1%). We found that the contribution of residual oil combustion at both urban and rural sites was much higher than that at the roadside site (2 ± 0.4%), perhaps due to the marine vessel activities of the container terminal near the urban site and close distance of pathway for the marine vessels to the rural site. The large contribution of secondary sulfate aerosols at all the three sites reflected the wide influence of regional pollution. With regard to the temporal trend, the contributions of vehicular emission and secondary sulfate to PM 2.5 showed higher autumn and winter values

  6. Size distribution, mixing state and source apportionment of black carbon aerosol in London during wintertime

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J. D.; Young, D. E.; Coe, H.; Beddows, D.; Fleming, Z. L.; Flynn, M. J.; Gallagher, M. W.; Harrison, R. M.; Lee, J.; Prevot, A. S. H.; Taylor, J. W.; Yin, J.; Williams, P. I.; Zotter, P.

    2014-09-01

    Black carbon aerosols (BC) at a London urban site were characterised in both winter- and summertime 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorisation (PMF) factors of organic aerosol mass spectra measured by a high-resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However, the size distribution of sf (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different sf distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC-AMS-PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), and easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm and 169 ± 29 nm, respectively. The corresponding bulk relative coating thickness of BC (coated particle size/BC core - Dp/Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0

  7. Size distribution, mixing state and source apportionments of black carbon aerosols in London during winter time

    NASA Astrophysics Data System (ADS)

    Liu, D.; Allan, J. D.; Young, D. E.; Coe, H.; Beddows, D.; Fleming, Z. L.; Flynn, M. J.; Gallagher, M. W.; Harrison, R. M.; Lee, J.; Prevot, A. S. H.; Taylor, J. W.; Yin, J.; Williams, P. I.; Zotter, P.

    2014-06-01

    Black carbon aerosols (BC) at a London urban site were characterized in both winter and summer time 2012 during the Clean Air for London (ClearfLo) project. Positive matrix factorization (PMF) factors of organic aerosol mass spectra measured by a high resolution aerosol mass spectrometer (HR-AMS) showed traffic-dominant sources in summer but in winter the influence of additional non-traffic sources became more important, mainly from solid fuel sources (SF). Measurements using a single particle soot photometer (SP2, DMT), showed the traffic-dominant BC exhibited an almost uniform BC core size (Dc) distribution with very thin coating thickness throughout the detectable range of Dc. However the size distribution of Dc (project average mass median Dc = 149 ± 22 nm in winter, and 120 ± 6 nm in summer) and BC coating thickness varied significantly in winter. A novel methodology was developed to attribute the BC number concentrations and mass abundances from traffic (BCtr) and from SF (BCsf), by using a 2-D histogram of the particle optical properties as a function of BC core size, as measured by the SP2. The BCtr and BCsf showed distinctly different Dc distributions and coating thicknesses, with BCsf displaying larger Dc and larger coating thickness compared to BCtr. BC particles from different sources were also apportioned by applying a multiple linear regression between the total BC mass and each AMS-PMF factor (BC-AMS-PMF method), and also attributed by applying the absorption spectral dependence of carbonaceous aerosols to 7-wavelength Aethalometer measurements (Aethalometer method). Air masses that originated from westerly (W), southeasterly (SE), or easterly (E) sectors showed BCsf fractions that ranged from low to high, and whose mass median Dc values were 137 ± 10 nm, 143 ± 11 nm, and 169 ± 29 nm respectively. The corresponding bulk relative coating thickness of BC (coated particle size / BC core - Dp / Dc) for these same sectors was 1.28 ± 0.07, 1.45 ± 0

  8. Source apportionment of fine organic aerosol in Mexico City during the MILAGRO Experiment 2006

    NASA Astrophysics Data System (ADS)

    Stone, E. A.; Snyder, D. C.; Sheesley, R. J.; Sullivan, A. P.; Weber, R. J.; Schauer, J. J.

    2007-07-01

    Organic carbon (OC) comprises a large fraction of fine particulate matter (PM2.5) in Mexico City. Daily and select 12-h PM2.5 samples were collected in urban and peripheral sites in Mexico City from 17-30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time water-soluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 47% of OC in the urban area and 31% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5-30% at the urban site and 11-50% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MILAGRO 2006 field campaign.

  9. Source apportionment of fine organic aerosol in Mexico City during the MILAGRO experiment 2006

    NASA Astrophysics Data System (ADS)

    Stone, E. A.; Snyder, D. C.; Sheesley, R. J.; Sullivan, A. P.; Weber, R. J.; Schauer, J. J.

    2008-03-01

    Organic carbon (OC) comprises a large fraction of fine particulate matter (PM2.5) in Mexico City. Daily and select 12-h PM2.5 samples were collected in urban and peripheral sites in Mexico City from 17-30 March 2006. Samples were analyzed for OC and elemental carbon (EC) using thermal-optical filter-based methods. Real-time water-soluble organic carbon (WSOC) was collected at the peripheral site. Organic compounds, particularly molecular markers, were quantified by soxhlet extraction with methanol and dichloromethane, derivitization, and gas chromatography with mass spectrometric detection (GCMS). A chemical mass balance model (CMB) based on molecular marker species was used to determine the relative contribution of major sources to ambient OC. Motor vehicles, including diesel and gasoline, consistently accounted for 49% of OC in the urban area and 32% on the periphery. The daily contribution of biomass burning to OC was highly variable, and ranged from 5-26% at the urban site and 7-39% at the peripheral site. The remaining OC unapportioned to primary sources showed a strong correlation with WSOC and was considered to be secondary in nature. Comparison of temporally resolved OC showed that contributions from primary aerosol sources during daylight hours were not significantly different from nighttime. This study provides quantitative understanding of the important sources of OC during the MILAGRO 2006 field campaign.

  10. Sensitivity and bias of molecular marker-based aerosol source apportionment models to small conltibutions of coal combustion soot.

    PubMed

    Rutter, Andrew P; Snyder, David C; Schauer, James J; DeMinter, Jeff; Shelton, Brandon

    2009-10-15

    Carbonaceous atmospheric particulate matter (PM25) collected in the midwestern United States revealed that soot emissions from incomplete coal combustion were important sources of several organic molecular markers used in source apportionment studies. Despite not constituting a major source of organic carbon in the PM25, coal soot was an important source of polyaromatic hydrocarbons, hopanes, and elemental carbon. These marker compounds are becoming widely used for source apportionment of atmospheric organic PM, meaning that significant emissions of these marker compounds from unaccounted sources such as coal soot could bias apportionment results. This concept was demonstrated using measurements of atmospheric PM collected on a 1-in-6 day schedule at three monitoring sites in Ohio: Mingo Junction (near Steubenville), Cincinnati, and Cleveland. Impacts of coal sootwere measured to be significant at Mingo Junction and small at Cleveland and Cincinnati. As a result, biases in apportionment results were substantial at Mingo Junction and insignificant at Cleveland and Cincinnati. Misapportionments of organic carbon mass at Mingo Junction were significant when coal soot was detected in the particulate samples as identified bythe presence of picene, but when coal soot was not included in the model: gasoline engines (+8% to +58% of OC), smoking engines (0% to -17% of OC), biomass combustion (+1% to +11% of OC), diesel engines (-1% to -2% of OC), natural gas combustion (0% to -2% of OC), and unapportioned OC (0% to -47% of OC). These results suggest that the role of coal soot in source apportionment studies needs to be better examined in many parts of the United States and other parts of the world.

  11. Radiocarbon-based source apportionment of elemental carbon aerosols at two South Asian receptor observatories over a full annual cycle

    NASA Astrophysics Data System (ADS)

    Budhavant, Krishnakant; Andersson, August; Bosch, Carme; Kruså, Martin; Kirillova, E. N.; Sheesley, R. J.; Safai, P. D.; Rao, P. S. P.; Gustafsson, Örjan

    2015-06-01

    Black carbon (BC) aerosols impact climate and air quality. Since BC from fossil versus biomass combustion have different optical properties and different abilities to penetrate the lungs, it is important to better understand their relative contributions in strongly affected regions such as South Asia. This study reports the first year-round 14C-based source apportionment of elemental carbon (EC), the mass-based correspondent to BC, using as regional receptor sites the international Maldives Climate Observatory in Hanimaadhoo (MCOH) and the mountaintop observatory of the Indian Institute of Tropical Meteorology in Sinhagad, India (SINH). For the highly-polluted winter season (December-March), the fractional contribution to EC from biomass burning (fbio) was 53 ± 5% (n = 6) at MCOH and 56 ± 3% at SINH (n = 5). The fbio for the non-winter remainder was 53 ± 11% (n = 6) at MCOH and 48 ± 8% (n = 7) at SINH. This observation-based constraint on near-equal contributions from biomass burning and fossil fuel combustion at both sites compare with predictions from eight technology-based emission inventory (EI) models for India of (fbio)EI spanning 55-88%, suggesting that most current EI for Indian BC systematically under predict the relative contribution of fossil fuel combustion. A continued iterative testing of bottom-up EI with top-down observational source constraints has the potential to lead to reduced uncertainties regarding EC sources and emissions to the benefit of both models of climate and air quality as well as guide efficient policies to mitigate emissions.

  12. Source apportionment of submicron organic aerosol at an urban background and a road site in Barcelona, Spain

    NASA Astrophysics Data System (ADS)

    Alier, M.; van Drooge, B. L.; Dall'Osto, M.; Querol, X.; Grimalt, J. O.; Tauler, R.

    2013-04-01

    This study investigates the contribution of potential sources to the sub-micron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September-October 2010). 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by Gas Chromatography-Mass Spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by Multivariate Curve Resolution-Alternating Least Squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin, three of secondary OA origin while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (Urban primary organic aerosol, Urban POA) contributed for 43% (1.5 μg OC m-3) and 18% (0.4 μg OC m-3) to OA in RS and UB, respectively. A secondary primary source - biomass burning (BBOA) - was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m-3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation. Three Secondary Organic Aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO), i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols, showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m-3, 16% and 7%, at UB and RS, respectively). By contrast, a SOA biogenic component attributed to α-pinene oxidation (SOA

  13. Source apportionment of submicron organic aerosol at an urban background and a road site in Barcelona (Spain) during SAPUSS

    NASA Astrophysics Data System (ADS)

    Alier, M.; van Drooge, B. L.; Dall'Osto, M.; Querol, X.; Grimalt, J. O.; Tauler, R.

    2013-10-01

    This study investigates the contribution of potential sources to the submicron (PM1) organic aerosol (OA) simultaneously detected at an urban background (UB) and a road site (RS) in Barcelona during the 30 days of the intensive field campaign of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies, September-October 2010). A total of 103 filters at 12 h sampling time resolution were collected at both sites. Thirty-six neutral and polar organic compounds of known emission sources and photo-chemical transformation processes were analyzed by gas chromatography-mass spectrometry (GC-MS). The concentrations of the trace chemical compounds analyzed are herein presented and discussed. Additionally, OA source apportionment was performed by multivariate curve resolution-alternating least squares (MCR-ALS) and six OA components were identified at both sites: two were of primary anthropogenic OA origin and three of secondary OA origin, while a sixth one was not clearly defined. Primary organics from emissions of local anthropogenic activities (urban primary organic aerosol, or POA Urban), mainly traffic emissions but also cigarette smoke, contributed 43% (1.5 μg OC m-3) and 18% (0.4 μg OC m-3) to OA at RS and UB, respectively. A secondary primary source - biomass burning (BBOA) - was found in all the samples (average values 7% RS; 12% UB; 0.3 μg OC m-3), but this component was substantially contributing to OA only when the sampling sites were under influence of regional air mass circulation (REG.). Three secondary organic aerosol (SOA) components (describing overall 60% of the variance) were observed in the urban ambient PM1. Products of isoprene oxidation (SOA ISO) - i.e. 2-methylglyceric acid, C5 alkene triols and 2-methyltetrols - showed the highest abundance at both sites when the city was under influence of inland air masses. The overall concentrations of SOA ISO were similar at both sites (0.4 and 0.3 μg m-3, or 16% and 7%, at UB and RS, respectively

  14. Chemical characterization of fine organic aerosol for source apportionment at Monterrey, Mexico

    NASA Astrophysics Data System (ADS)

    Mancilla, Y.; Mendoza, A.; Fraser, M. P.; Herckes, P.

    2015-07-01

    , source attribution results obtained using the CMB model indicate that emissions from motor vehicle exhausts are the most important, accounting for the 64 % of the PM2.5. The vegetative detritus and biomass burning had the smallest contribution (2.2 % of the PM2.5). To our knowledge, this is the second study to explore the broad chemical characterization of fine organic aerosol in Mexico and the first for the MMA.

  15. Radiocarbon-Based Source apportionment of Elemental Carbon Aerosols at Seoul, South Korea

    NASA Astrophysics Data System (ADS)

    Shakerian Ghahferrokhi, Farid; Ahn, Jinho; Czimczik, Claudia I.; Holden, Sandra; Park, JinSoo

    2016-04-01

    In this study, 10 samples of PM2.5 (aerosol particle with diameter less than 2.5 μm) were collected in the Northeast of Seoul (37.60o N, 127.05o E), South Korea, over 2-4 day periods in May and June of 2015 with a high volume air sampler. The samples were analyzed for their bulk carbon (TC) and nitrogen (N) elemental and stable isotope composition with EA-IRMS. Elemental carbon (EC) was quantified with the Swiss_4S protocol using a Sunset OC/EC analyzer. Both, TC and EC were analyzed for their radiocarbon (14C) content via accelerator mass spectrometry. The mass and isotopic composition of organic carbon (OC) was quantified by (isotope) mass balance. TC loads were 6.6 +/- 1.5 ug C m-3 air (ave. +/- sd; range 4.7-9.7), with a ∆14C ranging from 240 to -446 per mill and a δ13C of -25.4+/-0.3 per mill. EC was a minor fraction of TC (7.2+/-1.9% or 0.5+/-0.2 ug C m-3 air). EC was strongly depleted in 14C (∆14C = -915 to -819 per mill), with fossil sources accounting for 88+/-3% of EC (6.3+/-1.7% of TC). OC was enriched in 14C above natural levels (∆14C = -401 to 309 per mill), and thus could not be partitioned into fossil and modern sources. Local wind directions showed that air masses originated from the South, demonstrating that regional sources may be the crucial contributor to PM pollution in Seoul during that sampling period (early summer).

  16. Source Apportionment of Primary and Secondary Organic Aerosols in Southern California during the 2005 Study of Organic Aerosols in Riverside (SOAR-1)

    NASA Astrophysics Data System (ADS)

    Docherty, K. D.; Jimenez, J. L.; Stone, E. A.; Ulbrich, I. M.; Decarlo, P. F.; Schauer, J. J.; Williams, B.; Goldstein, A. H.; Peltier, R.; Weber, R.

    2009-04-01

    Ambient sampling was conducted in Riverside, California during the 2005 Study of Organic Aerosols in Riverside (SOAR-1) to characterize the composition and sources of organic aerosol using a variety of state-of-the-art instrumentation and source apportionment techniques. The secondary organic aerosol (SOA) mass is estimated by elemental carbon and carbon monoxide tracer methods, water soluble organic carbon content, chemical mass balance of organic molecular markers, and positive matrix factorization of high-resolution aerosol mass spectrometer data. Estimates obtained from each of these methods indicate that the organic fraction in ambient aerosol is overwhelmingly secondary in nature during a period of several weeks with moderate ozone concentrations and that SOA is the single largest component of PM1 aerosol in Riverside. Average SOA/OA contributions of 70-90% were observed during mid-day periods while minimum SOA/OA contributions of 45% were observed during peak morning traffic periods. These results are contrary to previous estimates of SOA throughout the Los Angeles Basin which reported that, other than during severe photochemical smog episodes, SOA was lower than primary OA. Possible reasons for these differences include: (a) for studies that used the EC-tracer method, a large systematic underestimation of SOA can occur when primary OC/EC ratios are derived from ambient measurements during periods "dominated by POA" since there is almost always a large SOA background present (Zhang et al., ACP, 2005); and (b) for model-based studies a large underestimation of SOA is observed for this area, consistent with previous studies (e.g. Volkamer et al., GRL, 2006). The results of the PMF analysis of high-resolution AMS spectra will also be summarized, and tracers from 1-hr data from the thermal-aerosol-GCMS instrument (TAG, Williams et al., JGR 2007) are used to help the interpretation of the AMS components. PMF is applied both to ambient-only and ambient plus

  17. Chemical characterization of fine particulate matter in Changzhou, China, and source apportionment with offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Ye, Zhaolian; Liu, Jiashu; Gu, Aijun; Feng, Feifei; Liu, Yuhai; Bi, Chenglu; Xu, Jianzhong; Li, Ling; Chen, Hui; Chen, Yanfang; Dai, Liang; Zhou, Quanfa; Ge, Xinlei

    2017-02-01

    matter-to-organic carbon (OM / OC) ratios of 0.54, 1.69, 0.11, and 1.99, respectively. Source apportionment of WSOA further identified two secondary OA (SOA) factors (a less oxidized and a more oxidized oxygenated OA) and two primary OA (POA) factors (a nitrogen-enriched hydrocarbon-like traffic OA and a local primary OA likely including species from cooking, coal combustion, etc.). On average, the POA contribution outweighed SOA (55 % vs. 45 %), indicating the important role of local anthropogenic emissions in the aerosol pollution in Changzhou. Our measurement also shows the abundance of organic nitrogen species in WSOA, and the source analyses suggest these species are likely associated with traffic emissions, which warrants more investigations on PM samples from other locations.

  18. Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 1: Fine particle composition and organic source apportionment

    SciTech Connect

    Aiken, A.C.; Wang, J.; Salcedo, D.; Cubison, M. J.; Huffman, J. A.; DeCarlo, P. F.; Ulbrich, I. M.; Docherty, K. S.; Sueper, D.; Kimmel, J. R.; Worsnop, D. R.; Trimborn, A.; Northway, M.; Stone, E. A.; Schauer, J. J.; Volkamer, R. M.; Fortner, E.; de Foy, B.; Laskin, A.; Shutthanandan, V.; Zheng, J.; Zhang, R.; Gaffney, J.; Marley, N. A.; Paredes-Miranda, G.; Arnott, W. P.; Molina, L. T.; Sosa, G.; Jimenez, J. L.

    2009-09-01

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM{sub 2.5} chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM{sub 2.5} emissions by a factor of {approx}4, and it is {approx}16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.

  19. Source apportionment of submicron organic aerosol collected from Atlanta, Georgia, during 2014-2015 using the aerosol chemical speciation monitor (ACSM)

    NASA Astrophysics Data System (ADS)

    Rattanavaraha, Weruka; Canagaratna, Manjula R.; Budisulistiorini, Sri Hapsari; Croteau, Philip L.; Baumann, Karsten; Canonaco, Francesco; Prevot, Andre S. H.; Edgerton, Eric S.; Zhang, Zhenfa; Jayne, John T.; Worsnop, Douglas R.; Gold, Avram; Shaw, Stephanie L.; Surratt, Jason D.

    2017-10-01

    The Aerodyne Aerosol Chemical Speciation Monitor (ACSM) was redeployed at the Jefferson Street (JST) site in downtown Atlanta, Georgia (GA) for 1 year (March 20, 2014-February 08, 2015) to chemically characterize non-refractory submicron particulate matter (NR-PM1) in near real-time and to assess whether organic aerosol (OA) types and amounts change from year-to-year. Submicron organic aerosol (OA) mass spectra were analyzed by season using multilinear engine (ME-2) to apportion OA subtypes to potential sources and chemical processes. A suite of real-time collocated measurements from the Southeastern Aerosol Research and Characterization (SEARCH) network was compared with ME-2 factor solutions to aid in the interpretation of OA subtypes during each season. OA tracers measured from high-volume filter samples using gas chromatography interfaced with electron ionization-mass spectrometry (GC/EI-MS) also aided in identifying OA sources. The initial application of ME-2 to the yearlong ACSM dataset revealed that OA source apportionment by season was required to better resolve sporadic OA types. Spring and fall OA mass spectral datasets were separated into finer periods to capture potential OA sources resulting from non-homogeneous emissions during transitioning periods. NR-PM1 was highest in summer (16.7 ± 8.4 μg m-3) and lowest in winter (8.0 ± 5.7 μg m-3), consistent with prior studies. OA dominated NR-PM1 mass (56-74% on average) in all seasons. Hydrocarbon-like OA (HOA) from primary emissions was observed in all seasons, averaging 5-22% of total OA mass. Strong correlations of HOA with carbon monoxide (CO) (R = 0.71-0.88) and oxides of nitrogen (NOx) (R = 0.55-0.79) indicated that vehicular traffic was the likely source. Biomass burning OA (BBOA) was observed in all seasons, with lower contributions (2%) in summer and higher in colder seasons (averaging 8-20% of total OA mass). BBOA correlated strongly with levoglucosan (R = 0.78-0.95) during colder seasons

  20. Aerosol species concentrations and source apportionment of ammonia at Rocky Mountain National Park.

    PubMed

    Malm, William C; Schichtel, Bret A; Barna, Michael G; Gebhart, Kristi A; Rodriguez, Marco A; Collett, Jeffrey L; Carrico, Christian M; Benedict, Katherine B; Prenni, Anthony J; Kreidenweis, Sonia M

    2013-11-01

    Changes in ecosystem function at Rocky Mountain National Park (RMNP) are occurring because of emissions of nitrogen and sulfate species along the Front Range of the Colorado Rocky Mountains, as well as sources farther east and west. The nitrogen compounds include both oxidized and reduced nitrogen. A year-long monitoring program of various oxidized and reduced nitrogen species was initiated to better understand their origins as well as the complex chemistry occurring during transport from source to receptor. Specifically the goals of the study were to characterize the atmospheric concentrations of nitrogen species in gaseous, particulate, and aqueous phases (precipitation and clouds) along the east and west sides of the Continental Divide; identify the relative contributions to atmospheric nitrogen species in RMNP from within and outside of the state of Colorado; identify the relative contributions to atmospheric nitrogen species in RMNP from emission sources along the Colorado Front Range versus other areas within Colorado; and identify the relative contributions to atmospheric nitrogen species from mobile sources, agricultural activities, and large and small point sources within the state of Colorado. Measured ammonia concentrations are combined with modeled releases of conservative tracers from ammonia source regions around the United States to apportion ammonia to its respective sources, using receptor modeling tools.

  1. Source Apportionment of the Summer Time Carbonaceous Aerosol at Nordic Rural Background Sites

    EPA Science Inventory

    In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter <10µ collected at four Nordic rural backgro...

  2. Source Apportionment of the Summer Time Carbonaceous Aerosol at Nordic Rural Background Sites

    EPA Science Inventory

    In the present study, natural and anthropogenic sources of particulate organic carbon (OCp) and elemental carbon (EC) have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter <10µ collected at four Nordic rural backgro...

  3. Source Apportionment of Primary and Secondary Organic Aerosol Using Positive Matrix Factorization (PMF) of Molecular Markers

    EPA Science Inventory

    Monthly average ambient concentrations of more than eighty particle-phase organic compounds, as well as total organic carbon (OC) and elemental carbon (EC), were measured from March 2004 through February 2005 in five cities in the Midwestern United States. A multi-variant source...

  4. Source apportionment of the carbonaceous aerosol in Norway - quantitative estimates based on 14C, thermal-optical and organic tracer analysis

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Stenström, K.; Puxbaum, H.; Svendby, T.

    2011-09-01

    In the present study, source apportionment of the ambient summer and winter time particulate carbonaceous matter (PCM) in aerosol particles (PM1 and PM10) has been conducted for the Norwegian urban and rural background environment. Statistical treatment of data from thermal-optical, 14C and organic tracer analysis using Latin Hypercube Sampling has allowed for quantitative estimates of seven different sources contributing to the ambient carbonaceous aerosol. These are: elemental carbon from combustion of biomass (ECbb) and fossil fuel (ECff), primary and secondary organic carbon arising from combustion of biomass (OCbb) and fossil fuel (OCff), primary biological aerosol particles (OCPBAP, which includes plant debris, OCpbc, and fungal spores, OCpbs), and secondary organic aerosol from biogenic precursors (OCBSOA). Our results show that emissions from natural sources were particularly abundant in summer, and with a more pronounced influence at the rural compared to the urban background site. 80% of total carbon (TCp, corrected for the positive artefact) in PM10 and ca. 70% of TCpin PM1 could be attributed to natural sources at the rural background site in summer. Natural sources account for about 50% of TCp in PM10 at the urban background site as well. The natural source contribution was always dominated by OCBSOA, regardless of season, site and size fraction. During winter anthropogenic sources totally dominated the carbonaceous aerosol (80-90%). Combustion of biomass contributed slightly more than fossil-fuel sources in winter, whereas emissions from fossil-fuel sources were more abundant in summer. Mass closure calculations show that PCM made significant contributions to the mass concentration of the ambient PM regardless of size fraction, season, and site. A larger fraction of PM1 (ca. 40-60%) was accounted for by carbonaceous matter compared to PM10 (ca. 40-50%), but only by a small margin. In general, there were no pronounced differences in the relative

  5. Source apportionment of the carbonaceous aerosol in Norway - quantitative estimates based on 14C, thermal-optical and organic tracer analysis

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Simpson, D.; Stenström, K.; Puxbaum, H.; Svendby, T.

    2011-03-01

    In the present study, source apportionment of the ambient summer and winter time particulate carbonaceous matter (PCM) in aerosol particles (PM1 and PM10) has been conducted for the Norwegian urban and rural background environment. Statistical treatment of data from thermal-optical, 14C and organic tracer analysis using Latin Hypercube Sampling has allowed for quantitative estimates of seven different sources contributing to the ambient carbonaceous aerosol. These are: elemental carbon from combustion of biomass (ECbb) and fossil fuel (ECff), organic carbon from combustion of biomass (OCbb), fossil fuel (OCff), primary biological aerosol particles (OCPBAP, which includes plant debris, OCpbc, and fungal spores, OCpbs), and secondary organic aerosol from biogenic precursors (OCBSOA). Our results show that emissions from natural sources were particularly abundant in summer, and with a more pronounced influence at the rural compared to the urban background site. 80% of total carbon (TCp, corrected for the positive artefact) in PM10 and 70% of TCp in PM1 could be attributed to natural sources at the rural background site in summer. Natural sources account for about 50% of TCp in PM10 at the urban background site as well. The natural source contribution was always dominated by OCBSOA, regardless of season, site and size fraction. During winter anthropogenic sources totally dominated the carbonaceous aerosol (83-90%). Combustion of biomass contributed slightly more than fossil-fuel sources in winter, whereas emissions from fossil-fuel sources were more abundant in summer. Mass closure calculations show that PCM likely dominated the mass concentration of the ambient PM regardless of size fraction, season, and site. A larger fraction of PM1 (64-69%) was accounted for by carbonaceous matter compared to PM10 (51-67%), but only by a small margin. In general, there were no pronounced differences in the relative contribution of carbonaceous matter to PM with respect to season or

  6. Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers

    NASA Astrophysics Data System (ADS)

    Liu, Junwen; Li, Jun; Liu, Di; Ding, Ping; Shen, Chengde; Mo, Yangzhi; Wang, Xinming; Luo, Chunling; Cheng, Zhineng; Szidat, Sönke; Zhang, Yanlin; Chen, Yingjun; Zhang, Gan

    2016-03-01

    Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities in China, yet few studies simultaneously focus on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

  7. Source apportionment and dynamic changes of carbonaceous aerosols during the haze bloom-decay process in China based on radiocarbon and organic molecular tracers

    NASA Astrophysics Data System (ADS)

    Liu, J.; Li, J.; Liu, D.; Ding, P.; Shen, C.; Mo, Y.; Wang, X.; Luo, C.; Cheng, Z.; Szidat, S.; Zhang, Y.; Chen, Y.; Zhang, G.

    2015-12-01

    Fine carbonaceous aerosols (CAs) is the key factor influencing the currently filthy air in megacities of China, yet seldom study simultaneously focuses on the origins of different CAs species using specific and powerful source tracers. Here, we present a detailed source apportionment for various CAs fractions, including organic carbon (OC), water-soluble OC (WSOC), water-insoluble OC (WIOC), elemental carbon (EC) and secondary OC (SOC) in the largest cities of North (Beijing, BJ) and South China (Guangzhou, GZ), respectively, using the measurements of radiocarbon and anhydrosugars. Results show that non-fossil fuel sources such as biomass burning and biogenic emission make a significant contribution to the total CAs in Chinese megacities: 56 ± 4 % in BJ and 46 ± 5 % in GZ, respectively. The relative contributions of primary fossil carbon from coal and liquid petroleum combustions, primary non-fossil carbon and secondary organic carbon (SOC) to total carbon are 19, 28 and 54 % in BJ, and 40, 15 and 46 % in GZ, respectively. Non-fossil fuel sources account for 52 % in BJ and 71 % in GZ of SOC, respectively. These results suggest that biomass burning has a greater influence on regional particulate air pollution in North China than in South China. We observed an unabridged haze bloom-decay process in South China, which illustrates that both primary and secondary matter from fossil sources played a key role in the blooming phase of the pollution episode, while haze phase is predominantly driven by fossil-derived secondary organic matter and nitrate.

  8. Modelling winter organic aerosol at the European scale with CAMx: evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments

    NASA Astrophysics Data System (ADS)

    Ciarelli, Giancarlo; Aksoyoglu, Sebnem; El Haddad, Imad; Bruns, Emily A.; Crippa, Monica; Poulain, Laurent; Äijälä, Mikko; Carbone, Samara; Freney, Evelyn; O'Dowd, Colin; Baltensperger, Urs; Prévôt, André S. H.

    2017-06-01

    We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from -61 to -29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88 % (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64 % of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40 % to SOA formation (with increasing contributions at urban and near

  9. Radiocarbon-Based Source Apportionment of the Water-Soluble Organic Carbon (wsoc) of Atmospheric Aerosols in South and East Asia

    NASA Astrophysics Data System (ADS)

    Kirillova, E. N.; Sheesley, R. J.; Andersson, A.; Gustafsson, O.; Safai, P. D.; Budhavant, K.; Rao, P. S.; Kang, E.; Han, J.; Lee, M.

    2011-12-01

    The air quality and regional climate in South and East Asia are considerably affected by atmospheric aerosols produced by anthropogenic activities. Recent studies have investigated the sources of the black carbon aerosol component in these regions. This study seeks to make progress in apportioning the sources of the water soluble organic carbon (WSOC) component, which makes up 20-65% of the carbonaceous aerosol mass in these areas. WSOC is important as it enhances the ability of particles to serve as cloud condensation nuclei (CCN) and, therefore, has an impact on regional climate and radiative forcing. Atmospheric particulate matter was collected during fifteen-month continuous sampling campaigns Jan 2008 - March 2009 at both the Maldives Climate Observatory at Hannimaadho (MCOH) and at the Sinhagad hilltop sampling site of the Indian Institute of Tropical Meteorology (SIN) in central-western India. The radiocarbon method is an ideal approach to identify fossil sources (14C "dead") compared to biogenic and biomass combustion products (with a contemporary 14C signal). WSOC is a large fraction of organic aerosols and its annual average contribution to TOC during 2008 is 26% at MCOH and 40% at SIN. There is a distinct seasonal variability in WSOC concentrations at both sites with high concentrations during the winter season (0.92±0.49μg m-3 at MCOH and 3.5±2.0μg m-3 at SIN) and very low concentrations during the summer monsoon season (0.08±0.04μg m-3 at MCOH and 0.27±0.20μg m-3 at SIN). The radiocarbon source apportionment of WSOC in winter dry season was similar at MCOH and SIN with 80-85% from biogenic/biomass combustion and the rest from fossil fuel precursors. For the rest of the year, the biogenic/biomass contribution to WSOC is higher at the Indian Ocean site (86-93%) compared to the Indian site (74-83%). In March 2011 the GoPoEx2011 intensive sampling campaign at the Gosan ABC Superstation, Jeju Island, South Korea was dedicated to study atmospheric

  10. Aerosol Composition and Source Apportionment in the Mexico City Metropolitan Area with PIXE/PESA/STIM and Multivariate Analysis

    SciTech Connect

    Johnson, Kirsten S.; de Foy, B.; Zuberi, Bilal M.; Molina, Luisa; Molina, Mario J.; Xie, YuLong; Laskin, Alexander; Shutthanandan, V.

    2006-10-12

    Aerosols play an important role in the atmosphere but are poorly characterized, particularly in urban areas like the Mexico City Metropolitan Area (MCMA). The chemical composition of urban particles must be known to assess their effects on the environment, and specific particulate emissions sources should be identified to establish ef- 5 fective pollution control standards. For these reasons, samples of particulate matter _2.5 µm (PM2.5) were collected during the MCMA-2003 Field Campaign for elemental and multivariate analyses. Proton-Induced X-ray Emission (PIXE), Proton-Elastic Scattering Analysis (PESA) and Scanning Transmission Ion Microscopy (STIM) techniques were done to determine concentrations of 19 elements from Na to Pb, hydrogen, and 10 total mass, respectively. The most abundant elements from PIXE analysis were S, Si, K, Fe, Ca, and Al, while the major emissions sources associated with these elements were industry, wind-blown soil, and biomass burning. Wind trajectories suggest that metals associated with industrial emissions came from northern areas of the city whereas soil aerosols came from the southwest and increased in concentration during 15 dry conditions. Elemental markers for fuel oil combustion V and Ni correlated with a large SO2 plume to suggest an anthropogenic, rather than volcanic, emissions source. By subtracting major components of soil and sulfates determined by PIXE analysis from STIM total mass measurements, we estimate that approximately 50% of PM2.5 consisted of carbonaceous material.

  11. Argon offline-AMS source apportionment of organic aerosol over yearly cycles for an urban, rural, and marine site in northern Europe

    NASA Astrophysics Data System (ADS)

    Bozzetti, Carlo; Sosedova, Yuliya; Xiao, Mao; Daellenbach, Kaspar R.; Ulevicius, Vidmantas; Dudoitis, Vadimas; Mordas, Genrik; Byčenkienė, Steigvilė; Plauškaitė, Kristina; Vlachou, Athanasia; Golly, Benjamin; Chazeau, Benjamin; Besombes, Jean-Luc; Baltensperger, Urs; Jaffrezo, Jean-Luc; Slowik, Jay G.; El Haddad, Imad; Prévôt, André S. H.

    2017-01-01

    The widespread use of Aerodyne aerosol mass spectrometers (AMS) has greatly improved real-time organic aerosol (OA) monitoring, providing mass spectra that contain sufficient information for source apportionment. However, AMS field deployments remain expensive and demanding, limiting the acquisition of long-term datasets at many sampling sites. The offline application of aerosol mass spectrometry entailing the analysis of nebulized water extracted filter samples (offline-AMS) increases the spatial coverage accessible to AMS measurements, being filters routinely collected at many stations worldwide. PM1 (particulate matter with an aerodynamic diameter < 1 µm) filter samples were collected during an entire year in Lithuania at three different locations representative of three typical environments of the southeast Baltic region: Vilnius (urban background), Rūgšteli\\vskis (rural terrestrial), and Preila (rural coastal). Aqueous filter extracts were nebulized in Ar, yielding the first AMS measurements of water-soluble atmospheric organic aerosol (WSOA) without interference from air fragments. This enables direct measurement of the CO+ fragment contribution, whose intensity is typically assumed to be equal to that of CO2+. Offline-AMS spectra reveal that the water-soluble CO2+ : CO+ ratio not only shows values systematically > 1 but is also dependent on season, with lower values in winter than in summer. AMS WSOA spectra were analyzed using positive matrix factorization (PMF), which yielded four factors. These factors included biomass burning OA (BBOA), local OA (LOA) contributing significantly only in Vilnius, and two oxygenated OA (OOA) factors, summer OOA (S-OOA) and background OOA (B-OOA), distinguished by their seasonal variability. The contribution of traffic exhaust OA (TEOA) was not resolved by PMF due to both low concentrations and low water solubility. Therefore, the TEOA concentration was estimated using a chemical mass balance approach, based on the

  12. Single particle mass spectral signatures from vehicle exhaust particles and the source apportionment of on-line PM2.5 by single particle aerosol mass spectrometry.

    PubMed

    Yang, Jian; Ma, Shexia; Gao, Bo; Li, Xiaoying; Zhang, Yanjun; Cai, Jing; Li, Mei; Yao, Ling'ai; Huang, Bo; Zheng, Mei

    2017-09-01

    In order to accurately apportion the many distinct types of individual particles observed, it is necessary to characterize fingerprints of individual particles emitted directly from known sources. In this study, single particle mass spectral signatures from vehicle exhaust particles in a tunnel were performed. These data were used to evaluate particle signatures in a real-world PM2.5 apportionment study. The dominant chemical type originating from average positive and negative mass spectra for vehicle exhaust particles are EC species. Four distinct particle types describe the majority of particles emitted by vehicle exhaust particles in this tunnel. Each particle class is labeled according to the most significant chemical features in both average positive and negative mass spectral signatures, including ECOC, NaK, Metal and PAHs species. A single particle aerosol mass spectrometry (SPAMS) was also employed during the winter of 2013 in Guangzhou to determine both the size and chemical composition of individual atmospheric particles, with vacuum aerodynamic diameter (dva) in the size range of 0.2-2μm. A total of 487,570 particles were chemically analyzed with positive and negative ion mass spectra and a large set of single particle mass spectra was collected and analyzed in order to identify the speciation. According to the typical tracer ions from different source types and classification by the ART-2a algorithm which uses source fingerprints for apportioning ambient particles, the major sources of single particles were simulated. Coal combustion, vehicle exhaust, and secondary ion were the most abundant particle sources, contributing 28.5%, 17.8%, and 18.2%, respectively. The fraction with vehicle exhaust species particles decreased slightly with particle size in the condensation mode particles. Copyright © 2017 Elsevier B.V. All rights reserved.

  13. Chemical Composition and Source Apportionment of Size ...

    EPA Pesticide Factsheets

    The Cleveland airshed comprises a complex mixture of industrial source emissions that contribute to periods of non-attainment for fine particulate matter (PM 2.5 ) and are associated with increased adverse health outcomes in the exposed population. Specific PM sources responsible for health effects however are not fully understood. Size-fractionated PM (coarse, fine, and ultrafine) samples were collected using a ChemVol sampler at an urban site (G.T. Craig (GTC)) and rural site (Chippewa Lake (CLM)) from July 2009 to June 2010, and then chemically analyzed. The resulting speciated PM data were apportioned by EPA positive matrix factorization to identify emission sources for each size fraction and location. For comparisons with the ChemVol results, PM samples were also collected with sequential dichotomous and passive samplers, and evaluated for source contributions to each sampling site. The ChemVol results showed that annual average concentrations of PM, elemental carbon, and inorganic elements in the coarse fraction at GTC were ~ 2, ~7, and ~3 times higher than those at CLM, respectively, while the smaller size fractions at both sites showed similar annual average concentrat ions. Seasonal variations of secondary aerosols (e.g., high N03- level in winter and high SO42- level in summer) were observed at both sites. Source apportionment results demonstrated that the PM samples at GTC and CLM were enriched with local industrial sources (e.g., steel plant and coa

  14. ORGANIC MOLECULAR MARKER ANALYSIS OF LOW VOLUME RESIDENTIAL SAMPLES FOR SOURCE APPORTIONMENT IN THE DETROIT EXPOSURE AND AEROSOL RESEARCH STUDY

    EPA Science Inventory

    This abstract describes a poster on results for organic speciation analysis for Detroit Exposure and Aerosol Research Study (DEARS) to be presented at the 2006 International Aerosol Conference sponsored by the American Association for Aerosol Research in St. Paul, Minnesota on Se...

  15. Regional air quality in Leipzig, Germany: detailed source apportionment of size-resolved aerosol particles and comparison with the year 2000.

    PubMed

    van Pinxteren, D; Fomba, K W; Spindler, G; Müller, K; Poulain, L; Iinuma, Y; Löschau, G; Hausmann, A; Herrmann, H

    2016-07-18

    A detailed source apportionment of size-resolved aerosol particles in the area of Leipzig, Germany, was performed. Sampling took place at four sites (traffic, traffic/residential, urban background, regional background) in parallel during summer 2013 and the winters 2013/14/15. Twenty-one samples were taken per season with a 5-stage Berner impactor and analysed for particulate mass, inorganic ions, organic and elemental carbon, water-soluble organic carbon, trace metals, and a wide range of organic species. The compositional data were used to estimate source contributions to particulate matter (PM) in quasi-ultrafine (up to 140 nm), accumulation mode, and coarse size ranges using Positive Matrix Factorisation (PMF) receptor modelling. Traffic (exhaust and general traffic emissions), coal combustion, biomass combustion, photochemistry, general secondary formation, cooking, fungal spores, urban dust, fresh sea/road salt, and aged sea salt were all found to contribute to different extents to observed PM concentrations. PMF derived estimates agreed reasonably with estimates from established macrotracer approaches. Quasi-ultrafine PM originated mainly from traffic (20-50%) and photochemistry (30-50%) in summer, while it was dominated by solid fuel (mainly biomass) combustion in winter (50-70%). Tentatively identified cooking aerosol contributed up to 36% on average at the residential site. For accumulation mode particles, two secondary sources typically contributed 40-90% to particle mass. In winter, biomass and coal combustion contributions were up to ca. 25% and 45%, respectively. Main sources of coarse particles were diverse and included nearly all PMF-resolved ones depending on season and air mass origin. For PM10, traffic (typically 20-40% at kerbside sites), secondary formation (30-60%), biomass combustion (10-15% in winter), and coal combustion (30-40% in winter with eastern air mass inflow) were the main quantified sources. At the residential site, contributions

  16. Radiocarbon-based source apportionment of black carbon (BC) in PM 10 aerosols from residential area of suburban Tokyo

    NASA Astrophysics Data System (ADS)

    Uchida, Masao; Kumata, Hidetoshi; Koike, Yasuyo; Tsuzuki, Mikio; Uchida, Tatsuya; Fujiwara, Kitao; Shibata, Yasuyuki

    2010-04-01

    The AMS technique was applied to analyse black carbon (BC), total organic carbon (TOC), and previously reported polycyclic aromatic hydrocarbons (PAHs) in PM 10 aerosols from a residential area, suburban Tokyo, to determine natural abundance of radiocarbon ( 14C), an ideal tracer to distinguish fossil fuel ( 14C-free) from modern biomass combustion sources of pyrolytic products. The 14C concentrations in BC, isolated using the CTO-375 method, were 42% and 30% pMC (in terms of percent Modern Carbon: pMC) in summer and winter, respectively. The 14C concentrations in BC were also compared with those of compound-class specific 14C content of PAHs previously reported for the same samples: they were 45% and 33% pMC in summer and winter, respectively. The 14C signals of BC were identical to those of high molecular weight (MW ⩾ 226, 5-6 rings) PAHs. The resemblance between 14C signals of BC and PAHs can be referred as a 'certificate' for the validity of the BC isolation method employed in this study. Also, it suggests that 14C-BC approach can be a surrogate for PAHs specific 14C analyses to monitor seasonal source variation of combustion-derived pyrolytic products. On the other hand, 14C contents of total organic carbon in 2004 were 61% and 42% pMC in summer and winter, respectively. This is likely attributed to higher contribution of plant activity in summer.

  17. Chemical Characterization and Source Apportionment of Size Fractionated Atmospheric Aerosols, and, Evaluating Student Attitudes and Learning in Large Lecture General Chemistry Classes

    NASA Astrophysics Data System (ADS)

    Allen, Gregory Harold

    Chemical speciation and source apportionment of size fractionated atmospheric aerosols were investigated using laser desorption time-of-flight mass spectrometry (LD TOF-MS) and source apportionment was carried out using carbon-14 accelerator mass spectrometry (14C AMS). Sample collection was carried out using the Davis Rotating-drum Unit for Monitoring impact analyzer in Davis, Colfax, and Yosemite, CA. Ambient atmospheric aerosols collected during the winter of 2010/11 and 2011/12 showed a significant difference in the types of compounds found in the small and large sized particles. The difference was due to the increase number of oxidized carbon species that were found in the small particles size ranges, but not in the large particles size ranges. Overall, the ambient atmospheric aerosols collected during the winter in Davis, CA had and average fraction modern of F14C = 0.753 +/- 0.006, indicating that the majority of the size fractionated particles originated from biogenic sources. Samples collected during the King Fire in Colfax, CA were used to determine the contribution of biomass burning (wildfire) aerosols. Factor analysis was used to reduce the ions found in the LD TOF-MS analysis of the King Fire samples. The final factor analysis generated a total of four factors that explained an overall 83% of the variance in the data set. Two of the factors correlated heavily with increased smoke events during the sample period. The increased smoke events produced a large number of highly oxidized organic aerosols (OOA2) and aromatic compounds that are indicative of biomass burning organic aerosols (WBOA). The signal intensities of the factors generated in the King Fire data were investigated in samples collected in Yosemite and Davis, CA to look at the impact of biomass burning on ambient atmospheric aerosols. In both comparison sample collections the OOA2 and WBOA factors both increased during biomass burning events located near the sampling sites. The correlation

  18. PM2.5 source apportionment with organic markers in the Southeastern Aerosol Research and Characterization (SEARCH) study.

    PubMed

    Watson, John G; Chow, Judith C; Lowenthal, Douglas H; Antony Chen, L-W; Shaw, Stephanie; Edgerton, Eric S; Blanchard, Charles L

    2015-09-01

    acids. The PMF and EV solutions to the CMB equations are complementary to, rather than replacements for, each other, as comparisons of their results reveal uncertainties that are not otherwise evident. Organic markers can be measured on currently acquired PM(2.5) filter samples by thermal methods. These markers can complement element, ion, and carbon fraction measurements from long-term speciation networks. Applying the positive matrix factorization and effective variance solutions for the chemical mass balance equations provides useful information on the accuracy of the source contribution estimates. Nonpolar compounds need to be complemented with polar compounds to better apportion cooking and secondary organic aerosol contributors.

  19. Radiocarbon-based Source Apportionment of Organic, Elemental and Water-soluble Organic Carbon Aerosols and the Light Absorption of Water-soluble Organic Carbon Aerosols in the East Asia High-intensity Winter Campaigns in 2014

    NASA Astrophysics Data System (ADS)

    Fang, W.; Andersson, A.; Zheng, M.; Lee, M.; Kim, S. W.; Du, K.; Gustafsson, O.

    2016-12-01

    Improved understanding of anthropogenic aerosol effects on atmospheric chemistry and climate as well as efficient mitigation actions are hampered by the limited comprehension of the relative contributions of different sources of carbonaceous aerosols and of their subsequent atmospheric processing. Here, we present dual carbon isotope constrained source apportionment and optical properties of carbonaceous aerosols simultaneously both at urban and rural receptor sites, includes North China Plain (NCP, Beijing and Tianjin), Yangtze River Delta (YRD, Shanghai, Zhejiang), and Jeju Island (Korea Climate Observatory at Gosan) during January 2014 field campaigns. The radiocarbon (∆14C) data show that fossil combustions contribute equally ˜80 ± 5% to elemental carbon (EC) aerosol in Beijing, Tianjin, and Shanghai, and 66 ± 9% to Gosan-EC aerosol, while the specific sources of the dominant fossil fuel component were dramatically different among these sites. The mean fraction coal combustion of Beijing-EC, Tianjin-EC, and Gosan-EC is double that of Shanghai-EC. The other large fraction (72―92%) of carbonaceous aerosol is organic carbon (OC) aerosol which contains water soluble and water insoluble organic carbon (WSOC and WISOC). OC, WISOC, and WSOC in Beijing and Gosan sites were still observed largely from fossil sources (53―75%). The more 13C-enriched signature of Gosan-WSOC (-22.8 ± 0.2‰) compared to Gosan-EC (-23.9 ± 0.4‰) and Beijing-WSOC (-23.5 ± 0.7‰) reflects that WSOC is likely more affected by atmospheric aging during long-rang transport than is EC. The high light absorption coefficients of PM2.5, PM1, and TSP were observed at Gosan during this study and was frequently reaching 20―60 Mm-1 by aethalometer and continuous light absorption photometer. The mass absorption cross section of WSOC (MAC365) for above sites is high (1.5 ± 0.8 m2/g), accounted for ˜14 ± 5% of the total direct absorbance relative to EC, which is significantly higher than

  20. Spatial and Temporal Variations of Aerosols Around Beijing in the Summer 2006: Model Evaluation and Source Apportionment

    SciTech Connect

    Matsui, Hitoshi; Koike, Makoto; Kondo, Yutaka; Takegawa, Nobuyuki; Kita, K.; Miyazaki, Y.; Hu, M.; Chang, S-Y; Blake, D. R.; Fast, Jerome D.; Zaveri, Rahul A.; Streets, D. G.; Zhang, Q.; Zhou, T.

    2009-08-15

    Regional aerosol model calculations were made using the WRF-CMAQ and WRF-chem models to study spatial and temporal variations of aerosols around Beijing, China, in August and September 2006 when the CAREBEIJING-2006 campaign was conducted. Model calculations were compared with in-situ observations made at the urban site in Beijing and suburb site in Yufa, which is 50 km to the south of Beijing. In general, the two model calculations reproduced features of temporal variations of meteorological parameters and concentrations of elemental carbon (EC) and inorganic aerosols (sulfate, ammonium, and nitrate). Spatial distributions of aerosol optical depth (AOD) obtained by the MODIS satellite sensor are also generally well reproduced. Model calculations show that enhancements in inorganic aerosol concentrations simultaneously observed at the two sites 4 to 5 times during the one-month observation period were resulted by accumulation of pollutants under stagnated air condition. Because Beijing is located at the north border the high anthropogenic emission area (the Great North China Plain), northward motion of air under the influence of anti-cyclone system caused enhancements in fine aerosol concentrations at Beijing. Concentrations of primary aerosols, such as EC, are found to be generally controlled by emissions within 100 km around Beijing within previous 24 hours. On the other hand, emissions as far as 500 km within previous 3 days were found to affect concentrations of secondary aerosols, such as sulfate. Because of significant contributions of secondary aerosols in Beijing, regional emission controls are found to be necessary for improvement of air quality in Beijing.

  1. Chemical characterization and source apportionment of PM2.5 aerosols in a megacity of Southeast China

    NASA Astrophysics Data System (ADS)

    Li, Huiming; Wang, Qin'geng; Yang, Meng; Li, Fengying; Wang, Jinhua; Sun, Yixuan; Wang, Cheng; Wu, Hongfei; Qian, Xin

    2016-11-01

    PM2.5 aerosol samples were collected during a haze-fog event in winter, as well as in spring, summer, and fall in 2013 within an urban area (Xianlin) and city center area (Gulou) of Nanjing, a megacity of SE China. The PM2.5 showed typical seasonality of waxing in winter and waning in summer or fall with annual average concentrations of 145 and 139 μg/m3 in Xianlin and Gulou, respectively. Concentrations of SO42 -, NO3-, NH4+, Cl-, and K+, EC, OC, secondary organic carbon, and most elements were elevated in winter. The sulfur oxidation ratio and concentrations of SO42 - and Cl- were significantly higher in Xianlin than Gulou (p < 0.05), whereas the nitrogen oxidation ratio and NO3- concentrations were significantly higher in Gulou than Xianlin (p < 0.05). A chemical mass closure construction was used to apportion PM2.5 fractions. Using the positive matrix factorization model, six source factors were identified as having contributed to PM2.5. These were secondary nitrate, road dust, sea salt and ship emissions, coal combustion, secondary sulfate, and the iron and steel industry, which contributed annual averages of 17.8 ± 15.1, 10.6 ± 9.53, 4.50 ± 3.28, 12.4 ± 9.82, 46.3 ± 14.4, and 8.42 ± 5.15%, respectively, to the PM2.5 mass in Xianlin, and 34.5 ± 16.2, 7.82 ± 7.21, 7.27 ± 5.61, 10.5 ± 9.35, 33.0 ± 16.6, and 7.00 ± 6.1%, respectively, in Gulou. Distinct seasonal patterns of the source factors in the two areas associated with the main chemical components were identified, which could be explained by various sources and meteorological conditions. Fig. S2 Temporal trends of sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR) in all four seasons in Xianlin (a) and Gulou (b). Fig. S3 The OC/EC ratios found in four seasons in Xianlin (a) and Gulou (b). Fig. S4 The enrichment factors (EF) obtained in four seasons in Xianlin (a) and Gulou (b). Fig. S5 Estimated versus observed PM2.5 mass concentrations during sampling period in the two areas (95

  2. IMPROVING SOURCE PROFILES AND APPORTIONMENT OF COMBUSTION SOURCES USING THERMAL CARBON FRACTIONS IN MULTIVARIATE RECEPTOR MODELS

    EPA Science Inventory

    The purpose of this study was to improve combustion source profiles and apportionment of a PM2.5 urban aerosol by using 7 individual organic and elemental carbon thermal fractions in place of total organic and elemental carbon. This study used 3 years (96-99) of speciated data...

  3. IMPROVING SOURCE PROFILES AND APPORTIONMENT OF COMBUSTION SOURCES USING THERMAL CARBON FRACTIONS IN MULTIVARIATE RECEPTOR MODELS

    EPA Science Inventory

    The purpose of this study was to improve combustion source profiles and apportionment of a PM2.5 urban aerosol by using 7 individual organic and elemental carbon thermal fractions in place of total organic and elemental carbon. This study used 3 years (96-99) of speciated data...

  4. Source apportionment of airborne particulates through receptor modeling: Indian scenario

    NASA Astrophysics Data System (ADS)

    Banerjee, Tirthankar; Murari, Vishnu; Kumar, Manish; Raju, M. P.

    2015-10-01

    Airborne particulate chemistry mostly governed by associated sources and apportionment of specific sources is extremely essential to delineate explicit control strategies. The present submission initially deals with the publications (1980s-2010s) of Indian origin which report regional heterogeneities of particulate concentrations with reference to associated species. Such meta-analyses clearly indicate the presence of reservoir of both primary and secondary aerosols in different geographical regions. Further, identification of specific signatory molecules for individual source category was also evaluated in terms of their scientific merit and repeatability. Source signatures mostly resemble international profile while, in selected cases lack appropriateness. In India, source apportionment (SA) of airborne particulates was initiated way back in 1985 through factor analysis, however, principal component analysis (PCA) shares a major proportion of applications (34%) followed by enrichment factor (EF, 27%), chemical mass balance (CMB, 15%) and positive matrix factorization (PMF, 9%). Mainstream SA analyses identify earth crust and road dust resuspensions (traced by Al, Ca, Fe, Na and Mg) as a principal source (6-73%) followed by vehicular emissions (traced by Fe, Cu, Pb, Cr, Ni, Mn, Ba and Zn; 5-65%), industrial emissions (traced by Co, Cr, Zn, V, Ni, Mn, Cd; 0-60%), fuel combustion (traced by K, NH4+, SO4-, As, Te, S, Mn; 4-42%), marine aerosols (traced by Na, Mg, K; 0-15%) and biomass/refuse burning (traced by Cd, V, K, Cr, As, TC, Na, K, NH4+, NO3-, OC; 1-42%). In most of the cases, temporal variations of individual source contribution for a specific geographic region exhibit radical heterogeneity possibly due to unscientific orientation of individual tracers for specific source and well exaggerated by methodological weakness, inappropriate sample size, implications of secondary aerosols and inadequate emission inventories. Conclusively, a number of challenging

  5. Accuracy and precision of 14C-based source apportionment of organic and elemental carbon in aerosols using the Swiss_4S protocol

    NASA Astrophysics Data System (ADS)

    Mouteva, G. O.; Fahrni, S. M.; Santos, G. M.; Randerson, J. T.; Zhang, Y.-L.; Szidat, S.; Czimczik, C. I.

    2015-09-01

    Aerosol source apportionment remains a critical challenge for understanding the transport and aging of aerosols, as well as for developing successful air pollution mitigation strategies. The contributions of fossil and non-fossil sources to organic carbon (OC) and elemental carbon (EC) in carbonaceous aerosols can be quantified by measuring the radiocarbon (14C) content of each carbon fraction. However, the use of 14C in studying OC and EC has been limited by technical challenges related to the physical separation of the two fractions and small sample sizes. There is no common procedure for OC/EC 14C analysis, and uncertainty studies have largely focused on the precision of yields. Here, we quantified the uncertainty in 14C measurement of aerosols associated with the isolation and analysis of each carbon fraction with the Swiss_4S thermal-optical analysis (TOA) protocol. We used an OC/EC analyzer (Sunset Laboratory Inc., OR, USA) coupled to a vacuum line to separate the two components. Each fraction was thermally desorbed and converted to carbon dioxide (CO2) in pure oxygen (O2). On average, 91 % of the evolving CO2 was then cryogenically trapped on the vacuum line, reduced to filamentous graphite, and measured for its 14C content via accelerator mass spectrometry (AMS). To test the accuracy of our setup, we quantified the total amount of extraneous carbon introduced during the TOA sample processing and graphitization as the sum of modern and fossil (14C-depleted) carbon introduced during the analysis of fossil reference materials (adipic acid for OC and coal for EC) and contemporary standards (oxalic acid for OC and rice char for EC) as a function of sample size. We further tested our methodology by analyzing five ambient airborne particulate matter (PM2.5) samples with a range of OC and EC concentrations and 14C contents in an interlaboratory comparison. The total modern and fossil carbon blanks of our setup were 0.8 ± 0.4 and 0.67 ± 0.34 μg C, respectively

  6. Accuracy and precision of 14C-based source apportionment of organic and elemental carbon in aerosols using the Swiss_4S protocol

    NASA Astrophysics Data System (ADS)

    Mouteva, G. O.; Fahrni, S. M.; Santos, G. M.; Randerson, J. T.; Zhang, Y. L.; Szidat, S.; Czimczik, C. I.

    2015-04-01

    Aerosol source apportionment remains a critical challenge for understanding the transport and aging of aerosols, as well as for developing successful air pollution mitigation strategies. The contributions of fossil and non-fossil sources to organic carbon (OC) and elemental carbon (EC) in carbonaceous aerosols can be quantified by measuring the radiocarbon (14C) content of each carbon fraction. However, the use of 14C in studying OC and EC has been limited by technical challenges related to the physical separation of the two fractions and small sample sizes. There is no common procedure for OC/EC 14C analysis, and uncertainty studies have largely focused on the precision of yields. Here, we quantified the uncertainty in 14C measurement of aerosols associated with the isolation and analysis of each carbon fraction with the Swiss_4S thermal-optical analysis (TOA) protocol. We used an OC/EC analyzer (Sunset Laboratory Inc., OR, USA) coupled to vacuum line to separate the two components. Each fraction was thermally desorbed and converted to carbon dioxide (CO2) in pure oxygen (O2). On average 91% of the evolving CO2 was then cryogenically trapped on the vacuum line, reduced to filamentous graphite, and measured for its 14C content via accelerator mass spectrometry (AMS). To test the accuracy of our set-up, we quantified the total amount of extraneous carbon introduced during the TOA sample processing and graphitization as the sum of modern and fossil (14C-depleted) carbon introduced during the analysis of fossil reference materials (adipic acid for OC and coal for EC) and contemporary standards (oxalic acid for OC and rice char for EC) as a function of sample size. We further tested our methodology by analyzing five ambient airborne particulate matter (PM2.5) samples with a range of OC and EC concentrations and 14C contents in an interlaboratory comparison. The total modern and fossil carbon blanks of our set-up were 0.8 ± 0.4 and 0.67 ± 0.34 μg C, respectively

  7. Evaluation of the absorption Ångström exponents for traffic and wood burning in the Aethalometer-based source apportionment using radiocarbon measurements of ambient aerosol

    NASA Astrophysics Data System (ADS)

    Zotter, Peter; Herich, Hanna; Gysel, Martin; El-Haddad, Imad; Zhang, Yanlin; Močnik, Griša; Hüglin, Christoph; Baltensperger, Urs; Szidat, Sönke; Prévôt, André S. H.

    2017-03-01

    Equivalent black carbon (EBC) measured by a multi-wavelength Aethalometer can be apportioned to traffic and wood burning. The method is based on the differences in the dependence of aerosol absorption on the wavelength of light used to investigate the sample, parameterized by the source-specific absorption Ångström exponent (α). While the spectral dependence (defined as α values) of the traffic-related EBC light absorption is low, wood smoke particles feature enhanced light absorption in the blue and near ultraviolet. Source apportionment results using this methodology are hence strongly dependent on the α values assumed for both types of emissions: traffic αTR, and wood burning αWB. Most studies use a single αTR and αWB pair in the Aethalometer model, derived from previous work. However, an accurate determination of the source specific α values is currently lacking and in some recent publications the applicability of the Aethalometer model was questioned.Here we present an indirect methodology for the determination of αWB and αTR by comparing the source apportionment of EBC using the Aethalometer model with 14C measurements of the EC fraction on 16 to 40 h filter samples from several locations and campaigns across Switzerland during 2005-2012, mainly in winter. The data obtained at eight stations with different source characteristics also enabled the evaluation of the performance and the uncertainties of the Aethalometer model in different environments. The best combination of αTR and αWB (0.9 and 1.68, respectively) was obtained by fitting the Aethalometer model outputs (calculated with the absorption coefficients at 470 and 950 nm) against the fossil fraction of EC (ECF / EC) derived from 14C measurements. Aethalometer and 14C source apportionment results are well correlated (r = 0.81) and the fitting residuals exhibit only a minor positive bias of 1.6 % and an average precision of 9.3 %. This indicates that the Aethalometer model reproduces

  8. Submicron aerosol analysis and organic source apportionment in an urban atmosphere in Pearl River Delta of China using high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    He, Ling-Yan; Huang, Xiao-Feng; Xue, Lian; Hu, Min; Lin, Yun; Zheng, Jun; Zhang, Renyi; Zhang, Yuan-Hang

    2011-06-01

    The Pearl River Delta (PRD) region in South China is one of the most economically developed regions in China while also noted for its severe air pollution, especially in the urban environments. In order to understand in depth the aerosol chemistry and the emission sources in PRD, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site in the Hong Kong-Shenzhen metropolitan area between 25 October and 2 December 2009. Ten minute-resolved measurement data were analyzed, and an average mass concentration of 44.5 ± 34.0 μg m-3 was calculated for the entire campaign. On average, organic matter was the most abundant PM1 component accounting for 39.7% of the total mass, followed by sulfate (24.5%), black carbon (measured by aethalometer, 14.0%), ammonium (10.2%), nitrate (10.0%), and chloride (1.6%). Moreover, organic matter comprised an increasing fraction of the PM1 loading as the PM1 loading increased, denoting its key role in particulate pollution in this region. Calculations of organic elemental composition based on the high-resolution organic mass spectra obtained indicated that C, H, O, and N on average contributed 33.8%, 55.1%, 10.2%, and 0.9%, respectively, to the total atomic numbers of organic aerosol (OA), which corresponded to an OM/OC ratio (the ratio of organic matter mass/organic carbon mass) of 1.57 ± 0.08. Positive matrix factorization analysis was then conducted on the high-resolution organic mass spectral data set. Four OA components were identified, including a hydrocarbon-like (HOA), a biomass burning (BBOA), and two oxygenated (LV-OOA and SV-OOA) components, which on average accounted for 29.5%, 24.1%, 18.8%, and 27.6%, respectively, of the total organic mass. The HOA was found to have contributions from both fossil fuel combustion and cooking emissions, while the BBOA was well correlated with acetonitrile, a known biomass burning marker. The LV-OOA and SV-OOA corresponded to more aged and

  9. Source apportionment of diesel and spark ignition exhaust aerosol using on-road data from the Minneapolis metropolitan area

    NASA Astrophysics Data System (ADS)

    Johnson, Jason P.; Kittelson, David B.; Watts, Winthrop F.

    Air quality measurements were made on interstate highways in the Minneapolis metropolitan area. Gas and aerosol concentrations were measured on weekdays and weekends. By exploiting the difference in the relative volumes of heavy duty (HD) diesel and light duty (LD) spark ignition (SI) vehicles on weekdays and weekends, we were able to estimate apportioned fuel specific emissions. The on-road, apportioned, fuel specific particle number emissions factors, estimated from condensation particle counter (CPC) measurements were 1.34±0.2×10 16 particles kg -1 for diesels and 7.1±1.6×10 15 particles kg -1 for spark ignition vehicles. Estimates from the scanning mobility particle sizer (SMPS) measurements were 2.1±0.3×10 15 particles kg -1 for diesels and 3.9±0.6×10 14 particles kg -1 for SI vehicles. The difference between CPC and SMPS measurements is mainly due to different lower size detection limits of the instruments, ˜3 and ˜10 nm, respectively. On a weekly weighted basis and on weekdays, the majority of particle number was attributed to HD diesel traffic. Weekend production of particles can be primarily attributed to light duty SI automobiles. On a per vehicle basis, HD vehicles produced substantially greater numbers of particles. On a fuel specific basis, HD vehicles produce slightly higher concentrations of particles than light duty vehicles. The relative contribution of LD vehicles to particle number emissions increased as particle size decreased. The HD apportioned size distributions were similar to size distributions measured during other on-road and laboratory studies. The LD apportioned size distribution was bounded by laboratory and on-road size distributions. Our work is representative of summer, highway cruise conditions. It is likely that under cold start and high load operating conditions LD emissions will increase relative to HD emissions.

  10. The importance of non-fossil sources in carbonaceous aerosols in a megacity of central China during the 2013 winter haze episode: A source apportionment constrained by radiocarbon and organic tracers

    NASA Astrophysics Data System (ADS)

    Liu, Junwen; Li, Jun; Vonwiller, Matthias; Liu, Di; Cheng, Hairong; Shen, Kaijun; Salazar, Gary; Agrios, Konstantinos; Zhang, Yanlin; He, Quanfu; Ding, Xiang; Zhong, Guangcai; Wang, Xinming; Szidat, Sönke; Zhang, Gan

    2016-11-01

    To determine the causes of a severe haze episode in January 2013 in China, a source apportionment of different carbonaceous aerosols (CAs) was conducted in a megacity in central China (Wuhan, Hubei Province) by using the measurements of radiocarbon and molecular organic tracers. Non-fossil sources (e.g., domestic biofuel combustion and biogenic emissions) were found to be responsible for 62% ± 5% and 26% ± 8% of organic carbon (OC) and elemental carbon (EC) components by mass, respectively. Non-fossil sources contributed 57% ± 4% to total CAs in this large-scale haze event, whereas fossil-fuel sources were less dominant (43% ± 4%). The CAs were composed of secondary organic carbon (SOC; 46% ± 10%), primary fossil-fuel carbon (29% ± 4%) and primary biomass-burning carbon (25% ± 10%). Although SOC was formed mainly from non-fossil sources (70% ± 4%), the role of fossil precursors was substantial (30% ± 4%), much higher than at the global scale. Combined measurement of organic tracers and radiocarbon showed that most non-fossil SOC was probably derived from biomass burning during this long-lasting haze episode in central China.

  11. Characterization and source apportionment of aerosol light extinction with a coupled model of CMB-IMPROVE in Hangzhou, Yangtze River Delta of China

    NASA Astrophysics Data System (ADS)

    Wang, Jiao; Zhang, Yu-fen; Feng, Yin-chang; Zheng, Xian-jue; Jiao, Li; Hong, Sheng-mao; Shen, Jian-dong; Zhu, Tan; Ding, Jing; Zhang, Qi

    2016-09-01

    To investigate the characteristics and sources of aerosol light extinction in the Yangtze River Delta of China, a campaign was carried out in Hangzhou from December 2013 to November 2014. Hourly data for air pollutants including PM2.5, SO2, NO2, O3 and CO, and aerosol optical properties including aerosol scattering coefficient and aerosol absorbing coefficient was obtained in the environmental air quality automatic monitoring station. Meteorological parameters were measured synchronously in the automated meteorology monitoring station. Additionally, around seven sets of ambient PM2.5 samples per month were collected and analyzed during the campaign. The annual mean aerosol scattering coefficient, aerosol absorbing coefficient and aerosol single scattering albedo measured in this study was 514 ± 284 Mm- 1, 35 ± 20 Mm- 1 and 94% respectively. The aerosol extinction coefficient reconstructed using the modified IMPROVE (Interagency Monitoring of Protected Visual Environment) formula was compared to the measured extinction coefficient. Better correlations could be found between the measured and reconstructed extinction coefficient when RH was under 90%. A coupled model of CMB (chemical mass balance) and modified IMPROVE was used to apportion the sources of aerosol light extinction in Hangzhou. Vehicle exhaust, secondary nitrate and secondary sulfate were identified as the most significant sources for aerosol light extinction, accounted for 30.2%, 24.1% and 15.8% respectively.

  12. Sensitivity of source apportionment results to mobile source profiles.

    PubMed

    Cai, Tianqi; Schauer, James J; Huang, Wei; Fang, Dongqing; Shang, Jing; Wang, Yuqin; Zhang, Yuanxun

    2016-12-01

    The sensitivity of a source apportionment model to mobile source profiles was examined to determine the impact of using non-local mobile source profiles in chemical mass balance (CMB) models. We examined the impact of USA and Chinese mobile source profiles on source apportionment results in St. Louis, Missouri, and Beijing. The results showed that the use of non-local mobile source profiles did not impact the model apportionment results for vegetative detritus and biomass burning, but other primary source contributions were influenced by the use of non-local source profiles. Secondary organic carbon (SOC) contributions estimated by the CMB models with local and non-local profiles were compared to estimate of SOC from the EC tracer method and were found to be consistent with little bias. The results also showed that it is feasible to use the USA mobile profiles in China while model results were biased by using Chinese mobile profiles in the USA. Monthly and annual average concentrations of molecular markers in the source apportionment model showed lower sensitivity to source profiles than daily measurements, which has implications to the design of source apportionment studies.

  13. Sensitivity of source apportionment results to mobile source profiles

    NASA Astrophysics Data System (ADS)

    Zhang, Y.; Schauer, J. J.; Cai, T.; Zhang, Y.

    2016-12-01

    The sensitivity of a source apportionment model to mobile source profiles was examined to determine the impact of using non-local mobile source profiles in chemical mass balance (CMB) models. We examined the impact of USA and Chinese mobile source profiles on source apportionment results in St. Louis, Missouri, and Beijing. The results showed that the use of non-local mobile source profiles did not impact the model apportionment results for vegetative detritus and biomass burning, but other primary source contributions were influenced by the use of non-local source profiles. Secondary organic carbon (SOC) contributions estimated by the CMB models with local and non-local profiles were compared to estimate of SOC from the EC tracer method and were found to be consistent with little bias. The results also showed that it is feasible to use the USA mobile profiles in China while model results were biased by using Chinese mobile profiles in the USA. Monthly and annual average concentrations of molecular markers in the source apportionment model showed lower sensitivity to source profiles than daily measurements, which has implications to the design of source apportionment studies.

  14. Mexico City Aerosol Analysis during MILAGRO using High Resolution Aerosol Mass Spectrometry at the Urban Supersite (T0). Part 1: Fine Particle Composition and Organic Source Apportionment

    SciTech Connect

    Aiken, Allison; Salcedo, D.; Cubison, Michael J.; Huffman, J.; DeCarlo, Peter; Ulbrich, Ingrid M.; Docherty, Kenneth S.; Sueper, D. T.; Kimmel, Joel; Worsnop, Douglas R.; Trimborn, Achim; Northway, Megan; Stone, Elizabeth A.; Schauer, James J.; Volkamer, Rainer M.; Fortner, Edward; de Foy, B.; Wang, Jian; Laskin, Alexander; Shutthanandan, V.; Zheng, Junsheng; Zhang, Renyi; Gaffney, Jeffrey S.; Marley, Nancy A.; Paredes-Miranda, Guadalupe L.; Arnott, W. P.; Molina, Luisa T.; Sosa, G.; Jimenez, Jose L.

    2009-09-11

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identifies three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning.

  15. SOURCE APPORTIONMENT OF SEATTLE PM 2.5 USING STN ORGANIC CARBON PEAKS

    EPA Science Inventory

    Results from the Source Apportionment of Seattle PM2.5 Using STN Organic Carbon Peaks study will be presented at the American Association for Aerosol Research (AAAR) 24th Annual Conference in Austin, Texas (Oct 17 - 21, 2005). Receptor modeling results from Seattle us...

  16. "OZONE SOURCE APPORTIONMENT IN CMAQ'

    EPA Science Inventory

    Ozone source attribution has been used to support various policy purposes including interstate transport (Cross State Air Pollution Rule) by U.S. EPA and ozone nonattainment area designations by State agencies. Common scientific applications include tracking intercontinental tran...

  17. "OZONE SOURCE APPORTIONMENT IN CMAQ'

    EPA Science Inventory

    Ozone source attribution has been used to support various policy purposes including interstate transport (Cross State Air Pollution Rule) by U.S. EPA and ozone nonattainment area designations by State agencies. Common scientific applications include tracking intercontinental tran...

  18. Radiocarbon and Organic Tracer-based Source Apportionment Study of Carbonaceous Aerosol Collected during Two Ozone Regimes in Houston, TX, USA

    NASA Astrophysics Data System (ADS)

    Yoon, Subin; Usenko, Sascha; Ortiz, Stephanie; Clark, Adelaide; Sheesley, Rebecca

    2017-04-01

    Houston is a prime study site for both primary and secondary carbonaceous organic aerosols due to the city's high anthropogenic activity combined with high potential for biogenic contributions from large forested regions that are proximate to the city. During NASA's DISCOVER-AQ sampling campaign in Houston, TX in September 2013, fine particulate matter (PM2.5) samples were collected and measured for fraction contemporary and fossil carbon utilizing radiocarbon analysis. Contemporary sources can include primary and secondary aerosol from biomass burning, biogenic sources, meat cooking, etc. Fossil sources of carbonaceous aerosol include fossil fuel combustion, non-combustion sources and secondary aerosol from fossil precursors. Fraction contemporary carbon of samples collected from September 8 to 15 ranged from 45-67% with an average of 55% while samples from September 21 to 28 ranged from 47-70% with an average of 61%, both sample sets varying significantly. There were two different air quality regimes during the September campaign: multi-day increases in organic carbon (OC) with low ozone, and multi-day increases in OC with high ozone. To differentiate emission source, meteorology and photochemistry factors in these air quality regimes, HYSPLIT back trajectory, ozone, OC, radiocarbon and organic tracer-based chemical mass balance modeling were used. During the last week of the campaign (September 21-28) high ozone concentration and peak carbonaceous aerosol concentrations were observed throughout the Houston metropolitan area. HYSPLIT back trajectory (BT) analysis also indicates a shift in air mass contributions which corresponded to changes in radiocarbon, ozone and OC concentrations. Daytime OC concentrations for the two different regimes are correlated with ozone daily max at a downtown Houston site (r2 = 0.57). Daytime fossil carbon concentrations have a higher correlation with ozone than contemporary carbon concentrations (r2 = 0.51 and 0.32, respectively

  19. An atmospheric lead source-areas apportionment study in Europe

    NASA Astrophysics Data System (ADS)

    Flament, P.; Deboudt, K.; Bertho, M.-L.; Véron, A.; Puskaric, E.

    2003-05-01

    Atmospheric particulate matter samples, for which the origin of aerosols was unambiguousty determined, has been collected in the Eastern Channel (Northem France). Associated lead concentrations are higher by a factor of about 7, when air masses are runnig from continental Europe, by comparison with marine air masses. We statistically evidence that air masses originating from continental Europe exhibit a more radiogenic composition (1.134<^{206}Pb/^{207}Pb<1.172) than air masses coming from British Islands (1.106<^{206}Pb/^{207}Pb<1.1243. Generally, lead isotopic compositions in aerosols are dearly distinct from the gasoline signatures in European countries, strongly suggesting that automotive lead is no more the major component of this metal in the air. Gasoline and industrial isotopic signatures could explain the origin of lead in our aerosol samples. A source apportionment based upon ^{206}Pb/^{207}Pb ratios suggests that thé difference between British (^{206}Pb/^{207}Pb = 1.122 ± 0.038) and continental (^{206}Pb/^{207}Pb = 1.155 ± 0.022) signatures may be explained by differenees iro the petrol leard content of aerosols (23 to 62% in Great Britain versus 10 to 36% in continental Europe).

  20. Calibration method for a photoacoustic system for real time source apportionment of light absorbing carbonaceous aerosol based on size distribution measurements

    NASA Astrophysics Data System (ADS)

    Utry, Noemi; Ajtai, Tibor; Pinter, Mate; Orvos, Peter I.; Szabo, Gabor; Bozoki, Zoltan

    2016-04-01

    In this study, we introduce a calibration method with which sources of light absorbing carbonaceous particulate matter (LAC) can be apportioned in real time based on multi wavelength optical absorption measurements with a photoacoustic system. The method is primary applicable in wintry urban conditions when LAC is dominated by traffic and biomass burning. The proposed method was successfully tested in a field campaign in the city center of Szeged, Hungary during winter time where the dominance of traffic and wood burning aerosol has been experimentally demonstrated earlier. With the help of the proposed calibration method a relationship between the measured Aerosol Angström Exponent (AAE) and the number size distribution can be deduced. Once the calibration curve is determined, the relative strength of the two pollution sources can be deduced in real time as long as the light absorbing fraction of PM is exclusively related to traffic and wood burning. This assumption is indirectly confirmed in the presented measurement campaign by the fact that the measured size distribution is composed of two unimodal size distributions identified to correspond to traffic and wood burning aerosols. The proposed method offers the possibility of replacing laborious chemical analysis with simple in-situ measurement of aerosol size distribution data.

  1. Source apportionment of atmospheric particles in the UK and Pakistan

    SciTech Connect

    Smith, D.J.T.; Harrison, R.M.; Luhana, L.

    1995-12-31

    Intensive seasonal sampling was undertaken at urban and rural locations throughout Birmingham (UK). Dichotomous Stacked Filter Units (DSFUS) were run simultaneously with hi-vol samplers. DSFU filters were analyzed for nineteen metal species, ammonium and various anions. Hi-vol samplers were modified in order to collect particulate and vapor phase PAHs by means of filter papers and polyurethane foam plugs. Eighteen PAH species were determined by reversed-phase HPLC. Filter portions were forwarded to the University of Aveiro for analysis of elemental and organic carbon. Hi-vol air sampling equipment was run at three sites in Lahore (Pakistan) for over a year. Selected metals, anions and ammonium were quantified, along with eighteen species of particle-associated PAH. Chemical source apportionment of both the Birmingham and Lahore aerosol loads was completed using multivariate analysis. Metals and anionic data were utilized, along with organic concentrations and meteorological data. This technique typically enabled six major air pollution source categories to be identified, along with the quantitative contributions of pollutant species to each source group. The combination of measurements of PAH and inorganic pollutants proved to be a far more powerful tracer of emission sources than PAH data alone. The largest contribution to aerosol mass in the coarse sized fraction in Birmingham was observed to be soil. Whereas in the fine sized fraction major contributors are vehicular/road dust followed by secondary aerosol formation plus oil combustion. Multivariate analysis of the Lahore data revealed similar source categories to those found in Birmingham. The largest contribution to aerosol mass at all three Punjabi sites was soil. This source is followed by metallurgical processes, vehicular emissions and refuse burning.

  2. Radiocarbon based source apportionment of black carbon in the form of PM10 elemental carbon aerosol particles at the Zeppelin Observatory, Svalbard

    NASA Astrophysics Data System (ADS)

    Winiger, Patrik; Andersson, August; Espen Yttri, Karl; Tunved, Peter; Gustafsson, Örjan

    2015-04-01

    Black carbon (BC) aerosol particles are formed from incomplete combustion of fossil fuel and biomass. Transported into the Arctic, they potentially contributes to climate warming. However, there are still large uncertainties related to the climate effects of BC, including aspects of radiative properties, mixing state of the particles, transport, atmospheric lifetime and sources. The current study aims to reduce source uncertainties by applying a top-down (observational) source-diagnostic isotope approach and comparing these to bottom-up (modeling) emission inventories to better constrain the source types and source regions. The use of natural abundance radiocarbon (Δ14C) is a powerful tool to distinguish between fossil (void of 14C) and biomass (contemporary 14C) combustion sources. Due to the well-defined end-members, 14C-measurements (alone) provide high precision (

  3. Source apportionment of 1 h semi-continuous data during the 2005 Study of Organic Aerosols in Riverside (SOAR) using positive matrix factorization

    NASA Astrophysics Data System (ADS)

    Eatough, Delbert J.; Grover, Brett D.; Woolwine, Woods R.; Eatough, Norman L.; Long, Russell; Farber, Robert

    Positive matrix factorization (PMF2) was used to elucidate sources of fine particulate material (PM 2.5) for a study conducted during July and August 2005, in Riverside, CA. One-hour averaged semi-continuous measurements were made with a suite of instruments to provide PM 2.5 mass and chemical composition data. Total PM 2.5 mass concentrations (non-volatile plus semi-volatile) were measured with an R&P filter dynamic measurement system (FDMS TEOM) and a conventional TEOM monitor was used to measure non-volatile mass concentrations. PM 2.5 chemical species monitors included a dual-oven Sunset monitor to measure both non-volatile and semi-volatile carbonaceous material, an ion chromatographic-based monitor to measure sulfate and nitrate and an Anderson Aethalometer to measure black carbon (BC). Gas phase data including CO, NO 2, NO x and O 3 were also collected during the sampling period. In addition, single-particle measurements were made using aerosol time-of-flight mass spectrometry (ATOFMS). Twenty different single-particle types consistent with those observed in previous ATOFMS studies in Riverside were identified for the PMF2 analysis. Finally, time-of-flight aerosol mass spectrometry (ToF-AMS) provided data on markers of primary and secondary organic aerosol. Two distinct PMF2 analyses were performed. In analysis 1, all the data except for the ATOFMS and ToF-AMS data were used in an initial evaluation of sources at Riverside during the study. PMF2 was able to identify six factors from the data set corresponding to both primary and secondary sources, primarily from automobile emissions, diesel emissions, secondary nitrate formation, a secondary photochemical associated source, organic emissions and Basin transported pollutants. In analysis 2, the ATOFMS and ToF-AMS data were included in the analysis. In the second analysis, PMF2 was able to identify 16 factors with a variety of both primary and secondary factors being identified, corresponding to both primary

  4. Two year-long continuous monitoring of PM1 aerosol chemical composition at the Cyprus Atmospheric Observatory. Source apportionment of the Organic content and geographic origins.

    NASA Astrophysics Data System (ADS)

    Stavroulas, Iasonas; Pikridas, Michael; Oikonomou, Kostantina; Vasiliadou, Emily; Savvides, Chrysanthos; Vrekoussis, Mihalis; Mihalopoulos, Nikolaos; Gros, Valerie; Sciare, Jean

    2017-04-01

    Lagrangian dispersion model FLEXPART in backward mode. Analysis of the PMF on the organic mass spectra, based on good agreement with external standard mass spectra, led to the selection of a solution with three factors, an HOA (Hydrocarbon-like Organic Aerosol) factor with relatively low overall contribution (9{%}), a typical Low Volatility (LV-OOA) factor contributing 54{%}, and a factor attributed to Semi-Volatile organics (SV-OOA), contributing 37{%}. The FLEXPART model analysis, led to eight main regions of influence, namely Europe, West Turkey, Anatolia, Middle East, North Africa, Marine, Local and Mixed. Organic content exhibits maximum values when air masses originate from the wider northern sector (West Turkey and Anatolia) and the Middle East. Less aged organic content was identified for air masses originating from the immediate neighboring regions (West Turkey, Anatolia, Middle East and North Africa) while fresh organics peaked when air masses originated from the Middle East, coinciding with elevated BC concentrations, suggesting strong anthropogenic sources for this sector. This project received funding from the ChArMEx (Chemistry Aerosol Mediterranean Experiment) program, the ENVI-MED CyAr project, the European Union's Seventh Framework Programme (FP7) project BACCHUS under grant agreement no. 603445, and the European Union's Horizon 2020 research and innovation programme ACTRIS-2 under grant agreement No 654109.

  5. Source apportionment using reconstructed mass calculations.

    PubMed

    Siddique, Naila; Waheed, Shahida

    2014-01-01

    A long-term study was undertaken to investigate the air quality of the Islamabad/Rawalpindi area. In this regard fine and coarse particulate matter were collected from 4 sites in the Islamabad/Rawalpindi region from 1998 to 2010 using Gent samplers and polycarbonate filters and analyzed for their elemental composition using the techniques of Neutron Activation Analysis (NAA), Proton Induced X-ray Emission/Proton Induced Gamma-ray Emission (PIXE/PIGE) and X-ray Fluorescence (XRF) Spectroscopy. The elemental data along with the gravimetric measurements and black carbon (BC) results obtained by reflectance measurement were used to approximate or reconstruct the particulate mass (RCM) by estimation of pseudo sources such as soil, smoke, sea salt, sulfate and black carbon or soot. This simple analysis shows that if the analytical technique used does not measure important major elements then the data will not be representative of the sample composition and cannot be further utilized for source apportionment studies or to perform transboundary analysis. In this regard PIXE/PIGE and XRF techniques that can provide elemental compositional data for most of the major environmentally important elements appear to be more useful as compared to NAA. Therefore %RCM calculations for such datasets can be used as a quality assurance (QA) measure to treat data prior to application of chemometrical tools such as factor analysis (FA) or cluster analysis (CA).

  6. "OZONE SOURCE APPORTIONMENT IN CMAQ' | Science ...

    EPA Pesticide Factsheets

    Ozone source attribution has been used to support various policy purposes including interstate transport (Cross State Air Pollution Rule) by U.S. EPA and ozone nonattainment area designations by State agencies. Common scientific applications include tracking intercontinental transport of ozone and ozone precursors and delineating anthropogenic and non-anthropogenic contribution to ozone in North America. As in the public release due in September 2013, CMAQ’s Integrated Source Apportionment Method (ISAM) attributes PM EC/OC, sulfate, nitrate, ammonium, ozone and its precursors NOx and VOC, to sectors/regions of users’ interest. Although the peroxide-to-nitric acid productions ratio has been the most common indicator to distinguish NOx-limited ozone production from VOC-limited one, other indicators are implemented in addition to allowing for an ensemble decision based on a total of 9 available indicator ratios. Moreover, an alternative approach of ozone attribution based on the idea of chemical sensitivity in a linearized system that has formed the basis of chemical treatment in forward DDM/backward adjoint tools has been implemented in CMAQ. This method does not require categorization into either ozone regime. In this study, ISAM will simulate the 2010 North America ozone using all of the above gas-phase attribution methods. The results are to be compared with zero-out difference out of those sectors in the host model runs. In addition, ozone contribution wil

  7. Source apportionment of particulate matter in a large city of southeastern Po Valley (Bologna, Italy).

    PubMed

    Tositti, L; Brattich, E; Masiol, M; Baldacci, D; Ceccato, D; Parmeggiani, S; Stracquadanio, M; Zappoli, S

    2014-01-01

    This study reports the results of an experimental research project carried out in Bologna, a midsize town in central Po valley, with the aim at characterizing local aerosol chemistry and tracking the main source emissions of airborne particulate matter. Chemical speciation based upon ions, trace elements, and carbonaceous matter is discussed on the basis of seasonal variation and enrichment factors. For the first time, source apportionment was achieved at this location using two widely used receptor models (principal component analysis/multi-linear regression analysis (PCA/MLRA) and positive matrix factorization (PMF)). Four main aerosol sources were identified by PCA/MLRA and interpreted as: resuspended particulate and a pseudo-marine factor (winter street management), both related to the coarse fraction, plus mixed combustions and secondary aerosol largely associated to traffic and long-lived species typical of the fine fraction. The PMF model resolved six main aerosol sources, interpreted as: mineral dust, road dust, traffic, secondary aerosol, biomass burning and again a pseudo-marine factor. Source apportionment results from both models are in good agreement providing a 30 and a 33% by weight respectively for PCA-MLRA and PMF for the coarse fraction and 70% (PCA-MLRA) and 67% (PMF) for the fine fraction. The episodic influence of Saharan dust transport on PM10 exceedances in Bologna was identified and discussed in term of meteorological framework, composition, and quantitative contribution.

  8. A mass closure and PMF source apportionment study on the sub-micron sized aerosol fraction at urban sites in Italy

    NASA Astrophysics Data System (ADS)

    Vecchi, R.; Chiari, M.; D'Alessandro, A.; Fermo, P.; Lucarelli, F.; Mazzei, F.; Nava, S.; Piazzalunga, A.; Prati, P.; Silvani, F.; Valli, G.

    Sub-micron sized particles are of increasing concern owing to their effects on human health and on the environment. Up to now there are still very few studies on PM1 (i.e. particulate matter with aerodynamic diameter smaller than 1 μm) chemical characterisation; the sub-micron sized fraction is not under regulations although it is of interest because it is almost exclusively associated to anthropogenic sources. To perform the first large-scale assessment of sub-micron sized aerosol concentrations, composition and sources, two monitoring campaigns at three urban sites in Italy were carried out during the wintertime and summertime of 2004. Chemical characterisation (elements, soluble ionic fraction, elemental and organic carbon) was carried out on PM1 samples: major contributions were due to organic matter (about 30% in summer and 50% in winter) and ammonium sulphate (about 10% in winter and 40% in summer). During the cold season, nitrates also contributed up to 30% in Milan (lower contributions were registered at the other two urban sites). Chemical mass closure was achieved with an unaccounted mass in the range 14-22%. Positive Matrix Factorisation (PMF) was applied to identify the major sub-micron sized particles' sources.

  9. Source apportionment in oil spill remediation.

    PubMed

    Muñoz, Jorge; Mudge, Stephen M; Loyola-Sepulveda, Rodrigo; Muñoz, Gonzalo; Bravo-Linares, Claudio

    2012-05-01

    A pipe rupture during unloading led to a spillage of 350-700 tonnes of Caño Limon, a light sweet crude oil, into San Vicente Bay in 2007. Initial clean-up methods removed the majority of the oil from the sandy beaches although some oil remained on the rocky shores. It was necessary for the responsible party to clean the spilled oil even though at this location there were already crude oil hydrocarbons from previous industrial activity. A biosolvent based on vegetable oil derivatives was used to solubilise the remaining oil and a statistical approach to source apportionment was used to determine the efficacy of the cleaning. Sediment and contaminated rock samples were taken prior to cleaning and again at the same locations two days after application of the biosolvent. The oil was extracted using a modified USEPA Method 3550B. The alkanes were quantified together with oil biomarkers on a GC-MS. The contribution that Caño Limon made to the total oil hydrocarbons was calculated from a Partial Least Squares (PLS) analysis using Caño Limon crude oil as the source. By the time the biosolvent was applied, there had already been some attenuation of the oil with all alkanes source of the oil in this case and the contribution that Caño Limon made to the total oil ranged from 0% to 74%. The total hydrocarbon concentrations were lower after cleaning indicating an efficacy of 90% although the reduction in Caño Limon oil was smaller. This was sufficient to make further remediation unnecessary.

  10. Source apportionment of size resolved particulate matter at a European air pollution hot spot.

    PubMed

    Pokorná, P; Hovorka, J; Klán, M; Hopke, P K

    2015-01-01

    Positive Matrix Factorization-PMF was applied to hourly resolved elemental composition of fine (PM0.15-1.15) and coarse (PM1.15-10) aerosol particles to apportion their sources in the airshed of residential district, Ostrava-Radvanice and Bartovice in winter 2012. Multiple-site measurement by PM2.5 monitors complements the source apportionment. As there were no statistical significant differences amongst the monitors, the source apportionment derived for the central site data is expected to apply to whole residential district. The apportioned sources of the fine aerosol particles were coal combustion (58.6%), sinter production-hot phase (22.9%), traffic (15%), raw iron production (3.5%), and desulfurization slag processing (<0.5%) whilst road dust (47.3%), sinter production-cold phase (27.7%), coal combustion (16.8%), and raw iron production (8.2%) were resolved being sources of the coarse aerosol particles. The shape and elemental composition of size-segregated aerosol airborne-sampled by an airship aloft presumed air pollution sources helped to interpret the PMF solution.

  11. The Albuquerque carbon monoxide source apportionment study

    SciTech Connect

    Einfeld, W.

    1988-07-01

    At the request of the New Mexico Environmental Improvement Division, a study was carried out to examine, in detail, the relative contribution of various combustion sources to ambient carbon monoxide in Albuquerque during the winter season evening hours. The two-month field study (January--February 1985) included aerosol and gas monitoring at two sites in the Albuquerque area. Source contributions to ambient carbon monoxide were determined by regression techniques using tracer elements and by carbon isotope measurements on collected carbon monoxide. Results from isotopic carbon analysis of carbon monoxide show that, on average, mobile sources contributed 68 percent and wood burning sources 32 percent to ambient carbon monoxide levels during winter season evening hours. Good agreement was found between results from carbon isotope and linear regression techniques used to estimate average source strengths. The study results point to the significance of both mobile and residential wood burning sources as contributors to ambient carbon monoxide levels. 1 ref., 10 figs., 19 tabs.

  12. Source apportionment of particulate matter in Denmark

    NASA Astrophysics Data System (ADS)

    Moenster, J.; Glasius, M.; Nielsen, O. J.; Bilde, M.; Jensen, F. P.

    2005-12-01

    Atmospheric particulate matter (PM) has received considerable attention over the last decade as an important component of air pollution, particularly due to its health effects on the exposed population. Typically the mass of particles with diameters smaller that 10 μm (PM10) has been used in large cohort studies to estimate health effects such as increase in hospitalization rate, asthma attacks and premature deaths. Particles smaller than 2.5 μm (PM2.5) and ultra fine particles have been used in various epidemiological studies and correlations between exposure to fine and ultra fine particles and health effects have been found. Limits of acceptable concentrations of PM10, PM2.5 and some carcinogenic species have been made, and it is important to find the origin of the particulate matter to prevent exceeds of these limits. This can be done by measuring particle mass, organic/inorganic fractions of particles, the chemical components and other relevant factors, and then use receptor modeling for source apportionment of the particulate matter. We have done measurements at street level and urban background in Copenhagen, Denmark, to determine the origin of different sizes of particulate matter and the toxic organic compounds connected to these particles. We also did measurements in a small village with less traffic and more residential wood combustion for a comparison between traffic and wood combustion generated pollution. Our results show a significant amount of particulate matter coming from non local sources and are dominated by long-range transported inorganic salts. The amount of these is highly depended on the wind direction and thus on the origin of the wind plume. The origin of the carcinogenic organic compound benzo(a)pyrene was found to be local combustion sources. To prevent events of high particulate matter concentration in Copenhagen, Denmark, a reduction of emission from the local traffic will only lead to a minor effect, since the majority of the

  13. First measurements of reactive α-dicarbonyl concentrations on PM2.5 aerosol over the Boreal forest in Finland during HUMPPA-COPEC 2010 - source apportionment and links to aerosol aging

    NASA Astrophysics Data System (ADS)

    Kampf, C. J.; Corrigan, A. L.; Johnson, A. M.; Song, W.; Keronen, P.; Königstedt, R.; Williams, J.; Russell, L. M.; Petäjä, T.; Fischer, H.; Hoffmann, T.

    2012-07-01

    The first dataset for summertime boreal forest concentrations of two atmospherically relevant α-dicarbonyl compounds, glyoxal (Gly) and methylglyoxal (Mgly) on PM2.5 aerosol was obtained during the HUMPPA-COPEC-2010 field measurement intensive in Hyytiälä, Finland. Anthropogenic influences over the course of the campaign were identified using trace gas signatures and aerosol particle chemical composition analysis. The data evaluation allowed the identification of different events such as urban pollution plumes, biomass burning and sawmill emissions as sources of high Gly and Mgly concentrations. Mean aerosol concentrations during periods of biogenic influence were 0.81 ng m-3 for Gly and 0.31 ng m-3 for Mgly. Mgly was generally less abundant in PM2.5, probably due to its shorter photolysis lifetime and less effective partitioning into the particle phase due to its smaller effective Henry's Law constant compared to Gly. This is in contrast with previous urban studies which show significantly more Mgly than Gly. Peak concentrations for Gly coincided with nearby sources, e.g. high VOC emissions from nearby sawmills, urban pollution plumes from the city of Tampere located 50 km southwest of the sampling site and biomass burning emissions from wildfires. Calculated ratios of Gly in PM2.5 and total organic matter in PM1 aerosols indicate higher values in less aged aerosols. Irreversible processing of Gly in the particle phase, e.g. via oxidation by OH radicals, organo sulfate or imidazole formation are processes currently discussed in the literature which could likely explain these findings.

  14. First measurements of reactive α-dicarbonyl concentrations on PM2.5 aerosol over the boreal forest in Finland during HUMPPA-COPEC 2010 - source apportionment and links to aerosol aging

    NASA Astrophysics Data System (ADS)

    Kampf, C. J.; Corrigan, A. L.; Johnson, A. M.; Song, W.; Keronen, P.; Königstedt, R.; Williams, J.; Russell, L. M.; Petäjä, T.; Fischer, H.; Hoffmann, T.

    2012-01-01

    The first dataset for summertime boreal forest concentrations of two atmospherically relevant α-dicarbonyl compounds, glyoxal (Gly) and methylglyoxal (Mgly) on PM2.5 aerosol was obtained during the HUMPPA-COPEC-2010 field measurement intensive in Hyytiälä, Finland. Identification of anthropogenic influences over the course of the campaign, using trace gas signatures and aerosol particle chemical composition analysis, allowed the identification of different events such as urban pollution plumes, biomass burning and sawmill emissions as sources of high Gly and Mgly concentrations. Mean aerosol concentrations during periods of biogenic influence were 0.81 ng m-3 for Gly and 0.31 ng m-3 for Mgly. Mgly was generally less abundant in PM2.5, probably due to its shorter photolysis lifetime and less effective partitioning into the particle phase due to its smaller effective Henry's Law constant compared to Gly. This is in contrast with previous urban studies which show significantly more Mgly than Gly. Peak concentrations for Gly coincided with nearby sources, e.g. high VOC emissions from nearby sawmills, urban pollution plumes from the city of Tampere located 50 km southwest of the sampling site and biomass burning emissions from wildfires. Calculated ratios of Gly in PM2.5 and total organic matter in PM1 aerosols indicate higher values in less aged aerosols. Irreversible processing of Gly in the particle phase, e.g. via oxidation by OH radicals, organo sulfate or imidazole formation are processes currently discussed in the literature which could likely explain these findings.

  15. Rocky Mountain National Park reduced nitrogen source apportionment

    NASA Astrophysics Data System (ADS)

    Thompson, Tammy M.; Rodriguez, Marco A.; Barna, Michael G.; Gebhart, Kristi A.; Hand, Jennifer L.; Day, Derek E.; Malm, William C.; Benedict, Katherine B.; Collett, Jeffrey L., Jr.; Schichtel, Bret A.

    2015-05-01

    Excess wet and dry deposition of nitrogen-containing compounds are a concern at a number of national parks. The Rocky Mountain Atmospheric Nitrogen and Sulfur Study Part II (RoMANS II) campaign was conducted from November 2008 to November 2009 to characterize the composition of reactive nitrogen and sulfur deposited in Rocky Mountain National Park (RMNP). RoMANS II identified reduced nitrogen as the major contributor to reactive nitrogen deposition in RMNP, making up over 50% of the total. Motivated by this finding, the particulate source apportionment technology within the Comprehensive Air Quality Model with extensions was used here to estimate source apportionment of reduced nitrogen concentrations at RMNP. Source apportionment results suggest that approximately 40% of reduced nitrogen deposition to RMNP comes from ammonia sources within Colorado. However, the model evaluation also suggests that this number could be underrepresenting ammonia sources in eastern Colorado due to the difficulty of capturing upslope airflow on the eastern side of the Continental Divide with meteorological models. Emissions from California, the western model boundary, and the Snake River Valley in Idaho, the next three most influential sources, contribute approximately 15%, 8%, and 7%, respectively, to total reduced nitrogen measured in RMNP. Within Colorado, about 61%, 26%, and 13% of the total Colorado contribution comes from sources to the east of the Continental Divide, sources to the west of the Continental Divide, and from the park itself.

  16. Sensitivity of fine sediment source apportionment to mixing model assumptions

    NASA Astrophysics Data System (ADS)

    Cooper, Richard; Krueger, Tobias; Hiscock, Kevin; Rawlins, Barry

    2015-04-01

    Mixing models have become increasingly common tools for quantifying fine sediment redistribution in river catchments. The associated uncertainties may be modelled coherently and flexibly within a Bayesian statistical framework (Cooper et al., 2015). However, there is more than one way to represent these uncertainties because the modeller has considerable leeway in making error assumptions and model structural choices. In this presentation, we demonstrate how different mixing model setups can impact upon fine sediment source apportionment estimates via a one-factor-at-a-time (OFAT) sensitivity analysis. We formulate 13 versions of a mixing model, each with different error assumptions and model structural choices, and apply them to sediment geochemistry data from the River Blackwater, Norfolk, UK, to apportion suspended particulate matter (SPM) contributions from three sources (arable topsoils, road verges and subsurface material) under base flow conditions between August 2012 and August 2013 (Cooper et al., 2014). Whilst all 13 models estimate subsurface sources to be the largest contributor of SPM (median ~76%), comparison of apportionment estimates reveals varying degrees of sensitivity to changing prior parameter distributions, inclusion of covariance terms, incorporation of time-variant distributions and methods of proportion characterisation. We also demonstrate differences in apportionment results between a full and an empirical Bayesian setup and between a Bayesian and a popular Least Squares optimisation approach. Our OFAT sensitivity analysis reveals that mixing model structural choices and error assumptions can significantly impact upon fine sediment source apportionment results, with estimated median contributions in this study varying by up to 21% between model versions. Users of mixing models are therefore strongly advised to carefully consider and justify their choice of model setup prior to conducting fine sediment source apportionment investigations

  17. High altitude (˜4520 m amsl) measurements of black carbon aerosols over western trans-Himalayas: Seasonal heterogeneity and source apportionment

    NASA Astrophysics Data System (ADS)

    Babu, S. Suresh; Chaubey, Jai Prakash; Krishna Moorthy, K.; Gogoi, Mukunda M.; Kompalli, Sobhan Kumar; Sreekanth, V.; Bagare, S. P.; Bhatt, Bhuvan C.; Gaur, Vinod K.; Prabhu, Tushar P.; Singh, N. S.

    2011-12-01

    The first ever, year-round measurements of aerosol black carbon (BC) over the western part of trans- Himalayas are reported from Hanle (˜4520 m above mean sea level). The daily mean BC concentrations varied from as low as 7 ng m-3 to as high as 296 ng m-3 with an annual average of 77 ± 64 ng m-3, indicating significant BC burden even at free- tropospheric altitudes. Variation with in the day as well as from day to day were highly subdued during winter season (December to February) while they used to be the highest in Spring (March to May). In general, the less frequently occurring high BC values contributed more to the annual and seasonal means, while 64% of the values were below the annual mean. Seasonally, highest BC concentration (109 ± 78 ng m-3) occurred during Spring and lowest (66 ± 42/66 ± 62 ng m3) during Summer/Winter season(June to August/December to February). Diurnal variations in general were very weak, except during Spring and Summer when the effects of convective boundary layer dynamics is discernible. Back trajectory clustering and concentration weighted trajectory (CWT) analyses indicated that, most time of the year the sampling location is influenced by the advection from West and Southwest Asia, while the contribution from the Indo-Gangetic Plains (IGP) remained very low during Spring and Summer. The seasonal and annual mean BC at Hanle are significantly lower than the corresponding values reported for other Himalayan stations, while they were quite higher than those reported from the South Pole and pristine Antarctic environments.

  18. Sources of optically active aerosol particles over the Amazon forest

    NASA Astrophysics Data System (ADS)

    Guyon, Pascal; Graham, Bim; Roberts, Gregory C.; Mayol-Bracero, Olga L.; Maenhaut, Willy; Artaxo, Paulo; Andreae, Meinrat O.

    Size-fractionated ambient aerosol samples were collected at a pasture site and a primary rainforest site in the Brazilian Amazon Basin during two field campaigns (April-May and September-October 1999), as part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis (PIXE), for equivalent black carbon (BC e) by a light reflectance technique and for mass concentration by gravimetric analysis. Additionally, we made continuous measurements of absorption and light scattering by aerosol particles. The vertical chemical composition gradients at the forest site have been discussed in a companion article (Journal of Geophysical Research-Atmospheres 108 (D18), 4591 (doi:4510.1029/2003JD003465)). In this article, we present the results of a source identification and quantitative apportionment study of the wet and dry season aerosols, including an apportionment of the measured scattering and absorption properties of the total aerosol in terms of the identified aerosol sources. Source apportionments (obtained from absolute principal component analysis) revealed that the wet and dry season aerosols contained the same three main components, but in different (absolute and relative) amounts: the wet season aerosol consisted mainly of a natural biogenic component, whereas pyrogenic aerosols dominated the dry season aerosol mass. The third component identified was soil dust, which was often internally mixed with the biomass-burning aerosol. All three components contributed significantly to light extinction during both seasons. At the pasture site, up to 47% of the light absorption was attributed to biogenic particles during the wet season, and up to 35% at the tower site during the wet-to-dry transition period. The results from the present study suggest that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be

  19. Source Contributions to Wintertime Elemental and Organic Carbon in the Western Arctic Based on Radiocarbon and Tracer Apportionment.

    PubMed

    Barrett, T E; Robinson, E M; Usenko, S; Sheesley, R J

    2015-10-06

    To quantify the contributions of fossil and biomass sources to the wintertime Arctic aerosol burden source apportionment is reported for elemental (EC) and organic carbon (OC) fractions of six PM10 samples collected during a wintertime (2012-2013) campaign in Barrow, AK. Radiocarbon apportionment of EC indicates that fossil sources contribute an average of 68 ± 9% (0.01-0.07 μg m(-3)) in midwinter decreasing to 49 ± 6% (0.02 μg m(-3)) in late winter. The mean contribution of fossil sources to OC for the campaign was stable at 38 ± 8% (0.04-0.32 μg m(-3)). Samples were also analyzed for organic tracers, including levoglucosan, for use in a chemical mass balance (CMB) source apportionment model. The CMB model was able to apportion 24-53% and 99% of the OC and EC burdens, respectively, during the campaign, with fossil OC contributions ranging from 25 to 74% (0.02-0.09 μg m(-3)) and fossil EC contributions ranging from 73 to 94% (0.03-0.07 μg m(-3)). Back trajectories identified two major wintertime source regions to Barrow: the Russian and North American Arctic. Atmospheric lifetimes of levoglucosan, ranging from 50 to 320 h, revealed variability in wintertime atmospheric processing of this biomass burning tracer. This study allows for unambiguous apportionment of EC to fossil fuel and biomass combustion sources and intercomparison with CMB modeling.

  20. Radiocarbon-derived source apportionment of fine carbonaceous aerosols before, during, and after the 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing, China

    NASA Astrophysics Data System (ADS)

    Liu, Junwen; Mo, Yangzhi; Li, Jun; Liu, Di; Shen, Chengde; Ding, Ping; Jiang, Haoyu; Cheng, Zhineng; Zhang, Xiangyun; Tian, Chongguo; Chen, Yingjun; Zhang, Gan

    2016-04-01

    The Asia-Pacific Economic Cooperation (APEC) summit took place in Beijing, China, 5-11 November 2014, during which numerous measures were performed to control the air pollution, and consequently, the sky of Beijing was so clean that the public called it "APEC blue." The concentrations before, during, and after the APEC summit are 14.4 ± 6.81 µg C/m3, 6.66 ± 2.99 µg C/m3, and 32.3 ± 10.6 µg C/m3, respectively, for organic carbon (OC), and 2.27 ± 1.17 µg C/m3, 0.76 ± 0.52 µg C/m3, and 4.99 ± 1.74 µg C/m3, respectively, for elemental carbon (EC). We quantify the contributions of fossil and nonfossil sources to the OC and EC using radiocarbon. Results show that the contribution of nonfossil sources is 56 ± 1% (before APEC), 61 ± 1% (during APEC), and 48 ± 1% (after APEC), respectively, for OC, and 36 ± 4% (before APEC), 46 ± 1% (during APEC), and 33 ± 4% (after APEC), respectively, for EC. Comparing to the period before APEC, 70% and 60% of fossil EC and OC and 60% and 50% of nonfossil EC and OC are reduced, respectively, implying that the control on the nonfossil sources has considerable contribution to the good air quality in Beijing. Both EC and OC mass loadings during the APEC summit would have increased by 60% if the biomass-burning activities were not taken into account for control. In such a case, the atmospheric visibility would decrease 20% at least and the blue sky thereby would likely not have been visible during the summit.

  1. Enterococcus and Escherichia coli fecal source apportionment with microbial source tracking genetic markers - is it feasible?

    EPA Science Inventory

    Fecal pollution is measured in surface waters using culture-based measurements of enterococci and Escherichia coli bacteria. Source apportionment of these two fecal indicator bacteria is an urgent need for prioritizing remediation efforts and quantifying health risks associated...

  2. Enterococcus and Escherichia coli fecal source apportionment with microbial source tracking genetic markers - is it feasible?

    EPA Science Inventory

    Fecal pollution is measured in surface waters using culture-based measurements of enterococci and Escherichia coli bacteria. Source apportionment of these two fecal indicator bacteria is an urgent need for prioritizing remediation efforts and quantifying health risks associated...

  3. The use of levoglucosan and radiocarbon for source apportionment of PM(2.5) carbonaceous aerosols at a background site in East China.

    PubMed

    Liu, Di; Li, Jun; Zhang, Yanlin; Xu, Yue; Liu, Xiang; Ding, Ping; Shen, Chengde; Chen, Yingjun; Tian, Chongguo; Zhang, Gan

    2013-09-17

    Samples of fine particulate matter (PM2.5) were collected during July 2009 to March 2010 at a regional background site in East China. The mass concentrations of organic carbon (OC) and elemental carbon (EC) were characterized by the highest levels in winter (December to February) and the lowest abundances in summer (June to August). Conversely, the concentrations of levoglucosan were higher in summer than in winter. The observations were associated to the anthropogenic air pollutions (predominantly fossil-fuel combustions) transport from the center and north China with the northwest winds in winter and large contribution of the open biomass burning activities in South China and East China in summer, which was evident by air-mass trajectories and MODIS satellite fire counts. To assign fossil and nonfossil contributions of carbonaceous matters, the radiocarbon contents in water-insoluble OC (WINSOC) and EC in 4 combined samples representing four seasons were analyzed using the isolation system established in China. The results indicated that biomass burning and biogenic sources (59%) were the major contribution to the WINSOC, whereas fossil fuel (78%) was the dominant contributor to the refractory EC at this site. The source variation obtained by radiocarbon was consistent with other indicators, such as the OC/EC ratios and the levoglucosan concentration. Biomass burning and biogenic emissions were found to predominate in the summer and autumn, whereas fossil fuel emissions predominate in winter and spring.

  4. Source apportionment and the role of meteorological conditions in the assessment of air pollution exposure due to urban emissions

    NASA Astrophysics Data System (ADS)

    Schäfer, K.; Elsasser, M.; Arteaga-Salas, J. M.; Gu, J.; Pitz, M.; Schnelle-Kreis, J.; Cyrys, J.; Emeis, S.; Prevot, A. S. H.; Zimmermann, R.

    2014-01-01

    As particulate matter (PM) impacts human health, knowledge about its composition, exposure and source apportionment is required. A study of the urban atmosphere in the case of Augsburg, Germany, during winter (31 January-12 March 2010) is thus presented here. Investigations were performed on the basis of aerosol mass spectrometry and further air pollutants and meteorological measurements, including mixing layer height. Organic matter was separated by source apportionment of PM1 with positive matrix factorization (PMF) in three factors: OOA - oxygenated organic aerosol (secondary organic factor), HOA - hydrocarbon-like organic aerosol (traffic factor or primary organic factor) and WCOA - wood combustion organic aerosol (wood combustion factor), which extend the information from black carbon (BC) measurements. PMF was also applied to the particle size distribution (PSD) data of PM2.5 to determine different source profiles and we assigned them to the particle sources: nucleation aerosol, fresh traffic aerosol, aged traffic aerosol, stationary combustion aerosol and secondary aerosol. Ten different temporal phases were identified on the basis of weather characteristics and aerosol composition and used for correlations of all air pollutants and meteorological parameters. While source apportionment from both organic PM composition and PSD agree and show that the main emission sources of PM exposure are road traffic as well as stationary and wood combustion, secondary aerosol factor concentrations are very often the highest ones. The hierarchical clustering analysis with the Ward method of cross-correlations of each air pollutant and PM component and of the correlations of each pollutant with all meteorological parameters provided two clusters: "secondary pollutants of PM1 and fine particles" and "primary pollutants (including CO and benzene) and accumulation mode particles". The dominant meteorological influences on pollutant concentrations are wind speed and mixing

  5. Indoor source apportionment in urban communities near industrial sites

    NASA Astrophysics Data System (ADS)

    Tunno, Brett J.; Dalton, Rebecca; Cambal, Leah; Holguin, Fernando; Lioy, Paul; Clougherty, Jane E.

    2016-08-01

    Because fine particulate matter (PM2.5) differs in chemical composition, source apportionment is frequently used for identification of relative contributions of multiple sources to outdoor concentrations. Indoor air pollution and source apportionment is often overlooked, though people in northern climates may spend up to 90% of their time inside. We selected 21 homes for a 1-week indoor sampling session during summer (July to September 2011), repeated in winter (January to March 2012). Elemental analysis was performed using inductively-coupled plasma mass spectrometry (ICP-MS), and factor analysis was used to determine constituent grouping. Multivariate modeling was run on factor scores to corroborate interpretations of source factors based on a literature review. For each season, a 5-factor solution explained 86-88% of variability in constituent concentrations. Indoor sources (i.e. cooking, smoking) explained greater variability than did outdoor sources in these industrial communities. A smoking factor was identified in each season, predicted by number of cigarettes smoked. Cooking factors were also identified in each season, explained by frequency of stove cooking and stovetop frying. Significant contributions from outdoor sources including coal and motor vehicles were also identified. Higher coal and secondary-related elemental concentrations were detected during summer than winter. Our findings suggest that source contributions to indoor concentrations can be identified and should be examined in relation to health effects.

  6. Source-apportionment and model evaluation: experiences with the EMEP SOA model

    NASA Astrophysics Data System (ADS)

    Simpson, D.; Yttri, K. E.

    2009-04-01

    The EMEP MSC-W chemical transport model (Simpson et al., 2003) has been successfully used for the prediction of photochemical oxidants and various inorganic aerosol components (sulphate, nitrate, ammonium) for many years. The model generally performs well for such species, as should be expected for compounds whose emission sources and chemistry are fairly well know. For carbonaceous particulate matter (PCM) however the model has been found to give very different results in different parts of Europe, with typically poor performance in southern Europe, but rather good results in Northern Europe (Simpson et al., 2007). Earlier comparison with the results of source-apportionment studies from the CARBOSOL project (Gelencser et al., 2007, Simpson et al., 2007) has shown that the poor performance in southern Europe can partly be ascribed to difficulties with emissions from residential wood-burning, and partly due to an underestimate of the secondary organic aerosol (SOA) component. Such difficulties are expected for organic aerosols, a subject where the basic science is only partially understood, and where new experimental results continually lead to revisions in existing ideas concerning sources and formation mechanisms (e.g. Hallquist et al., 2009). In such a situation, it is essential that model results are evaluated as thoroughly as possible, and that where possible the various components of organic aerosol can be evaluated separately. A number of source-apportionment (SA) studies have recently become available in Europe, in which data on elemental carbon (EC), organic carbon (OC), 14C, levoglucosan, and various markers of primary organic carbon (cellulose, sugars/sugar-alcohols) have allowed estimates of various sources of carbonaceous particulate matter (PCM). As well as CARBOSOL, these studies include various sites in Switzerland (e.g. Lanz et al., 2008, Szidat et al., 2006), data are available from Gothenburg in Sweden (Szidat et al., 2008) and from southern

  7. Source apportionment of PM10 in the Western Mediterranean based on observations from a cruise ship

    NASA Astrophysics Data System (ADS)

    Schembari, C.; Bove, M. C.; Cuccia, E.; Cavalli, F.; Hjorth, J.; Massabò, D.; Nava, S.; Udisti, R.; Prati, P.

    2014-12-01

    Two intensive PM10 sampling campaigns were performed in the summers of 2009 and 2010 on the ship Costa Pacifica during cruises in the Western Mediterranean. Samples, mainly collected on an hourly basis, were analysed with different techniques (Particle Induced X-Ray Emission, PIXE; Energy Dispersive - X Ray Fluorescence, ED-XRF; Ion Chromatography, IC; Thermo-optical analysis) to retrieve the PM10 composition and its time pattern. The data were used for obtaining information about the sources of aerosol, with a focus on ship emissions, through apportionment using chemical marker compounds, correlation analysis and Positive Matrix Factorization (PMF) receptor modelling. For the campaign in 2010, 66% of the aerosol sulphate was found to be anthropogenic, only minor contributions of dust and sea salt sulphate were observed while the biogenic contribution, estimated based on the measurements of MSA, was found to be more important (26%), but influenced by large uncertainties. V and Ni were found to be suitable tracers of ship emissions during the campaigns. Four sources of aerosol were resolved by the PMF analysis; the source having the largest impact on PM10, BC and sulphate was identified as a mixed source, comprising emissions from ships. The correlations between sulphate and V and Ni showed the influence of ship emissions on sulphate in marine air masses. For the leg Palma-Tunis crossing a main ship route, the correlations between aerosol sulphate and V and Ni were particularly strong (r2 = 0.9 for both elements).

  8. An integrated PM2.5 source apportionment study: Positive Matrix Factorisation vs. the chemical transport model CAMx

    NASA Astrophysics Data System (ADS)

    Bove, M. C.; Brotto, P.; Cassola, F.; Cuccia, E.; Massabò, D.; Mazzino, A.; Piazzalunga, A.; Prati, P.

    2014-09-01

    Receptor and Chemical Transport Models are commonly used tools in source apportionment studies, even if different expertise is required. We describe an experiment using both approaches to apportion the PM2.5 (i.e., particulate matter with aerodynamic diameters below 2.5 μm) sources in the city of Genoa (Italy). A sampling campaign was carried out to collect PM2.5 samples daily for approximately six month during 2011 in three sites. The subsequent compositional analyses included the speciation of elements, major ions and both organic and elemental carbon; these data produced a large database for receptor modelling through Positive Matrix Factorisation (PMF). In the same period, a meteorological and air quality modelling system was implemented based on the mesoscale numerical weather prediction model WRF and the chemical transport model CAMx to obtain meteorological and pollutant concentrations up to a resolution of 1.1 km. The source apportionment was evaluated by CAMx over the same period that was used for the monitoring campaign using the Particulate Source Apportionment Technology tool. Even if the source categorisations were changed (i.e., groups of time-correlated compounds in PMF vs. activity categories in CAMx), the PM2.5 source apportionment by PMF and CAMx produced comparable results. The different information provided by the two approaches (e.g., real-world factor profile by PMF and apportionment of a secondary aerosol by CAMx) was used jointly to elucidate the composition and origin of PM2.5 and to develop a more general methodology. When studying the primary and secondary components of PM, the main anthropogenic sources in the area were road transportation, energy production/industry and maritime emissions, accounting for 40%-50%, 20%-30% and 10%-15%, of PM2.5, respectively.

  9. Source apportionment of volatile organic compounds in Tehran, Iran.

    PubMed

    Sarkhosh, Maryam; Mahvi, Amir Hossein; Yunesian, Masud; Nabizadeh, Ramin; Borji, Saeedeh Hemmati; Bajgirani, Ali Ghiami

    2013-04-01

    Identifying the sources of volatile organic compounds (VOCs) is key issue to reducing ground-level ozone and PAN. A multivariate receptor model (Unmix) was used for the determination of the contributions of VOCs sources in Tehran-Iran. Concentrations of ambient C2-C10 VOCs were measured continuously and online at the center of Tehran city during the winter of 2012. A high correlation coefficient existed between measured and predicted values (R (2) = 0.99), indicating that the data were well modeled. Five possible VOCs source categories were identified and mobile sources such as vehicle exhaust (61 %) and fuel evaporation (12 %) more than half of the total VOC concentration. City gas and CNG sources, biogenic source, and industrial solvent source categories accounted for 17 %, 8 % and 2 % of the total VOC, respectively. Result showed Unmix for VOCs source apportionment can be used to analyze and generate air pollution control strategies and policies.

  10. Source Apportionment of Elemental Carbon in Beijing, China: Insights from Radiocarbon and Organic Marker Measurements.

    PubMed

    Zhang, Yan-Lin; Schnelle-Kreis, Jürgen; Abbaszade, Gülcin; Zimmermann, Ralf; Zotter, Peter; Shen, Rong-rong; Schäfer, Klaus; Shao, Longyi; Prévôt, André S H; Szidat, Sönke

    2015-07-21

    Elemental carbon (EC) or black carbon (BC) in the atmosphere has a strong influence on both climate and human health. In this study, radiocarbon ((14)C) based source apportionment is used to distinguish between fossil fuel and biomass burning sources of EC isolated from aerosol filter samples collected in Beijing from June 2010 to May 2011. The (14)C results demonstrate that EC is consistently dominated by fossil-fuel combustion throughout the whole year with a mean contribution of 79% ± 6% (ranging from 70% to 91%), though EC has a higher mean and peak concentrations in the cold season. The seasonal molecular pattern of hopanes (i.e., a class of organic markers mainly emitted during the combustion of different fossil fuels) indicates that traffic-related emissions are the most important fossil source in the warm period and coal combustion emissions are significantly increased in the cold season. By combining (14)C based source apportionment results and picene (i.e., an organic marker for coal emissions) concentrations, relative contributions from coal (mainly from residential bituminous coal) and vehicle to EC in the cold period were estimated as 25 ± 4% and 50 ± 7%, respectively, whereas the coal combustion contribution was negligible or very small in the warm period.

  11. Source apportionment of urban air pollutants using constrained receptor models with a priori profile information.

    PubMed

    Liao, Ho-Tang; Yau, Yu-Chen; Huang, Chun-Sheng; Chen, Nathan; Chow, Judith C; Watson, John G; Tsai, Shih-Wei; Chou, Charles C-K; Wu, Chang-Fu

    2017-08-01

    Exposure to air pollutants such as volatile organic compounds (VOCs) and fine particulate matter (PM2.5) are associated with adverse health effects. This study applied multiple time resolution data of hourly VOCs and 24-h PM2.5 to a constrained Positive Matrix Factorization (PMF) model for source apportionment in Taipei, Taiwan. Ninety-two daily PM2.5 samples and 2208 hourly VOC measurements were collected during four seasons in 2014 and 2015. With some a priori information, we used different procedures to constrain retrieved factors toward realistic sources. A total of nine source factors were identified as: natural gas/liquefied petroleum gas (LPG) leakage, solvent use/industrial process, contaminated marine aerosol, secondary aerosol/long-range transport, oil combustion, traffic related, evaporative gasoline emission, gasoline exhaust, and soil dust. Results showed that solvent use/industrial process was the largest contributor (19%) to VOCs while the largest contributor to PM2.5 mass was secondary aerosol/long-range transport (57%). A robust regression analysis showed that secondary aerosol was mostly contributed by regional transport related factor (25%). Copyright © 2017 Elsevier Ltd. All rights reserved.

  12. Photochemical grid model implementation and application of VOC, NOx, and O3 source apportionment

    EPA Science Inventory

    For the purposes of developing optimal emissions control strategies, efficient approaches are needed to identify the major sources or groups of sources that contribute to elevated ozone (O3) concentrations. Source-based apportionment techniques implemented in photochemical grid m...

  13. Photochemical grid model implementation and application of VOC, NOx, and O3 source apportionment

    EPA Science Inventory

    For the purposes of developing optimal emissions control strategies, efficient approaches are needed to identify the major sources or groups of sources that contribute to elevated ozone (O3) concentrations. Source-based apportionment techniques implemented in photochemical grid m...

  14. Source Apportionment of VOCs in Edmonton, Alberta

    NASA Astrophysics Data System (ADS)

    McCarthy, M. C.; Brown, S. G.; Aklilu, Y.; Lyder, D. A.

    2012-12-01

    Regional emissions at Edmonton, Alberta, are complex, containing emissions from (1) transportation sources, such as cars, trucks, buses, and rail; (2) industrial sources, such as petroleum refining, light manufacturing, and fugitive emissions from holding tanks or petroleum terminals; and (3) miscellaneous sources, such as biogenic emissions and natural gas use and processing. From 2003 to 2009, whole air samples were collected at two sites in Edmonton and analyzed for over 77 volatile organic compounds (VOCs). VOCs were sampled in the downtown area (Central) and the industrial area on the eastern side of the city (East). Concentrations of most VOCs were highest at the East site. The positive matrix factorization (PMF) receptor model was used to apportion ambient concentration measurements of VOCs into eleven factors, which were associated with emissions source categories. Factors of VOCs identified in the final eleven-factor solution include transportation sources (both gasoline and diesel vehicles), industrial sources, a biogenic source, and a natural-gas-related source. Transportation sources accounted for more mass at the Central site than at the East site; this was expected because Central is in a core urban area where transportation emissions are concentrated. Transportation sources accounted for nearly half of the VOC mass at the Central site, but only 6% of the mass at the East site. Encouragingly, mass from transportation sources has declined by about 4% a year in this area; this trend is similar to the decline found throughout the United States, and is likely due to fleet turnover as older, more highly polluting cars are replaced with newer, cleaner cars. In contrast, industrial sources accounted for ten times more VOC mass at the East site than at the Central site and were responsible for most of the total VOC mass observed at the East site. Of the six industrial factors identified at the East site, four were linked to petrochemical industry production

  15. RADIOCARBON SOURCE APPORTIONMENT IN A BIOFUELS ERA

    EPA Science Inventory

    Biofuels (gasohol and biodiesel) introduce radiocarbon into the U.S. mobile source fuel supply where it was previously absent. Initial measurements of radiocarbon in the PM2.5 combustion emissions from engines using gasohol indicate that this may have less effect on r...

  16. SOURCE APPORTIONMENT RESULTS, UNCERTAINTIES, AND MODELING TOOLS

    EPA Science Inventory

    Advanced multivariate receptor modeling tools are available from the U.S. Environmental Protection Agency (EPA) that use only speciated sample data to identify and quantify sources of air pollution. EPA has developed both EPA Unmix and EPA Positive Matrix Factorization (PMF) and ...

  17. Iodine source apportionment in the Malawian diet

    PubMed Central

    Watts, M. J.; Joy, E. J. M.; Young, S. D.; Broadley, M. R.; Chilimba, A. D. C.; Gibson, R. S.; Siyame, E. W. P.; Kalimbira, A. A.; Chilima, B.; Ander, E. L.

    2015-01-01

    The aim of this study was to characterise nutritional-I status in Malawi. Dietary-I intakes were assessed using new datasets of crop, fish, salt and water-I concentrations, while I status was assessed for 60 women living on each of calcareous and non-calcareous soils as defined by urinary iodine concentration (UIC). Iodine concentration in staple foods was low, with median concentrations of 0.01 mg kg−1 in maize grain, 0.008 mg kg−1 in roots and tubers, but 0.155 mg kg−1 in leafy vegetables. Freshwater fish is a good source of dietary-I with a median concentration of 0.51 mg kg−1. Mean Malawian dietary-Iodine intake from food, excluding salt, was just 7.8 μg d−1 compared to an adult requirement of 150 μg d−1. Despite low dietary-I intake from food, median UICs were 203 μg L−1 with only 12% defined as I deficient whilst 21% exhibited excessive I intake. Iodised salt is likely to be the main source of dietary I intake in Malawi; thus, I nutrition mainly depends on the usage and concentration of I in iodised salt. Drinking water could be a significant source of I in some areas, providing up to 108 μg d−1 based on consumption of 2 L d−1. PMID:26503697

  18. Iodine source apportionment in the Malawian diet

    NASA Astrophysics Data System (ADS)

    Watts, M. J.; Joy, E. J. M.; Young, S. D.; Broadley, M. R.; Chilimba, A. D. C.; Gibson, R. S.; Siyame, E. W. P.; Kalimbira, A. A.; Chilima, B.; Ander, E. L.

    2015-10-01

    The aim of this study was to characterise nutritional-I status in Malawi. Dietary-I intakes were assessed using new datasets of crop, fish, salt and water-I concentrations, while I status was assessed for 60 women living on each of calcareous and non-calcareous soils as defined by urinary iodine concentration (UIC). Iodine concentration in staple foods was low, with median concentrations of 0.01 mg kg-1 in maize grain, 0.008 mg kg-1 in roots and tubers, but 0.155 mg kg-1 in leafy vegetables. Freshwater fish is a good source of dietary-I with a median concentration of 0.51 mg kg-1. Mean Malawian dietary-Iodine intake from food, excluding salt, was just 7.8 μg d-1 compared to an adult requirement of 150 μg d-1. Despite low dietary-I intake from food, median UICs were 203 μg L-1 with only 12% defined as I deficient whilst 21% exhibited excessive I intake. Iodised salt is likely to be the main source of dietary I intake in Malawi; thus, I nutrition mainly depends on the usage and concentration of I in iodised salt. Drinking water could be a significant source of I in some areas, providing up to 108 μg d-1 based on consumption of 2 L d-1.

  19. Source apportionment of ambient volatile organic compounds in Beijing.

    PubMed

    Song, Yu; Shao, Min; Liu, Ying; Lu, Sihua; Kuster, William; Goldan, Paul; Xie, Shaodong

    2007-06-15

    The ambient air quality standard for ozone is frequently exceeded in Beijing in summer and autumn. Source apportionments of volatile organic compounds (VOCs), which are precursors of ground-level ozone formation, can be helpful to the further study of tropospheric ozone formation. In this study, ambient concentrations of VOCs were continuously measured with a time resolution of 30 min in August 2005 in Beijing. By using positive matrix factorization (PMF), eight sources for the selected VOC species were extracted. Gasoline-related emissions (the combination of gasoline exhaust and gas vapor), petrochemicals, and liquefied petroleum gas (LPG) contributed 52, 20, and 11%, respectively, to total ambient VOCs. VOC emissions from natural gas (5%), painting (5%), diesel vehicles (3%), and biogenic emissions (2%) were also identified. The gasoline-related, petrochemical, and biogenic sources were estimated to be the major contributors to ozone formation potentials in Beijing.

  20. A model-based approach for imputing censored data in source apportionment studies.

    PubMed

    Krall, Jenna R; Simpson, Charles H; Peng, Roger D

    2015-12-01

    Sources of particulate matter (PM) air pollution are generally inferred from PM chemical constituent concentrations using source apportionment models. Concentrations of PM constituents are often censored below minimum detection limits (MDL) and most source apportionment models cannot handle these censored data. Frequently, censored data are first substituted by a constant proportion of the MDL or are removed to create a truncated dataset before sources are estimated. When estimating the complete data distribution, these commonly applied methods to adjust censored data perform poorly compared with model-based imputation methods. Model-based imputation has not been used in source apportionment and may lead to better source estimation. However if the censored chemical constituents are not important for estimating sources, censoring adjustment methods may have little impact on source estimation. We focus on two source apportionment models applied in the literature and provide a comprehensive assessment of how censoring adjustment methods, including model-based imputation, impact source estimation. A review of censoring adjustment methods critically informs how censored data should be handled in these source apportionment models. In a simulation study, we demonstrated that model-based multiple imputation frequently leads to better source estimation compared with commonly used censoring adjustment methods. We estimated sources of PM in New York City and found estimated source distributions differed by censoring adjustment method. In this study, we provide guidance for adjusting censored PM constituent data in common source apportionment models, which is necessary for estimation of PM sources and their subsequent health effects.

  1. A model-based approach for imputing censored data in source apportionment studies

    PubMed Central

    Krall, Jenna R.; Simpson, Charles H.

    2015-01-01

    Sources of particulate matter (PM) air pollution are generally inferred from PM chemical constituent concentrations using source apportionment models. Concentrations of PM constituents are often censored below minimum detection limits (MDL) and most source apportionment models cannot handle these censored data. Frequently, censored data are first substituted by a constant proportion of the MDL or are removed to create a truncated dataset before sources are estimated. When estimating the complete data distribution, these commonly applied methods to adjust censored data perform poorly compared with model-based imputation methods. Model-based imputation has not been used in source apportionment and may lead to better source estimation. However if the censored chemical constituents are not important for estimating sources, censoring adjustment methods may have little impact on source estimation. We focus on two source apportionment models applied in the literature and provide a comprehensive assessment of how censoring adjustment methods, including model-based imputation, impact source estimation. A review of censoring adjustment methods critically informs how censored data should be handled in these source apportionment models. In a simulation study, we demonstrated that model-based multiple imputation frequently leads to better source estimation compared with commonly used censoring adjustment methods. We estimated sources of PM in New York City and found estimated source distributions differed by censoring adjustment method. In this study, we provide guidance for adjusting censored PM constituent data in common source apportionment models, which is necessary for estimation of PM sources and their subsequent health effects. PMID:26640398

  2. Critical review of black carbon and elemental carbon source apportionment in Europe and the United States

    NASA Astrophysics Data System (ADS)

    Briggs, Nicole L.; Long, Christopher M.

    2016-11-01

    An increasing number of air pollution source apportionment studies in Europe and the United States have focused on the black carbon (BC) fraction of ambient particulate matter (PM) given its linkage with adverse public health and climate impacts. We conducted a critical review of European and US BC source apportionment studies published since 2003. Since elemental carbon (EC) has been used as a surrogate measure of BC, we also considered source apportionment studies of EC measurements. This review extends the knowledge presented in previous ambient PM source apportionment reviews because we focus on BC and EC and critically examine the differences between source apportionment results for different methods and source categories. We identified about 50 BC and EC source apportionment studies that have been conducted in either Europe or the US since 2003, finding a striking difference in the commonly used source apportionment methods between the two regions and variations in the assigned source categories. Using three dominant methodologies (radiocarbon, aethalometer, and macro-tracer methods) that only allow for BC to be broadly apportioned into either fossil fuel combustion or biomass burning source categories, European studies generally support fossil fuel combustion as the dominant ambient BC source, but also show significant biomass burning contributions, in particular in wintertime at non-urban locations. Among US studies where prevailing methods such as chemical mass balance (CMB) and positive matrix factorization (PMF) models have allowed for estimation of more refined source contributions, there are fewer findings showing the significance of biomass burning and variable findings on the relative proportion of BC attributed to diesel versus gasoline emissions. Overall, the available BC source apportionment studies provide useful information demonstrating the significance of both fossil fuel combustion and biomass burning BC emission sources in Europe and the US

  3. Source Apportionment of sub-Arctic Pollutants at Denali National Park, Alaska

    NASA Astrophysics Data System (ADS)

    Bian, Q.; Kreidenweis, S. M.

    2014-12-01

    The "bromine (Br) explosion" in the springtime Arctic region, associated with rapid ozone depletion events, is now a well-documented phenomenon. The source of Br appears to be sea salt but its cycling between the aerosol and gas phase is not well understood. In this study, we observed the occurrence of elevated aerosol-phase Br concentrations in springtime IMPROVE network PM2.5 measurements in the sub-Arctic Denali National Park (DNP; site elevation, 658 MASL). Episodic elevated aerosol Br levels were observed from February to May in all years in the data record, 1988 to 2013. Anti-correlation (R=-0.54) between O3 and Br for high-concentration Br samples (Br>2 ng/m3, 130 out of 730 springtime samples) implied its possible link to ozone depletion events in the Arctic region. To further identify the sources influencing aerosol observed at DNP, source apportionment using the EPA Positive Matrix Factorization 5.0 model was applied to the entire PM2.5 speciated data from the DNP site. Six sources were derived, including secondary sulfate, a factor containing both Br and NO3-, dust, sea salt, smelting, and a mixture of wildfire and other combustion sources. Concentration weighted trajectory analysis, which was employed to identify the possible source origins, suggested that the Br/NO3- factor originated from northern Alaska in the springtime, and the secondary sulfate was largely associated with Asian sources that included Russian Norilsk Nickel. Sea salt, also originating from northern and northwestern coastal Alaska, was highest in the wintertime when high surface winds and low surface temperatures are expected. Dust, generally enhanced in April, May and June, was traced back to Eurasian sources. The smelting factor had a decreasing trend from 1988 to 2013, consistent with other studies of aerosol metal concentrations in the Arctic. The combustion factor was usually highest in the summertime, originated from near the surface in central Alaska, and was linked to

  4. Receptor model source apportionment of nonmethane hydrocarbons in Mexico City.

    PubMed

    Mugica, V; Watson, J; Vega, E; Reyes, E; Ruiz, M E; Chow, J

    2002-03-29

    With the purpose of estimating the source contributions of nonmethane hydrocarbons (NMHC) to the atmosphere at three different sites in the Mexico City Metropolitan Area, 92 ambient air samples were measured from February 23 to March 22 of 1997. Light- and heavy-duty vehicular profiles were determined to differentiate the NMHC contribution of diesel and gasoline to the atmosphere. Food cooking source profiles were also determined for chemical mass balance receptor model application. Initial source contribution estimates were carried out to determine the adequate combination of source profiles and fitting species. Ambient samples of NMHC were apportioned to motor vehicle exhaust, gasoline vapor, handling and distribution of liquefied petroleum gas (LP gas), asphalt operations, painting operations, landfills, and food cooking. Both gasoline and diesel motor vehicle exhaust were the major NMHC contributors for all sites and times, with a percentage of up to 75%. The average motor vehicle exhaust contributions increased during the day. In contrast, LP gas contribution was higher during the morning than in the afternoon. Apportionment for the most abundant individual NMHC showed that the vehicular source is the major contributor to acetylene, ethylene, pentanes, n-hexane, toluene, and xylenes, while handling and distribution of LP gas was the major source contributor to propane and butanes. Comparison between CMB estimates of NMHC and the emission inventory showed a good agreement for vehicles, handling and distribution of LP gas, and painting operations; nevertheless, emissions from diesel exhaust and asphalt operations showed differences, and the results suggest that these emissions could be underestimated.

  5. On the autarchic use of solely PIXE data in particulate matter source apportionment studies by receptor modeling

    NASA Astrophysics Data System (ADS)

    Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.; Giannoni, M.; Traversi, R.; Udisti, R.

    2015-11-01

    Particle Induced X-ray Emission (PIXE) analysis of aerosol samples allows simultaneous detection of several elements, including important tracers of many particulate matter sources. This capability, together with the possibility of analyzing a high number of samples in very short times, makes PIXE a very effective tool for source apportionment studies by receptor modeling. However, important aerosol components, like nitrates, OC and EC, cannot be assessed by PIXE: this limitation may strongly compromise the results of a source apportionment study if based on PIXE data alone. In this work, an experimental dataset characterised by an extended chemical speciation (elements, EC-OC, ions) is used to test the effect of reducing input species in the application of one of the most widely used receptor model, namely Positive Matrix Factorization (PMF). The main effect of using only PIXE data is that the secondary nitrate source is not identified and the contribution of biomass burning is overestimated, probably due to the similar seasonal pattern of these two sources.

  6. Spatially and chemically resolved source apportionment analysis: Case study of high particulate matter event

    NASA Astrophysics Data System (ADS)

    Kim, Byeong-Uk; Bae, Changhan; Kim, Hyun Cheol; Kim, Eunhye; Kim, Soontae

    2017-08-01

    This article presents the results of a detailed source apportionment study of the high particulate matter (PM) event in the Seoul Metropolitan Area (SMA), South Korea, during late February 2014. Using the Comprehensive Air Quality Model with Extensions with its Particulate Source Apportionment Technology (CAMx-PSAT), we defined 10 source regions, including five in China, for spatially and chemically resolved analyses. During the event, the spatially averaged PM10 concentration at all PM10 monitors in the SMA was 129 μg/m3, while the PM10 and PM2.5 concentrations at the BulGwang Supersite were 143 μg/m3 and 123 μg/m3, respectively. CAMx-PSAT showed reasonably good PM model performance in both China and the SMA. For February 23-27, CAMx-PSAT estimated that Chinese contributions to the SMA PM10 and PM2.5 were 84.3 μg/m3 and 80.0 μg/m3, respectively, or 64% and 70% of the respective totals, while South Korea's respective domestic contributions were 36.5 μg/m3 and 23.3 μg/m3. We observed that the spatiotemporal pattern of PM constituent concentrations and contributions did not necessarily follow that of total PM10 and PM2.5 concentrations. For example, Beijing-Tianjin-Hebei produced high nitrate concentrations, but the two most-contributing regions to PM in the SMA were the Near Beijing area and South Korea. In addition, we noticed that the relative contributions from each region changed over time. We found that most ammonium mass that neutralized Chinese sulfate mass in the SMA came from South Korean sources, indicating that secondary inorganic aerosol in the SMA, especially ammonium sulfates, during this event resulted from different major precursors originating from different regions.

  7. Source apportionment of PM2.5 in urban Shanghai based PMF and PSCF model

    NASA Astrophysics Data System (ADS)

    Zhao, M.; Xiu, G.; Qiao, T.

    2016-12-01

    Source apportionment of PM2.5 in urban Shanghai based PMF and PSCF modelMengfei Zhao, Guangli Xiu*, Ting Qiao State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemicals Processes, East China University of Science and Technology, Shanghai, China*Corresponding author: xiugl@ecust.edu.cnAbstract: In the study, we analyzed chemical compositions of PM2.5 collected in urban Shanghai from July 2013 to August 2014. Based on the analyzed species, seven major sources of PM2.5 identified from Positive Matrix Factorization (PMF) model included sulfate and ammonium dominant, nitrate dominant, coal combustion, biomass burning, Cu and Ni smelt industry, marine aerosols and mineral dust. The annual contribution of secondary sources (sulfate, ammonium and nitrate dominant) was similar to primary sources. As for secondary sources, sulfate and ammonium dominant was much higher than nitrate dominant, while nitrate dominant which represented mobile source played more important roles on haze days. Potential Source Contribution Function (PSCF) model was used to investigate the distribution area of each area. The result showed that secondary sources were relatively concentrated, mainly from the surroundings of Shanghai. Most primary sources were affected by regional transports. The source of coal combustion was located in the Northwest, and marine aerosols were from the ocean. The Yangtze River Delta (YRD) region and Pearl River Delta (PRD) region were major source areas of biomass burning and Cu and Ni smelt industry, respectively. In addition, Liquid water content (LWC) in PM2.5 was calculated by a thermodynamic model (AIM-IV). LWC showed positive correlations with nitrate dominant and sulfate and ammonium dominant (r=0.64 and 0.49, p<0.01). The correlation between LWC and nitrate dominant was more significant during heavy haze episodes.

  8. Source apportionment modeling of volatile organic compounds in streams

    USGS Publications Warehouse

    Pankow, J.F.; Asher, W.E.; Zogorski, J.S.

    2006-01-01

    It often is of interest to understand the relative importance of the different sources contributing to the concentration cw of a contaminant in a stream; the portions related to sources 1, 2, 3, etc. are denoted cw,1, cw,2, cw,3, etc. Like c w, 'he fractions ??1, = cw,1/c w, ??2 = cw,2/cw, ??3 = cw,3/cw, etc. depend on location and time. Volatile organic compounds (VOCs) can undergo absorption from the atmosphere into stream water or loss from stream water to the atmosphere, causing complexities affecting the source apportionment (SA) of VOCs in streams. Two SA rules are elaborated. Rule 1: VOC entering a stream across the air/water interface exclusively is assigned to the atmospheric portion of cw. Rule 2: VOC loss by volatilization, flow loss to groundwater, in-stream degradation, etc. is distributed over cw,1 cw,2, c w,3, etc. in proportion to their corresponding ?? values. How the two SA rules are applied, as well as the nature of the SA output for a given case, will depend on whether transport across the air/water interface is handled using the net flux F convention or using the individual fluxes J convention. Four hypothetical stream cases involving acetone, methyl-tert-butyl ether (MTBE), benzene, chloroform, and perchloroethylene (PCE) are considered. Acetone and MTBE are sufficiently water soluble from air for a domestic atmospheric source to be capable of yielding cw values approaching the common water quality guideline range of 1 to 10 ??g/L. For most other VOCs, such levels cause net outgassing (F > 0). When F > 0 in a given section of stream, in the net flux convention, all of the ??j, for the compound remain unchanged over that section while cw decreases. A characteristic time ??d can be calculated to predict when there will be differences between SA results obtained by the net flux convention versus the individual fluxes convention. Source apportionment modeling provides the framework necessary for comparing different strategies for mitigating

  9. Sources of Size Segregated Sulfate Aerosols in the Arctic Summer

    NASA Astrophysics Data System (ADS)

    Ghahremaninezhadgharelar, R.; Norman, A. L.; Abbatt, J.; Levasseur, M.

    2015-12-01

    Aerosols drive significant radiative forcing and affect Arctic climate. Despite the importance of these particles in Arctic climate change, there are some key uncertainties in the estimation of their effects and sources. Aerosols in six size fractions between <0.49 to 7.0 microns in diameter were collected on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic, during July 2014. A cascade impactor fitted to a high volume sampler was used for this study and was modified to permit collection of SO2 after aerosols were removed from the gas stream. The isotopic composition of sulfate aerosols and SO2 was measured and apportionment calculations have been performed to quantify the contribution of biogenic as well as anthropogenic sources to the growth of different aerosol size fractions in the atmosphere. The presence of sea salt sulfate aerosols was especially high in coarse mode aerosols as expected. The contribution of biogenic sulfate concentration in this study was higher than anthropogenic sulfate. Around 70% of fine aerosols (<0.49 μm) and 86% of SO2 were from biogenic sources. Concentrations of biogenic sulfate for fine aerosols, ranging from 18 to 625 ng/m3, were five times higher than total biogenic sulfate concentrations measured during Fall in the same region (Rempillo et al., 2011). A comparison of the isotope ratio for SO2 and fine aerosols offers a way to determine aerosol growth from local SO2 oxidation. For some samples, the values for SO2 and fine aerosols were close together suggesting the same source for SO2 and aerosol sulfur.Aerosols drive significant radiative forcing and affect Arctic climate. Despite the importance of these particles in Arctic climate change, there are some key uncertainties in the estimation of their effects and sources. Aerosols in six size fractions between <0.49 to 7.0 microns in diameter were collected on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic, during July 2014. A cascade impactor

  10. Metals and metalloids in atmospheric dust: Use of lead isotopic analysis for source apportionment

    NASA Astrophysics Data System (ADS)

    Felix Villar, Omar I.

    Mining activities generate aerosol in a wide range of sizes. Smelting activities produce mainly fine particles (<1 microm). On the other hand, milling, crushing and refining processes, as well tailings management, are significant sources of coarse particles (> 1 microm). The adverse effects of aerosols on human health depend mainly on two key characteristics: size and chemical composition. One of the main objectives of this research is to analyze the size distribution of contaminants in aerosol produced by mining operations. For this purpose, a Micro-Orifice Uniform Deposit Impactor (MOUDI) was utilized. Results from the MOUDI samples show higher concentrations of the toxic elements like lead and arsenic in the fine fraction (<1 microm). Fine particles are more likely to be deposited in the deeper zones of the respiratory system; therefore, they are more dangerous than coarse particles that can be filtered out in the upper respiratory system. Unfortunately, knowing the total concentration of contaminants does not give us enough information to identify the source of contamination. For this reason, lead isotopes have been introduced as fingerprints for source apportionment. Each source of lead has specific isotopic ratios; by knowing these ratios sources can be identified. During this research, lead isotopic ratios were analyzed at different sites and for different aerosol sizes. From these analyses it can be concluded that lead isotopes are a powerful tool to identify sources of lead. Mitigation strategies could be developed if the source of contamination is well defined. Environmental conditions as wind speed, wind direction, relative humidity and precipitation have an important role in the concentration of atmospheric dust. Dry environments with low relative humidity are ideal for the transport of aerosols. Results obtained from this research show the relationship between dust concentrations and meteorological parameters. Dust concentrations are highly correlated

  11. A Source Apportionment of U.S. Fine Particulate Matter Air Pollution

    PubMed Central

    Thurston, George D.; Ito, Kazuhiko; Lall, Ramona

    2011-01-01

    .5 components agreed well with the U.S. PM2.5 observed during the study period (mean=14.3 ug/m3; R2= 0.91). Apportionment regression analyses using single-element tracers for each source category gave results consistent with the APCA estimates. Comparisons of nearby sites indicated that the PM2.5 mass and the secondary aerosols were most homogenous spatially, while traffic PM2.5 and its tracer, EC, were among the most spatially representative of the source-related components. Comparison of apportionment results to a previous analysis of the 1979–1982 IP Network revealed similar and correlated major U.S. source category factors, albeit at lower levels than in the earlier period, suggesting a consistency in the U.S. spatial patterns of these source-related exposures over time, as well. These results indicate that applying source apportionment methods to the nationwide CSN can be an informative avenue for identifying and quantifying source components for the subsequent estimation of source-specific health effects, potentially contributing to more efficient regulation of PM2.5. PMID:24634604

  12. A source apportionment of U.S. fine particulate matter air pollution

    NASA Astrophysics Data System (ADS)

    Thurston, George D.; Ito, Kazuhiko; Lall, Ramona

    2011-08-01

    2.5 components agreed well with the U.S. PM 2.5 observed during the study period (mean = 14.3 μg m -3; R2 = 0.94). Apportionment regression analyses using single-element tracers for each source category gave results consistent with the APCA estimates. Comparisons of nearby sites indicated that the PM 2.5 mass and the secondary aerosols were most homogenous spatially, while traffic PM 2.5 and its tracer, EC, were among the most spatially representative of the source-related components. Comparison of apportionment results to a previous analysis of the 1979-1982 IP Network revealed similar and correlated major U.S. source category factors, albeit at lower levels than in the earlier period, suggesting a consistency in the U.S. spatial patterns of these source-related exposures over time, as well. These results indicate that applying source-apportionment methods to the nationwide CSN can be an informative avenue for identifying and quantifying source components for the subsequent estimation of source-specific health effects, potentially contributing to more efficient regulation of PM 2.5.

  13. Source apportionment of PM2.5 size distribution and composition data from multiple stationary sites using a mobile platform

    NASA Astrophysics Data System (ADS)

    Liao, Ho-Tang; Chou, Charles C.-K.; Huang, Sheng-Hsiu; Lu, Chia-Jung; Chen, Chih-Chieh; Hopke, Philip K.; Wu, Chang-Fu

    2017-07-01

    Several source apportionment studies considering multiple sites showed spatial variability of source contributions. However, setting up multiple fixed sites to collect comprehensive chemical speciation data is resource demanding. In this study, field campaigns were conducted at multiple receptor sites in the Mailiao and Taishi townships in Yunlin County using a mobile platform to demonstrate the feasibility of receptor modeling with particle size distribution and PM2.5 speciation data. Sources of air pollutants to all of the monitoring sites were identified and quantified using a modified positive matrix factorization (PMF) model. Modeling results indicated that a mixed source dominated by secondary aerosol was the largest contributor to PM2.5 at most sites. Adding VOC measurements with high time resolution helped to improve the source separation. Different patterns of source contributions among sites and seasons were observed showing both spatial heterogeneity and seasonal variation.

  14. Source Apportionment Using Positive Matrix Factorization on Daily Measurements of Inorganic and Organic Speciated PM2.5

    PubMed Central

    Dutton, Steven J.; Vedal, Sverre; Piedrahita, Ricardo; Milford, Jana B.; Miller, Shelly L.; Hannigan, Michael P.

    2012-01-01

    Particulate matter less than 2.5 microns in diameter (PM2.5) has been linked with a wide range of adverse health effects. Determination of the sources of PM2.5 most responsible for these health effects could lead to improved understanding of the mechanisms of such effects and more targeted regulation. This has provided the impetus for the Denver Aerosol Sources and Health (DASH) study, a multi-year source apportionment and health effects study relying on detailed inorganic and organic PM2.5 speciation measurements. In this study, PM2.5 source apportionment is performed by coupling positive matrix factorization (PMF) with daily speciated PM2.5 measurements including inorganic ions, elemental carbon (EC) and organic carbon (OC), and organic molecular markers. A qualitative comparison is made between two models, PMF2 and ME2, commonly used for solving the PMF problem. Many previous studies have incorporated chemical mass balance (CMB) for organic molecular marker source apportionment on limited data sets, but the DASH data set is large enough to use multivariate factor analysis techniques such as PMF. Sensitivity of the PMF2 and ME2 models to the selection of speciated PM2.5 components and model input parameters was investigated in depth. A combination of diagnostics was used to select an optimum, 7-factor model using one complete year of daily data with pointwise measurement uncertainties. The factors included 1) a wintertime/methoxyphenol factor, 2) an EC/sterane factor, 3) a nitrate/polycyclic aromatic hydrocarbon (PAH) factor, 4) a summertime/selective aliphatic factor, 5) an n-alkane factor, 6) a middle oxygenated PAH/alkanoic acid factor and 7) an inorganic ion factor. These seven factors were qualitatively linked with known PM2.5 emission sources with varying degrees of confidence. Mass apportionment using the 7-factor model revealed the contribution of each factor to the mass of OC, EC, nitrate and sulfate. On an annual basis, the majority of OC and EC mass

  15. Source Apportionment Using Positive Matrix Factorization on Daily Measurements of Inorganic and Organic Speciated PM(2.5).

    PubMed

    Dutton, Steven J; Vedal, Sverre; Piedrahita, Ricardo; Milford, Jana B; Miller, Shelly L; Hannigan, Michael P

    2010-07-01

    Particulate matter less than 2.5 microns in diameter (PM(2.5)) has been linked with a wide range of adverse health effects. Determination of the sources of PM(2.5) most responsible for these health effects could lead to improved understanding of the mechanisms of such effects and more targeted regulation. This has provided the impetus for the Denver Aerosol Sources and Health (DASH) study, a multi-year source apportionment and health effects study relying on detailed inorganic and organic PM(2.5) speciation measurements.In this study, PM(2.5) source apportionment is performed by coupling positive matrix factorization (PMF) with daily speciated PM(2.5) measurements including inorganic ions, elemental carbon (EC) and organic carbon (OC), and organic molecular markers. A qualitative comparison is made between two models, PMF2 and ME2, commonly used for solving the PMF problem. Many previous studies have incorporated chemical mass balance (CMB) for organic molecular marker source apportionment on limited data sets, but the DASH data set is large enough to use multivariate factor analysis techniques such as PMF.Sensitivity of the PMF2 and ME2 models to the selection of speciated PM(2.5) components and model input parameters was investigated in depth. A combination of diagnostics was used to select an optimum, 7-factor model using one complete year of daily data with pointwise measurement uncertainties. The factors included 1) a wintertime/methoxyphenol factor, 2) an EC/sterane factor, 3) a nitrate/polycyclic aromatic hydrocarbon (PAH) factor, 4) a summertime/selective aliphatic factor, 5) an n-alkane factor, 6) a middle oxygenated PAH/alkanoic acid factor and 7) an inorganic ion factor. These seven factors were qualitatively linked with known PM(2.5) emission sources with varying degrees of confidence. Mass apportionment using the 7-factor model revealed the contribution of each factor to the mass of OC, EC, nitrate and sulfate. On an annual basis, the majority of OC

  16. Source apportionment using positive matrix factorization on daily measurements of inorganic and organic speciated PM 2.5

    NASA Astrophysics Data System (ADS)

    Dutton, Steven J.; Vedal, Sverre; Piedrahita, Ricardo; Milford, Jana B.; Miller, Shelly L.; Hannigan, Michael P.

    2010-07-01

    Particulate matter less than 2.5 microns in diameter (PM 2.5) has been linked with a wide range of adverse health effects. Determination of the sources of PM 2.5 most responsible for these health effects could lead to improved understanding of the mechanisms of such effects and more targeted regulation. This has provided the impetus for the Denver Aerosol Sources and Health (DASH) study, a multi-year source apportionment and health effects study relying on detailed inorganic and organic PM 2.5 speciation measurements. In this study, PM 2.5 source apportionment is performed by coupling positive matrix factorization (PMF) with daily speciated PM 2.5 measurements including inorganic ions, elemental carbon (EC) and organic carbon (OC), and organic molecular markers. A qualitative comparison is made between two models, PMF2 and ME2, commonly used for solving the PMF problem. Many previous studies have incorporated chemical mass balance (CMB) for organic molecular marker source apportionment on limited data sets, but the DASH data set is large enough to use multivariate factor analysis techniques such as PMF. Sensitivity of the PMF2 and ME2 models to the selection of speciated PM 2.5 components and model input parameters was investigated in depth. A combination of diagnostics was used to select an optimum, 7-factor model using one complete year of daily data with pointwise measurement uncertainties. The factors included 1) a wintertime/methoxyphenol factor, 2) an EC/sterane factor, 3) a nitrate/polycyclic aromatic hydrocarbon (PAH) factor, 4) a summertime/selective aliphatic factor, 5) an n-alkane factor, 6) a middle-oxygenated PAH/alkanoic acid factor and 7) an inorganic ion factor. These seven factors were qualitatively linked with known PM 2.5 emission sources with varying degrees of confidence. Mass apportionment using the 7-factor model revealed the contribution of each factor to the mass of OC, EC, nitrate and sulfate. On an annual basis, the majority of OC and EC

  17. Source apportionment of speciated PM10 in the United Kingdom in 2008: Episodes and annual averages

    NASA Astrophysics Data System (ADS)

    Redington, A. L.; Witham, C. S.; Hort, M. C.

    2016-11-01

    The Lagrangian atmospheric dispersion model NAME (Numerical Atmospheric-dispersion Modelling Environment), has been used to simulate the formation and transport of PM10 over North-West Europe in 2008. The model has been evaluated against UK measurement data and been shown to adequately represent the observed PM10 at rural and urban sites on a daily basis. The Lagrangian nature of the model allows information on the origin of pollutants (and hence their secondary products) to be retained to allow attribution of pollutants at receptor sites back to their sources. This source apportionment technique has been employed to determine whether the different components of the modelled PM10 have originated from UK, shipping, European (excluding the UK) or background sources. For the first time this has been done to evaluate the composition during periods of elevated PM10 as well as the annual average composition. The episode data were determined by selecting the model data for each hour when the corresponding measurement data was >50 μg/m3. All the modelled sites show an increase in European pollution contribution and a decrease in the background contribution in the episode case compared to the annual average. The European contribution is greatest in southern and eastern parts of the UK and decreases moving northwards and westwards. Analysis of the speciated attribution data over the selected sites reveals that for 2008, as an annual average, the top three contributors to total PM10 are UK primary PM10 (17-25%), UK origin nitrate aerosol (18-21%) and background PM10 (11-16%). Under episode conditions the top three contributors to modelled PM10 are UK origin nitrate aerosol (12-33%), European origin nitrate aerosol (11-19%) and UK primary PM10 (12-18%).

  18. pH of Aerosols in a Polluted Atmosphere: Source Contributions to Highly Acidic Aerosol.

    PubMed

    Shi, Guoliang; Xu, Jiao; Peng, Xing; Xiao, Zhimei; Chen, Kui; Tian, Yingze; Guan, Xinbei; Feng, Yinchang; Yu, Haofei; Nenes, Athanasios; Russell, Armistead G

    2017-04-18

    Acidity (pH) plays a key role in the physical and chemical behavior of PM2.5. However, understanding of how specific PM sources impact aerosol pH is rarely considered. Performing source apportionment of PM2.5 allows a unique link of sources pH of aerosol from the polluted city. Hourly water-soluble (WS) ions of PM2.5 were measured online from December 25th, 2014 to June 19th, 2015 in a northern city in China. Five sources were resolved including secondary nitrate (41%), secondary sulfate (26%), coal combustion (14%), mineral dust (11%), and vehicle exhaust (9%). The influence of source contributions to pH was estimated by ISORROPIA-II. The lowest aerosol pH levels were found at low WS-ion levels and then increased with increasing total ion levels, until high ion levels occur, at which point the aerosol becomes more acidic as both sulfate and nitrate increase. Ammonium levels increased nearly linearly with sulfate and nitrate until approximately 20 μg m(-3), supporting that the ammonium in the aerosol was more limited by thermodynamics than source limitations, and aerosol pH responded more to the contributions of sources such as dust than levels of sulfate. Commonly used pH indicator ratios were not indicative of the pH estimated using the thermodynamic model.

  19. Source apportionment of airborne particulate matter using inorganic and organic species as tracers

    NASA Astrophysics Data System (ADS)

    Wang, Yungang; Hopke, Philip K.; Xia, Xiaoyan; Rattigan, Oliver V.; Chalupa, David C.; Utell, Mark J.

    2012-08-01

    Source apportionment is typically performed on chemical composition data derived from particulate matter (PM) samples. However, many common sources no longer emit significant amounts of characteristic trace elements requiring the use of more comprehensive chemical characterization in order to fully resolve the PM sources. Positive matrix factorization (EPA PMF, version 4.1) was used to analyze 24-hr integrated molecular marker (MM), secondary inorganic ions, trace elements, carbonaceous species and light absorption data to investigate sources of PM2.5 in Rochester, New York between October 2009 and October 2010 to explore the role of specific MMs. An eight-factor solution was found for which the factors were identified as isoprene secondary organic aerosol (SOA), airborne soil, other SOA, diesel emissions, secondary sulfate, wood combustion, gasoline vehicle, and secondary nitrate contributing 6.9%, 12.8%, 3.7%, 7.8%, 45.5%, 9.1%, 7.9%, and 6.3% to the average PM2.5 concentration, respectively Concentrations of pentacosane, hexacosane, heptacosane, and octacosane in the gasoline vehicles factor were larger compared to diesel emissions. Aethalometer Delta-C was strongly associated with wood combustion. The compounds, n-heptacosanoic acid and n-octacosanoic acid, occasionally used in the past as tracers for road dust, were found to largely associate with SOA in this study. In comparison with a standard PMF analyses without MM, inclusion of them was necessary to resolve SOA and wood combustion factors in urban areas.

  20. Source apportionment of airborne particulate matter for the speciation trends network site in Cleveland, OH

    SciTech Connect

    Liming Zhou; Philip K. Hopke; Weixiang Zhao

    2009-03-15

    Aerosol composition data from the Speciation Trends Network (STN) site (East 14th Street) in Cleveland, OH, were analyzed by advanced receptor model methods for source apportionment as well as by the standard positive matrix factorization (PMF) using PMF2. These different models are used in combination to test model limitations. These data were 24-hr average mass concentrations and compositions obtained for samples taken every third day from 2001 to 2003. The Multilinear Engine (ME) was used to solve an expanded model to estimate the source profiles and source contributions and also to investigate the wind speed, wind direction, time-of-day, weekend/weekday, and seasonal effects. PMF2 was applied to the same dataset. Potential source contribution function (PSCF) and conditional probability function (CPF) analyses were used to locate the regional and local sources using the resolved source contributions and appropriate meteorological data. Very little difference was observed between the results of the expanded model and the PMF2 values for the profiles and source contribution time series. The identified sources were as ferrous smelter, secondary sulfate, secondary nitrate, soil/combustion mixture, steel mill, traffic, wood smoke, and coal burning. The CPF analysis was useful in helping to identify local sources, whereas the PSCF results were only useful for regional source areas. Both of these analyses were more useful than the wind directional factor derived from the expanded factor analysis. However, the expanded analysis provided direct information on seasonality and day-of-week behavior of the sources. 28 refs., 8 figs., 4 tabs.

  1. Open air mineral treatment operations and ambient air quality: assessment and source apportionment.

    PubMed

    Escudero, M; Alastuey, A; Moreno, T; Querol, X; Pérez, P

    2012-11-01

    We present a methodology for evaluating and quantifying the impact of inhalable mineral dust resuspension close to a potentially important industrial point source, in this case an open air plant producing sand, flux and kaolin in the Capuchinos district of Alcañiz (Teruel, NE Spain). PM(10) levels at Capuchinos were initially high (42 μg m(-3) as the annual average with 91 exceedances of the EU daily limit value during 2007) but subsequently decreased (26 μg m(-3) with 16 exceedances in 2010) due to a reduced demand for minerals from the ceramic industry and construction sector during the first stages of the economic crisis. Back trajectory and local wind pattern analyses revealed only limited contribution from exotic PM sources such as African dust intrusions whereas there was clearly a strong link with the mineral stockpiles of the local industry. This link was reinforced by chemical and mineral speciation and source apportionment analysis which showed a dominance of mineral matter (sum of CO(3)(2-), SiO(2), Al(2)O(3), Ca, Fe, K, Mg, P, and Ti: mostly aluminosilicates) which in 2007 contributed 76% of the PM(10) mass (44 μg m(-3) on average). The contribution from Secondary Inorganic Aerosols (SIA, sum of SO(4)(2-), NO(3)(-) and NH(4)(+)) reached 8.4 μg m(-3), accounting for 14% of the PM(10) mass, similar to the amount of calcareous road dust estimated to be present (8 μg m(-3); 13%). Organic matter and elemental carbon contributed 5.3 μg m(-3) (9%) whereas marine aerosol (Na + Cl) levels were minor with an average concentration of 0.4 μg m(-3) (1% of the PM(10) mass). Finally, chemical and mineralogical analysis of stockpile samples and comparison with filter samples confirmed the local industry to be the major source of ambient PM(10) in the area.

  2. Source Apportionment of Atmospheric Particles by Electron Probe X-Ray Microanalysis and Receptor Models.

    NASA Astrophysics Data System (ADS)

    van Borm, Werner August

    Electron probe X-ray microanalysis (EPXMA) in combination with an automation system and an energy-dispersive X-ray detection system was used to analyse thousands of microscopical particles, originating from the ambient atmosphere. The huge amount of data was processed by a newly developed X-ray correction method and a number of data reduction procedures. A standardless ZAF procedure for EPXMA was developed for quick semi-quantitative analysis of particles starting from simple corrections, valid for bulk samples and modified taking into account the particle finit diameter, assuming a spherical shape. Tested on a limited database of bulk and particulate samples, the compromise between calculation speed and accuracy yielded for elements with Z > 14 accuracies on concentrations less than 10% while absolute deviations remained below 4 weight%, thus being only important for low concentrations. Next, the possibilities for the use of supervised and unsupervised multivariate particle classification were investigated for source apportionment of individual particles. In a detailed study of the unsupervised cluster analysis technique several aspects were considered, that have a severe influence on the final cluster analysis results, i.e. data acquisition, X-ray peak identification, data normalization, scaling, variable selection, similarity measure, cluster strategy, cluster significance and error propagation. A supervised approach was developed using an expert system-like approach in which identification rules are builded to describe the particle classes in a unique manner. Applications are presented for particles sampled (1) near a zinc smelter (Vieille-Montagne, Balen, Belgium), analyzed for heavy metals, (2) in an urban aerosol (Antwerp, Belgium), analyzed for over 20 elements and (3) in a rural aerosol originating from a swiss mountain area (Bern). Thus is was possible to pinpoint a number of known and unknown sources and characterize their emissions in terms of particles

  3. Nitrate source apportionment in a subtropical watershed using Bayesian model.

    PubMed

    Yang, Liping; Han, Jiangpei; Xue, Jianlong; Zeng, Lingzao; Shi, Jiachun; Wu, Laosheng; Jiang, Yonghai

    2013-10-01

    Nitrate (NO3-) pollution in aquatic system is a worldwide problem. The temporal distribution pattern and sources of nitrate are of great concern for water quality. The nitrogen (N) cycling processes in a subtropical watershed located in Changxing County, Zhejiang Province, China were greatly influenced by the temporal variations of precipitation and temperature during the study period (September 2011 to July 2012). The highest NO3- concentration in water was in May (wet season, mean±SD=17.45±9.50 mg L(-1)) and the lowest concentration occurred in December (dry season, mean±SD=10.54±6.28 mg L(-1)). Nevertheless, no water sample in the study area exceeds the WHO drinking water limit of 50 mg L(-1) NO3-. Four sources of NO3(-) (atmospheric deposition, AD; soil N, SN; synthetic fertilizer, SF; manure & sewage, M&S) were identified using both hydrochemical characteristics [Cl-, NO3-, HCO3-, SO42-, Ca2+, K+, Mg2+, Na+, dissolved oxygen (DO)] and dual isotope approach (δ15N-NO3- and δ(18)O-NO3-). Both chemical and isotopic characteristics indicated that denitrification was not the main N cycling process in the study area. Using a Bayesian model (stable isotope analysis in R, SIAR), the contribution of each source was apportioned. Source apportionment results showed that source contributions differed significantly between the dry and wet season, AD and M&S contributed more in December than in May. In contrast, SN and SF contributed more NO3- to water in May than that in December. M&S and SF were the major contributors in December and May, respectively. Moreover, the shortcomings and uncertainties of SIAR were discussed to provide implications for future works. With the assessment of temporal variation and sources of NO3-, better agricultural management practices and sewage disposal programs can be implemented to sustain water quality in subtropical watersheds. Copyright © 2013 Elsevier B.V. All rights reserved.

  4. Sensitivity of fluvial sediment source apportionment to mixing model assumptions: A Bayesian model comparison

    PubMed Central

    Cooper, Richard J; Krueger, Tobias; Hiscock, Kevin M; Rawlins, Barry G

    2014-01-01

    Mixing models have become increasingly common tools for apportioning fluvial sediment load to various sediment sources across catchments using a wide variety of Bayesian and frequentist modeling approaches. In this study, we demonstrate how different model setups can impact upon resulting source apportionment estimates in a Bayesian framework via a one-factor-at-a-time (OFAT) sensitivity analysis. We formulate 13 versions of a mixing model, each with different error assumptions and model structural choices, and apply them to sediment geochemistry data from the River Blackwater, Norfolk, UK, to apportion suspended particulate matter (SPM) contributions from three sources (arable topsoils, road verges, and subsurface material) under base flow conditions between August 2012 and August 2013. Whilst all 13 models estimate subsurface sources to be the largest contributor of SPM (median ∼76%), comparison of apportionment estimates reveal varying degrees of sensitivity to changing priors, inclusion of covariance terms, incorporation of time-variant distributions, and methods of proportion characterization. We also demonstrate differences in apportionment results between a full and an empirical Bayesian setup, and between a Bayesian and a frequentist optimization approach. This OFAT sensitivity analysis reveals that mixing model structural choices and error assumptions can significantly impact upon sediment source apportionment results, with estimated median contributions in this study varying by up to 21% between model versions. Users of mixing models are therefore strongly advised to carefully consider and justify their choice of model structure prior to conducting sediment source apportionment investigations. Key Points An OFAT sensitivity analysis of sediment fingerprinting mixing models is conducted Bayesian models display high sensitivity to error assumptions and structural choices Source apportionment results differ between Bayesian and frequentist approaches PMID

  5. Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

    2014-02-01

    to better understand the chemical nature of atypical factors from high resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

  6. Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modeling of complete high time-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    McGuire, M. L.; Chang, R. Y.-W.; Slowik, J. G.; Jeong, C.-H.; Healy, R. M.; Lu, G.; Mihele, C.; Abbatt, J. P. D.; Brook, J. R.; Evans, G. J.

    2014-08-01

    method would be even more useful for HR-ToF-AMS data, due to the ability to understand better the chemical nature of atypical factors from high-resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of the extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

  7. Chemical Characterization and Source Apportionment of Particulate Matter in Lahore, Pakistan

    NASA Astrophysics Data System (ADS)

    von Schneidemesser, Erika; Stone, Elizabeth; Quraishi, Tauseef; Schauer, James; Shafer, Martin; Mahmood, Abid

    2010-05-01

    Lahore, Pakistan is a rapidly growing megacity with a population approaching 10 million. A significant issue affecting many of the world's megacities is extremely high levels of air pollution associated with transportation, solid fuel combustion, and industrial sources. High ambient concentrations of particulate matter (PM), as well as high levels of toxic components of PM, have been linked to increased mortality and morbidity. Although much focus has been directed at particulate matter mass, in many developing and underdeveloped nations, the adverse health impacts of high levels of PM are further enhanced by the high concentrations of toxic components in PM. To address these issues is Lahore, a measurement campaign of fine (PM2.5) and coarse (PM10-2.5) particulate matter was conducted for the 2007 calendar year, which included measurements of particle mass, detailed chemical composition of PM and source apportionment calculations. Annual average PM2.5 and PM10 concentrations were measured to be 194 µg m-3 and 336 µg m-3, respectively, with daily 24-hour maximum concentrations of 410 µg m-3 and 650 µg m-3 for PM2.5 and PM10, respectively. PM2.5 and PM10 samples were analysed for organic and elemental carbon, organic species, ionic species, elemental composition, water soluble elements and biological activity using a macrophage ROS assay. The coarse mode was dominated by crustal dust components, while the fine fraction was dominated by carbonaceous aerosols. The PM10 elemental composition data, which included data for toxic metals, was processed using principle component analysis to determine likely source categories. Seven factors were identified explaining 91% of the variance of the measured components. The factors included a number of industrial sources, re-suspended soil, mobile sources, and regional secondary aerosol. Source contributions to the organic carbon (OC) component of the PM2.5 fraction were identified using organic tracer species and chemical

  8. Fine particulate matter in the tropical environment: monsoonal effects, source apportionment, and health risk assessment

    NASA Astrophysics Data System (ADS)

    Khan, M. F.; Latif, M. T.; Saw, W. H.; Amil, N.; Nadzir, M. S. M.; Sahani, M.; Tahir, N. M.; Chung, J. X.

    2016-01-01

    The health implications of PM2.5 in the tropical region of Southeast Asia (SEA) are significant as PM2.5 can pose serious health concerns. PM2.5 concentration and sources here are strongly influenced by changes in the monsoon regime from the south-west quadrant to the north-east quadrant in the region. In this work, PM2.5 samples were collected at a semi-urban area using a high-volume air sampler at different seasons on 24 h basis. Analysis of trace elements and water-soluble ions was performed using inductively coupled plasma mass spectroscopy (ICP-MS) and ion chromatography (IC), respectively. Apportionment analysis of PM2.5 was carried out using the United States Environmental Protection Agency (US EPA) positive matrix factorization (PMF) 5.0 and a mass closure model. We quantitatively characterized the health risks posed to human populations through the inhalation of selected heavy metals in PM2.5. 48 % of the samples collected exceeded the World Health Organization (WHO) 24 h PM2.5 guideline but only 19 % of the samples exceeded 24 h US EPA National Ambient Air Quality Standard (NAAQS). The PM2.5 concentration was slightly higher during the north-east monsoon compared to south-west monsoon. The main trace metals identified were As, Pb, Cd, Ni, Mn, V, and Cr while the main ions were SO42-, NO3-, NH4+, and Na. The mass closure model identified four major sources of PM2.5 that account for 55 % of total mass balance. The four sources are mineral matter (MIN) (35 %), secondary inorganic aerosol (SIA) (11 %), sea salt (SS) (7 %), and trace elements (TE) (2 %). PMF 5.0 elucidated five potential sources: motor vehicle emissions coupled with biomass burning (31 %) were the most dominant, followed by marine/sulfate aerosol (20 %), coal burning (19 %), nitrate aerosol (17 %), and mineral/road dust (13 %). The hazard quotient (HQ) for four selected metals (Pb, As, Cd, and Ni) in PM2.5 mass was highest in PM2.5 mass from the coal burning source and least in PM2.5 mass

  9. MONITORING AND SOURCE APPORTIONMENT OF PARTICULATE MATTER NEAR A LARGE PHOSPHORUS PRODUCTION FACILITY

    EPA Science Inventory

    A source apportionment study was conducted to identify sources within a large elemental phosphorus plant that contribute to exceedances of the National Ambient Air Quality Standard for 24-h PM10. Ambient data were collected at three monitoring sites from October 1996 through Ju...

  10. DEVELOPMENT AND EVALUATION OF PM 2.5 SOURCE APPORTIONMENT METHODOLOGIES

    EPA Science Inventory

    The receptor model called Positive Matrix Factorization (PMF) has been extensively used to apportion sources of ambient fine particulate matter (PM2.5), but the accuracy of source apportionment results currently remains unknown. In addition, air quality forecast model...

  11. MONITORING AND SOURCE APPORTIONMENT OF PARTICULATE MATTER NEAR A LARGE PHOSPHORUS PRODUCTION FACILITY

    EPA Science Inventory

    A source apportionment study was conducted to identify sources within a large elemental phosphorus plant that contribute to exceedances of the National Ambient Air Quality Standard for 24-h PM10. Ambient data were collected at three monitoring sites from October 1996 through Ju...

  12. DEVELOPMENT AND EVALUATION OF PM 2.5 SOURCE APPORTIONMENT METHODOLOGIES

    EPA Science Inventory

    The receptor model called Positive Matrix Factorization (PMF) has been extensively used to apportion sources of ambient fine particulate matter (PM2.5), but the accuracy of source apportionment results currently remains unknown. In addition, air quality forecast model...

  13. Source apportionment of PM10, organic carbon and elemental carbon at Swiss sites: an intercomparison of different approaches.

    PubMed

    Gianini, M F D; Piot, C; Herich, H; Besombes, J-L; Jaffrezo, J-L; Hueglin, C

    2013-06-01

    In this study, the results of source apportionment of particulate matter (PM10), organic carbon (OC), and elemental carbon (EC) - as obtained through different approaches at different types of sites (urban background, urban roadside, and two rural sites in Switzerland) - are compared. The methods included in this intercomparison are positive matrix factorisation modelling (PMF, applied to chemical composition data including trace elements, inorganic ions, OC, and EC), molecular marker chemical mass balance modelling (MM-CMB), and the aethalometer model (AeM). At all sites, the agreement of the obtained source contributions was reasonable for OC, EC, and PM10. Based on an annual average, and at most of the considered sites, secondary organic carbon (SOC) is the component with the largest contribution to total OC; the most important primary source of OC is wood combustion, followed by road traffic. Secondary aerosols predominate in PM10. All considered techniques identified road traffic as the dominant source of EC, while wood combustion emissions are of minor importance for this constituent. The intercomparison of different source apportionment approaches is helpful to identify the strengths and the weaknesses of the different methods. Application of PMF has limitations when source emissions have a strong temporal correlation, or when meteorology has a strong impact on PM variability. In these cases, the use of PMF can result in mixed source profiles and consequently in the under- or overestimation of the real-world sources. The application of CMB models can be hampered by the unavailability of source profiles and the non-representativeness of the available profiles for local source emissions. This study also underlines that chemical transformations of molecular markers in the atmosphere can lead to the underestimation of contributions from primary sources, in particular during the summer period or when emission sources are far away from the receptor sites.

  14. Chemical speciation and source apportionment of fine particulate matter in Santiago, Chile, 2013.

    PubMed

    Villalobos, Ana M; Barraza, Francisco; Jorquera, Héctor; Schauer, James J

    2015-04-15

    Santiago is one of the largest cities in South America and has experienced high fine particulate matter (PM2.5) concentrations in fall and winter months for decades. To better understand the sources of fall and wintertime pollution in Santiago, PM2.5 samples were collected for 24 h every weekday from March to October 2013 for chemical analysis. Samples were analyzed for mass, elemental carbon (EC), organic carbon (OC), water soluble organic carbon (WSOC), water soluble nitrogen (WSTN), secondary inorganic ions, and particle-phase organic tracers for source apportionment. Selected samples were analyzed as monthly composites for organic tracers. PM2.5 concentrations were considerably higher in the coldest months (June-July), averaging (mean ± standard deviation) 62±15 μg/m(3) in these two months. Average fine particle mass concentration during the study period was 40±20 μg/m(3). Organic matter during the peak winter months was the major component of fine particles comprising around 70% of the particle mass. Source contributions to OC were calculated using organic molecular markers and a chemical mass balance (CMB) receptor model. The four combustion sources identified were wood smoke, diesel engine emission, gasoline vehicles, and natural gas. Wood smoke was the predominant source of OC, accounting for 58±42% of OC in fall and winter. Wood smoke and nitrate were the major contributors to PM2.5. In fall and winter, wood smoke accounted for 9.8±7.1 μg/m(3) (21±15%) and nitrate accounted for 9.1±4.8 μg/m(3) (20±10%) of fine PM. The sum of secondary inorganic ions (sulfate, nitrate, and ammonium) represented about 30% of PM2.5 mass. Secondary organic aerosols contributed only in warm months, accounting for about 30% of fine PM during this time. Copyright © 2015 Elsevier B.V. All rights reserved.

  15. Source apportionment of urban fine and ultra-fine particle number concentration in a Western Mediterranean city

    NASA Astrophysics Data System (ADS)

    Pey, Jorge; Querol, Xavier; Alastuey, Andrés; Rodríguez, Sergio; Putaud, Jean Philippe; Van Dingenen, Rita

    Extensive measurements on particle number concentration and size distribution (13-800 nm), together with detailed chemical composition of PM 2.5 have constituted the main inputs of the database used for a source apportionment analysis. Data were collected at an urban background site in Barcelona, Western Mediterranean. The source identification analysis helped us to distinguish five emission sources (vehicle exhausts, mineral dust, sea spray, industrial source and fuel-oil combustion) and two atmospheric processes (photochemical induced nucleation and regional/urban background particles derived from coagulation and condensation processes). After that, a multilinear regression analysis was applied in order to quantify the contribution of each factor. This study reveals that vehicle exhausts contribute dominantly to the number concentration in all the particle sizes (52-86%), but especially in the range 30-200 nm. This work also points out the importance of the regional and/or urban formed aerosols (secondary inorganic particles) on the total number concentration (around 25% of the total number), with a higher impact on the accumulation mode. The photo-chemically induced nucleation of aerosols only represents a small proportion of the total number as an annual mean (3%), but is very relevant when considering only the nucleation mode (13-20 nm) fraction (23%). The other sources recognized registered sporadic contributions to the total number, coinciding with specific meteorological scenarios. This study discloses the main sources and features affecting and controlling the fine and ultra-fine aerosols in a typical city in the Western Mediterranean coast. Whereas the road traffic appears to be the most important source of sub-micrometric aerosols, other sources may not be negligible under specific meteorological conditions.

  16. Modeling and source apportionment of diesel particulate matter.

    PubMed

    Díaz-Robles, L A; Fu, J S; Reed, G D

    2008-01-01

    The fine and ultra fine sizes of diesel particulate matter (DPM) are of greatest health concern. The composition of these primary and secondary fine and ultra fine particles is principally elemental carbon (EC) with adsorbed organic compounds, sulfate, nitrate, ammonia, metals, and other trace elements. The purpose of this study was to use an advanced air quality modeling technique to predict and analyze the emissions and the primary and secondary aerosols concentrations that come from diesel-fueled sources (DFS). The National Emissions Inventory for 1999 and a severe southeast ozone episode that occurred between August and September 1999 were used as reference. Five urban areas and one rural area in the Southeastern US were selected to compare the main results. For urban emissions, results showed that DFS contributed (77.9%+/-8.0) of EC, (16.8%+/-8.2) of organic aerosols, (14.3%+/-6.2) of nitrate, and (8.3%+/-6.6) of sulfate during the selected episodes. For the rural site, these contributions were lower. The highest DFS contribution on EC emissions was allocated in Memphis, due mainly to diesel non-road sources (60.9%). For ambient concentrations, DFS contributed (69.5%+/-6.5) of EC and (10.8%+/-2.4) of primary anthropogenic organic aerosols, where the highest DFS contributions on EC were allocated in Nashville and Memphis on that episode. The DFS contributed (8.3%+/-1.2) of the total ambient PM(2.5) at the analyzed sites. The maximum primary DPM concentration occurred in Atlanta (1.44 microg/m(3)), which was 3.8 times higher than that from the rural site. Non-linearity issues were encountered and recommendations were made for further research. The results indicated significant geographic variability in the EC contribution from DFS, and the main DPM sources in the Southeastern U.S. were the non-road DFS. The results of this work will be helpful in addressing policy issues targeted at designing control strategies on DFS in the Southeastern U.S.

  17. Problems in the fingerprints based polycyclic aromatic hydrocarbons source apportionment analysis and a practical solution.

    PubMed

    Zou, Yonghong; Wang, Lixia; Christensen, Erik R

    2015-10-01

    This work intended to explain the challenges of the fingerprints based source apportionment method for polycyclic aromatic hydrocarbons (PAH) in the aquatic environment, and to illustrate a practical and robust solution. The PAH data detected in the sediment cores from the Illinois River provide the basis of this study. Principal component analysis (PCA) separates PAH compounds into two groups reflecting their possible airborne transport patterns; but it is not able to suggest specific sources. Not all positive matrix factorization (PMF) determined sources are distinguishable due to the variability of source fingerprints. However, they constitute useful suggestions for inputs for a Bayesian chemical mass balance (CMB) analysis. The Bayesian CMB analysis takes into account the measurement errors as well as the variations of source fingerprints, and provides a credible source apportionment. Major PAH sources for Illinois River sediments are traffic (35%), coke oven (24%), coal combustion (18%), and wood combustion (14%). Copyright © 2015. Published by Elsevier Ltd.

  18. Wood burning pollution in southern Chile: PM2.5 source apportionment using CMB and molecular markers.

    PubMed

    Villalobos, Ana M; Barraza, Francisco; Jorquera, Héctor; Schauer, James J

    2017-06-01

    Temuco is a mid-size city representative of severe wood smoke pollution in southern Chile; i.e., ambient 24-h PM2.5 concentrations have exceeded 150 μg/m(3) in the winter season and the top concentration reached 372 μg/m(3) in 2010. Annual mean concentrations have decreased but are still above 30 μg/m(3). For the very first time, a molecular marker source apportionment of ambient organic carbon (OC) and PM2.5 was conducted in Temuco. Primary resolved sources for PM2.5 were wood smoke (37.5%), coal combustion (4.4%), diesel vehicles (3.3%), dust (2.2%) and vegetative detritus (0.7%). Secondary inorganic PM2.5 (sulfates, nitrates and ammonium) contributed 4.8% and unresolved organic aerosols (generated from volatile emissions from incomplete wood combustion), including secondary organic aerosols, contributed 47.1%. Adding the contributions of unresolved organic aerosols to those from primary wood smoke implies that wood burning is responsible for 84.6% of the ambient PM2.5 in Temuco. This predominance of wood smoke is ultimately due to widespread poverty and a lack of efficient household heating methods. The government has been implementing emission abatement policies but achieving compliance with ambient air quality standards for PM2.5 in southern Chile remains a challenge. Copyright © 2017 Elsevier Ltd. All rights reserved.

  19. Apportionment of sources of fine and coarse particles in four major Australian cities by positive matrix factorisation

    NASA Astrophysics Data System (ADS)

    Chan, Yiu-Chung; Cohen, David D.; Hawas, Olga; Stelcer, Eduard; Simpson, Rod; Denison, Lyn; Wong, Neil; Hodge, Mary; Comino, Eva; Carswell, Stewart

    In this study, 437 days of 6-daily, 24-h samples of PM 2.5, PM 2.5-10 and PM 10 were collected over a 12-month period during 2003-2004 in Melbourne, Sydney, Brisbane and Adelaide. The elemental, ionic and polycyclic aromatic hydrocarbon composition of the particles were determined. Source apportionment was carried out by using the positive matrix factorisation software (PMF2). Eight factors were identified for the fine particle samples including 'motor vehicles', 'industry', 'other combustion sources', 'ammonium sulphates', 'nitrates', 'marine aerosols', 'chloride depleted marine aerosols' and 'crustal/soil dust'. On average combustion sources, secondary nitrates/sulphates and natural origin dust contributed about 46%, 25% and 26% of the mass of the fine particle samples, respectively. 'Crustal/soil dust', 'marine aerosols', 'nitrates' and 'road side dust' were the four factors identified for the coarse particle samples. On average natural origin dust contributed about 76% of the mass of the coarse particle samples. The contributions of the sources to the sample mass basically reflect the emission source characteristics of the sites. Secondary sulphates and nitrates were found to spread out evenly within each city. The average contribution of secondary nitrates to fine particles was found to be rather uniform in different seasons, rather than higher in winter as found in other studies. This could be due to the low humidity conditions in winter in most of the Australian cities which made the partitioning of the particle phase less favourable in the NH 4NO 3 equilibrium system. A linear relationship was found between the average contribution of marine aerosols and the distance of the site from the bay side. Wind erosion was found associated with higher contribution of crustal dust on average and episodes of elevated concentration of coarse particles in spring and summer.

  20. Concentrations and source apportionment of PM10 and associated major and trace elements in the Rhodes Island, Greece.

    PubMed

    Argyropoulos, Georgios; Manoli, Evangelia; Kouras, Athanasios; Samara, Constantini

    2012-08-15

    Ambient concentrations of PM(10) and associated major and trace elements were measured over the cold and the warm season of 2007 at two sites located in the Rhodes Island (Greece), in Eastern Mediterranean, aimed at source apportionment by Chemical Mass Balance (CMB) receptor modeling. Source chemical profiles, necessary in CMB modeling, were obtained for a variety of emission sources that could possibly affect the study area, including sea spray, geological material, soot emissions from the nearby oil-fuelled thermal power plant, and other anthropogenic activities, such as vehicular traffic, residential oil combustion, wood burning, and uncontrolled open-air burning of agricultural biomass and municipal waste. Source apportionment of PM(10) and elemental components was carried out by employing an advanced CMB version, the Robotic Chemical Mass Balance model (RCMB). Vehicular emissions were found to be major PM(10) contributor accounting, on average, for 36.8% and 31.7% during the cold period, and for 40.9% and 39.2% in the warm period at the two sites, respectively. The second largest source of ambient PM(10), with minor seasonal variation, was secondary sulfates (mainly ammonium and calcium sulfates), with total average contribution around 16.5% and 18% at the two sites. Soil dust was also a remarkable source contributing around 22% in the warm period, whereas only around 10% in the cold season. Soot emitted from the thermal power plant was found to be negligible contributor to ambient PM(10) (<1%), however it appeared to appreciably contribute to the ambient V and Ni (11.3% and 5.1%, respectively) at one of the sites during the warm period, when electricity production is intensified. Trajectory analysis did not indicate any transport of Sahara dust; on the contrary, long range transport of soil dust from arid continental regions of Minor Asia and of biomass burning aerosol from the countries surrounding the Black Sea was considered possible.

  1. Source apportionment of black carbon in PM2.5 in China and its implications on estimation of direct radiative forcing

    NASA Astrophysics Data System (ADS)

    Du, K.; Deng, J.; Chen, B.; Gustafsson, O.; Andersson, A.-; Lee, M.; Kirillova, E. N.; Kruså, M.

    2012-12-01

    Chinese black carbon (BC) causes concerns for climate warming and air pollution, yet the emission sources of black carbon are in large uncertainty. Emission inventory models suggest that fossil fuel and biomass/biofuel burning are the primary contributors to atmospheric BC. In this study, top-down sourcing of Chinese BC was conducted to quantify the apportionment between bio- and fossil- based fuel burning using radiocarbon method. Results for black carbon aerosols collected at urban and regional receptor areas showed that 81±5% of Chinese BC were produced from fossil fuel combustion, contrasting with the results from emission inventories, which report 50-70% of BC were from fossil fuel combustion. Since fossil BC aerosols are perceived as stronger climate forcers than biomass BC aerosols, accurate understanding of BC apportionment would be essential to improve modeling of climate effect of BC. A simulation on BC's radiative forcing effect was carried out by differentiating the sources using the top-down approach. Preliminary modeling results are presented.

  2. Weak acid extractable metals in Bramble Bay, Queensland, Australia: temporal behaviour, enrichment and source apportionment.

    PubMed

    Brady, James P; Ayoko, Godwin A; Martens, Wayde N; Goonetilleke, Ashantha

    2015-02-15

    Sediment samples were taken from six sampling sites in Bramble Bay, Queensland, Australia between February and November in 2012. They were analysed for a range of heavy metals including Al, Fe, Mn, Ti, Ce, Th, U, V, Cr, Co, Ni, Cu, Zn, As, Cd, Sb, Te, Hg, Tl and Pb. Fraction analysis, Enrichment Factors and Principal Component Analysis-Absolute Principal Component Scores (PCA-APCS) were carried out in order to assess metal pollution, potential bioavailability and source apportionment. Cr and Ni exceeded the Australian Interim Sediment Quality Guidelines at some sampling sites, while Hg was found to be the most enriched metal. Fraction analysis identified increased weak acid soluble Hg and Cd during the sampling period. Source apportionment via PCA-APCS found four sources of metals pollution, namely, marine sediments, shipping, antifouling coatings and a mixed source. These sources need to be considered in any metal pollution control measure within Bramble Bay. Copyright © 2014 Elsevier Ltd. All rights reserved.

  3. Workgroup Report: Workshop on Source Apportionment of Particulate Matter Health Effects—Intercomparison of Results and Implications

    PubMed Central

    Thurston, George D.; Ito, Kazuhiko; Mar, Therese; Christensen, William F.; Eatough, Delbert J.; Henry, Ronald C.; Kim, Eugene; Laden, Francine; Lall, Ramona; Larson, Timothy V.; Liu, Hao; Neas, Lucas; Pinto, Joseph; Stölzel, Matthias; Suh, Helen; Hopke, Philip K.

    2005-01-01

    Although the association between exposure to ambient fine particulate matter with aerodynamic diameter < 2.5 μm (PM2.5) and human mortality is well established, the most responsible particle types/sources are not yet certain. In May 2003, the U.S. Environmental Protection Agency’s Particulate Matter Centers Program sponsored the Workshop on the Source Apportionment of PM Health Effects. The goal was to evaluate the consistency of the various source apportionment methods in assessing source contributions to daily PM2.5 mass–mortality associations. Seven research institutions, using varying methods, participated in the estimation of source apportionments of PM2.5 mass samples collected in Washington, DC, and Phoenix, Arizona, USA. Apportionments were evaluated for their respective associations with mortality using Poisson regressions, allowing a comparative assessment of the extent to which variations in the apportionments contributed to variability in the source-specific mortality results. The various research groups generally identified the same major source types, each with similar elemental makeups. Intergroup correlation analyses indicated that soil-, sulfate-, residual oil-, and salt-associated mass were most unambiguously identified by various methods, whereas vegetative burning and traffic were less consistent. Aggregate source-specific mortality relative risk (RR) estimate confidence intervals overlapped each other, but the sulfate-related PM2.5 component was most consistently significant across analyses in these cities. Analyses indicated that source types were a significant predictor of RR, whereas apportionment group differences were not. Variations in the source apportionments added only some 15% to the mortality regression uncertainties. These results provide supportive evidence that existing PM2.5 source apportionment methods can be used to derive reliable insights into the source components that contribute to PM2.5 health effects. PMID:16330361

  4. Sources and components of organic aerosols in Central Europe

    NASA Astrophysics Data System (ADS)

    Lanz, V. A.; Prévôt, A. S. H.; Alfarra, M. R.; Hüglin, C.; Mohr, C.; Weimer, S.; Baltensperger, U.

    2009-04-01

    The quadrupole version of the Aerodyne Aerosol Mass Spectrometer (q-AMS) was deployed at several places in Switzerland, Austria, and Liechtenstein. The q-AMS provides real-time information on mass concentration and composition of the non-refractory species in particulate matter smaller than 1 µm (NR-PM1) with high time- and size-resolution at unit mass resolution. The combination of factor analysis and ambient AMS data represents a relatively new approach to identify organic aerosol (OA) sources/components (Zhang et al., 2005). In this study, such an approach (PMF - positive matrix factorization; Lanz et al., 2007, 2008) was applied to various OA data sets covering a wide range of pollution levels (mobile measurements on motorways, urban, rural, and even a high-alpine location) as well as all seasons of the year. Dominating aerosol components were representing oxygenated and secondary organic aerosol (OOA-I and OOA-II), primary particles from wood burning (P-BBOA; especially in residential areas in wintertime with abundances of ~50% OA and more) and primary traffic-related aerosols (usually ~10% of OA, but up to 60% on motorways). Close to sources, charbroiling and potentially food cooking aerosols could be distinguished as well. The OOAs' time series were compared to measurements of AMS inorganics (sulphate, nitrate, and ammonium) in order to facilitate their interpretation as secondary OA (SOA). Diurnal cycles of the estimated source strengths, ancillary gas-phase and meteorological data, estimated emission ratios etc. were also used to validate the interpretations of the factor analytical results. Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B., Hueglin, C., and Prévôt, A. S. H.: Source apportionment of submicron organic aerosols at an urban site by factor analytical modelling of aerosol mass spectra, Atmos. Chem. Phys., 7, 1503-1522, 2007, http://www.atmos-chem-phys.net/7/1503/2007/. Lanz, V. A., Alfarra, M. R., Baltensperger, U., Buchmann, B

  5. Single source impacts estimated with photochemical model source sensitivity and apportionment approaches

    NASA Astrophysics Data System (ADS)

    Baker, Kirk R.; Kelly, James T.

    2014-10-01

    Some sources may need to estimate ozone and secondarily formed PM2.5 as part of the permit application process under the Clean Air Act New Source Review program. Photochemical grid models represent state-of-the-science gas- and particle-phase chemistry and provide a realistic chemical and physical environment for assessing changes in air quality resulting from changes in emissions. When using these tools for single source impact assessments, it is important to differentiate a single source impact from other emissions sources and to understand how well contemporary grid model applications capture near-source transport and chemistry. Here for the first time, both source apportionment and source sensitivity approaches (brute-force changes and high-order direct decoupled method) are used in a photochemical grid model to isolate impacts of a specific facility. These single source impacts are compared with in-plume measurements made as part of a well-characterized 1999 TVA Cumberland aircraft plume transect field study. The techniques were able to isolate the impacts of the TVA plume in a manner consistent with observations. The model predicted in-plume concentrations well when the observations were averaged to the grid scale, although peak concentrations of primary pollutants were generally underestimated near the source, possibly due to dilution in the 4-km grid cell.

  6. Evaluation of Organic Aerosol Formation and Apportionment in a polluted Megacity

    NASA Astrophysics Data System (ADS)

    Tsimpidi, A. P.; Karydis, V. A.; Zavala, M.; Lei, W.; Decarlo, P. F.; Ulbrich, I.; Jimenez, J. L.; Molina, L. T.; Pandis, S. N.

    2009-04-01

    Pollution from megacities and large urban areas is important not only for local effects on health, visibility, and ecosystems but also because of their collective influence on atmospheric chemistry and radiative forcing in regional and global scale. Organic species account for a large fraction of the submicron aerosol mass at most megacities. Urban areas are large sources of organic aerosols and their precursors. Nevertheless, the contributions of primary (POA) and secondary organic aerosol (SOA) have been difficult to quantify. In this study, new primary and secondary organic aerosol modules were added to PMCAMx, a three dimensional chemical transport model (Gaydos et al., 2007). The new modeling framework is based on the volatility basis-set approach (Lane et al., 2007): both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. The emission inventory is modified and the POA emissions are distributed by volatility based on dilution experiments (Robinson et al., 2007). PMCAMx is applied in the Mexico City Metropolitan Area during April 2003 and March 2006. The model predictions are compared with Aerodyne's Aerosol Mass Spectrometer (AMS) observations from the MCMA and MILAGRO campaigns respectively. Furthermore, the predicted concentrations over Mexico City are compared against measurements from a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) which was onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign (DeCarlo et al., 2008). The organic aerosol (OA) to CO ratio is used as an indicator in order to evaluate the photo-oxidation of the predicted OA after its horizontal and vertical advection. References Gaydos, T.M.; Pinder, R.W.; Koo, B.; Fahey, K.M.; Pandis, S.N., 2007. Development and application of a three-dimensional aerosol chemical transport model, PMCAMx. Atmospheric Environment 41, 2594-2611. Lane, T

  7. The qualitative and quantitative source apportionments of polycyclic aromatic hydrocarbons in size dependent road deposited sediment.

    PubMed

    Zhang, Jin; Wang, Jing; Hua, Pei; Krebs, Peter

    2015-02-01

    This study showcases the qualitative and quantitative source apportionments of size-dependent polycyclic aromatic hydrocarbons (PAHs) in road deposited sediment by means of molecular diagnostic ratio (MDR) and positive matrix factorisation (PMF) approaches. The MDR was initially used to narrow the PAH source candidates. PMF modelling was subsequently used to provide more precise source apportionment with the assistance of a multiple linear regression analysis. Through a combined qualitative and quantitative source apportionment, different potential source contributors were identified at different size fractions. Explicitly, three major contributors to sorption at the size fraction of 1000-400 μm were tentatively identified as incineration (26%), coal combustion (53%) and gasoline-powered vehicle (20%). Four major contributors to the size fraction of 400-100 μm were identified as gasoline-powered vehicle (25%), surface pavement (15%), diesel-powered vehicle (37%) and industrial boiler (24%). Four major contributors to the size fraction of 100-63 μm were identified as cogeneration emission (13%), diesel-powered vehicle (28%), tire debris (45%) and wood combustion (14%). The potential contributors in the size fraction 63-0.45 μm were identified as diesel-powered vehicle (21%), heterogeneous sources (41%) and biomass burning (38%). In addition, the highest ∑16PAH concentration was found in the smallest size fraction of 63-0.45 μm, which is also where the highest BaPE and TEF values for potential risk assessment occurred.

  8. Advanced source apportionment of size-resolved trace elements at multiple sites in London during winter

    NASA Astrophysics Data System (ADS)

    Visser, S.; Slowik, J. G.; Furger, M.; Zotter, P.; Bukowiecki, N.; Canonaco, F.; Flechsig, U.; Appel, K.; Green, D. C.; Tremper, A. H.; Young, D. E.; Williams, P. I.; Allan, J. D.; Coe, H.; Williams, L. R.; Mohr, C.; Xu, L.; Ng, N. L.; Nemitz, E.; Barlow, J. F.; Halios, C. H.; Fleming, Z. L.; Baltensperger, U.; Prévôt, A. S. H.

    2015-10-01

    Trace element measurements in PM10-2.5, PM2.5-1.0 and PM1.0-0.3 aerosol were performed with 2 h time resolution at kerbside, urban background and rural sites during the ClearfLo winter 2012 campaign in London. The environment-dependent variability of emissions was characterized using the Multilinear Engine implementation of the positive matrix factorization model, conducted on data sets comprising all three sites but segregated by size. Combining the sites enabled separation of sources with high temporal covariance but significant spatial variability. Separation of sizes improved source resolution by preventing sources occurring in only a single size fraction from having too small a contribution for the model to resolve. Anchor profiles were retrieved internally by analysing data subsets, and these profiles were used in the analyses of the complete data sets of all sites for enhanced source apportionment. A total of nine different factors were resolved (notable elements in brackets): in PM10-2.5, brake wear (Cu, Zr, Sb, Ba), other traffic-related (Fe), resuspended dust (Si, Ca), sea/road salt (Cl), aged sea salt (Na, Mg) and industrial (Cr, Ni); in PM2.5-1.0, brake wear, other traffic-related, resuspended dust, sea/road salt, aged sea salt and S-rich (S); and in PM1.0-0.3, traffic-related (Fe, Cu, Zr, Sb, Ba), resuspended dust, sea/road salt, aged sea salt, reacted Cl (Cl), S-rich and solid fuel (K, Pb). Human activities enhance the kerb-to-rural concentration gradients of coarse aged sea salt, typically considered to have a natural source, by 1.7-2.2. These site-dependent concentration differences reflect the effect of local resuspension processes in London. The anthropogenically influenced factors traffic (brake wear and other traffic-related processes), dust and sea/road salt provide further kerb-to-rural concentration enhancements by direct source emissions by a factor of 3.5-12.7. The traffic and dust factors are mainly emitted in PM10-2.5 and show strong

  9. Concentration, sources, and degradation of organic aerosol at Summit, Greenland

    NASA Astrophysics Data System (ADS)

    von Schneidemesser, Erika

    Characterization and understanding of the carbonaceous portion of the aerosol in the Arctic is limited. The objective of the research presented in this thesis was to improve the scope of knowledge pertaining to carbonaceous aerosols, in terms of atmospheric and snow concentrations, sources, and post-depositional processing. An extraction technique was developed to quantitatively identify a suite of organic compounds, typically observed in aerosol samples, at trace level concentrations in snow melt water samples. A field campaign of sampling and exposure experiments was carried out at Summit, Greenland. A 3-meter snow pit, sampled at 20 cm intervals, was analyzed for organic compounds and total organic carbon (TOC). The average concentration of TOC for the entire pit was 64 mug C kg-1. The quantified organic compounds comprised 6 to 24% of TOC throughout the layers. Median concentrations of the water insoluble individual organic compounds ranged from 0.14 ng kg-1 (hopane) to 2200 ng kg-1 (alkanoic acid) at any one depth. High-volume aerosol samples were collected over a six month period and analyzed for organics. Median concentrations ranged from 0.00045 ng kg-1 (hopane) to 0.23 ng kg-1 (levoglucosan) in the air samples. Source apportionment results from the aerosol samples indicate anthropogenic influence at Summit from biomass burning, fossil fuels, and vegetative detritus. The majority (>90%) of the organic carbon in the aerosol was estimated to be secondary organic aerosol. To investigate the post-depositional processing of organic compounds in snow, contaminant labeled snow was produced and exposed for up to 72 hours on the surface of the Greenland ice sheet at Summit. Degradation of alkanes, acids, and PAHs to a threshold concentration was observed. The threshold concentration, at which no further degradation was observed, ranged from 10 to 60% of the original (non-exposed) snow concentrations, depending on the reaction rate. This would indicate that a

  10. Preliminary Results of the first European Source Apportionment intercomparison for Receptor and Chemical Transport Models

    NASA Astrophysics Data System (ADS)

    Belis, Claudio A.; Pernigotti, Denise; Pirovano, Guido

    2017-04-01

    Source Apportionment (SA) is the identification of ambient air pollution sources and the quantification of their contribution to pollution levels. This task can be accomplished using different approaches: chemical transport models and receptor models. Receptor models are derived from measurements and therefore are considered as a reference for primary sources urban background levels. Chemical transport model have better estimation of the secondary pollutants (inorganic) and are capable to provide gridded results with high time resolution. Assessing the performance of SA model results is essential to guarantee reliable information on source contributions to be used for the reporting to the Commission and in the development of pollution abatement strategies. This is the first intercomparison ever designed to test both receptor oriented models (or receptor models) and chemical transport models (or source oriented models) using a comprehensive method based on model quality indicators and pre-established criteria. The target pollutant of this exercise, organised in the frame of FAIRMODE WG 3, is PM10. Both receptor models and chemical transport models present good performances when evaluated against their respective references. Both types of models demonstrate quite satisfactory capabilities to estimate the yearly source contributions while the estimation of the source contributions at the daily level (time series) is more critical. Chemical transport models showed a tendency to underestimate the contribution of some single sources when compared to receptor models. For receptor models the most critical source category is industry. This is probably due to the variety of single sources with different characteristics that belong to this category. Dust is the most problematic source for Chemical Transport Models, likely due to the poor information about this kind of source in the emission inventories, particularly concerning road dust re-suspension, and consequently the

  11. Impact of gas/particle partitioning of semivolatile organic compounds on source apportionment with positive matrix factorization.

    PubMed

    Xie, Mingjie; Hannigan, Michael P; Barsanti, Kelley C

    2014-08-19

    To quantify and minimize the influence of gas/particle (G/P) partitioning on receptor-based source apportionment using particle-phase semivolatile organic compound (SVOC) data, positive matrix factorization (PMF) coupled with a bootstrap technique was applied to three data sets mainly composed of "measured-total" (measured particle- + gas-phase), "particle-only" (measured particle-phase) and "predicted-total" (measured particle-phase + predicted gas-phase) SVOCs to apportion carbonaceous aerosols. Particle- (PM2.5) and gas-phase SVOCs were collected using quartz fiber filters followed by PUF/XAD-4/PUF adsorbents and measured using gas chromatography-mass spectrometry (GC-MS). Concentrations of gas-phase SVOCs were also predicted from their particle-phase concentrations using absorptive partitioning theory. Five factors were resolved for each data set, and the factor profiles were generally consistent across the three PMF solutions. Using a previous source apportionment study at the same receptor site, those five factors were linked to summertime biogenic emissions (odd n-alkane factor), unburned fossil fuels (light SVOC factor), road dust and/or cooking (n-alkane factor), motor vehicle emissions (PAH factor), and lubricating oil combustion (sterane factor). The "measured-total" solution was least influenced by G/P partitioning and used as reference. Two out of the five factors (odd n-alkane and PAH factors) exhibited consistent contributions for "particle-only" vs "measured-total" and "predicted-total" vs "measured-total" solutions. Factor contributions of light SVOC and n-alkane factors were more consistent for "predicted-total" vs "measured-total" than "particle-only" vs "measured-total" solutions. The remaining factor (sterane factor) underestimated the contribution by around 50% from both "particle-only" and "predicted-total" solutions. The results of this study confirm that when measured gas-phase SVOCs are not available, "predicted-total" SVOCs should be used

  12. Source apportionment of atmospheric aliphatic and polycyclic aromatic hydrocarbons using compound-specific radiocarbon analysis

    NASA Astrophysics Data System (ADS)

    Gustafsson, Ö.; Mandalakis, M.; Zencak, Z.; Sheesley, R.; Kruså, M.

    2009-04-01

    Recent development in compound-specific radiocarbon analysis (CSRA) now allows application of this analytical dimension toward source apportionment of natural and anthropogenic compounds in the atmosphere. CSRA studies of semi-volatile n-alkanes and polycyclic aromatic hydrocarbons (PAHs) in air collected at various locations throughout Europe combine to reveal both inter-compound, inter-regional and inter-seasonal variations in sources. For instance, modern biogenic sources contribute a significant portion (frequently up to 50%) of the atmospheric load of priority pollutant PAHs and long-chained n-alkanes, suggesting that such sources should be scrutinized for effective reduction.

  13. Size-resolved source apportionment of carbonaceous particulate matter in urban and rural sites in central California

    NASA Astrophysics Data System (ADS)

    Ham, Walter A.; Kleeman, Michael J.

    2011-08-01

    Very little is currently known about the relationship between exposure to different sources of ambient ultrafine particles (PM 0.1) and human health effects. If human health effects are enhanced by PM 0.1's ability to cross cell membranes, then more information is needed describing the sources of ultrafine particles that are deposited in the human respiratory system. The current study presents results for the source apportionment of airborne particulate matter in six size fractions smaller than 1.8 μm particle diameter including ultrafine particles (PM 0.1) in one of the most polluted air basins in the United States. Size-resolved source apportionment results are presented at an urban site and rural site in central California's heavily polluted San Joaquin Valley during the winter and summer months using a molecular marker chemical mass balance (MM-CMB) method. Respiratory deposition calculations for the size-resolved source apportionment results are carried out with the Multiple Path Particle Dosimetry Model ( MPPD v 2.0), including calculations for ultrafine (PM 0.1) source deposition. Diesel engines accounted for the majority of PM 0.1 and PM 1.8 EC at both the urban and rural sampling locations during both summer and winter seasons. Meat cooking accounted for 33-67% and diesel engines accounted for 15-21% of the PM 0.1 OC at Fresno. Meat cooking accounted for 22-26% of the PM 0.1 OC at the rural Westside location, while diesel engines accounted for 8-9%. Wood burning contributions to PM 0.1 OC increased to as much as 12% of PM 0.1 OC during the wintertime. The modest contribution of wood smoke reflects the success of emissions control programs over the past decade. In contrast to PM 0.1, PM 1.8 OC had a higher fraction of unidentified source contributions (68-85%) suggesting that this material is composed of secondary organic aerosol (SOA) or primary organic aerosol (POA) that has been processed by atmospheric chemical reactions. Meat cooking was the largest

  14. Source apportionment of fine particulate matter in the southeastern United States

    SciTech Connect

    Sangil Lee; Armistead G. Russell; Karsten Baumann

    2007-09-15

    Particulate matter (PM) less than 2.5 {mu}m in size (PM2.5) source apportionment by chemical mass balance receptor modeling was performed to enhance regional characterization of source impacts in the southeastern United States. Secondary particles, such as NH{sub 4}HSO{sub 4}, (NH{sub 4}){sub 2}SO{sub 4}, NH{sub 4}NO{sub 3}, and secondary organic carbon (OC) (SOC), formed by atmospheric photochemical reactions, contribute the majority ({gt} 50%) of ambient PM2.5 with strong seasonality. Source apportionment results indicate that motor vehicle and biomass burning are the two main primary sources in the southeast, showing relatively more motor vehicle source impacts rather than biomass burning source impacts in populated urban areas and vice versa in less urbanized areas. Spatial distributions of primary source impacts show that each primary source has distinctively different spatial source impacts. For coal combustion, higher concentrations occur in areas close to source and are highest at Jefferson (Birmingham), AL where industrial facilities use coal for fuel. Pulp and paper mills contribute high sources along the coast where oil combustion contribution is also high. Results also find impacts from shipping activities along the coast. Spatiotemporal correlations indicate that secondary particles are more regionally distributed, as are biomass burning and dust, whereas impacts of other primary sources are more local. 60 refs., 7 figs., 1 tab.

  15. Sediment source apportionment in Laurel Hill Creek, PA, using Bayesian chemical mass balance and isotope fingerprinting

    USGS Publications Warehouse

    Stewart, Heather; Massoudieh, Arash; Gellis, Allen C.

    2015-01-01

    A Bayesian chemical mass balance (CMB) approach was used to assess the contribution of potential sources for fluvial samples from Laurel Hill Creek in southwest Pennsylvania. The Bayesian approach provides joint probability density functions of the sources' contributions considering the uncertainties due to source and fluvial sample heterogeneity and measurement error. Both elemental profiles of sources and fluvial samples and 13C and 15N isotopes were used for source apportionment. The sources considered include stream bank erosion, forest, roads and agriculture (pasture and cropland). Agriculture was found to have the largest contribution, followed by stream bank erosion. Also, road erosion was found to have a significant contribution in three of the samples collected during lower-intensity rain events. The source apportionment was performed with and without isotopes. The results were largely consistent; however, the use of isotopes was found to slightly increase the uncertainty in most of the cases. The correlation analysis between the contributions of sources shows strong correlations between stream bank and agriculture, whereas roads and forest seem to be less correlated to other sources. Thus, the method was better able to estimate road and forest contributions independently. The hypothesis that the contributions of sources are not seasonally changing was tested by assuming that all ten fluvial samples had the same source contributions. This hypothesis was rejected, demonstrating a significant seasonal variation in the sources of sediments in the stream.

  16. Spallation Neutron Source Availability Top-Down Apportionment Using Characteristic Factors and Expert Opinion

    SciTech Connect

    Haire, M.J.; Schryver, J.C.

    1999-10-01

    Apportionment is the assignment of top-level requirements to lower tier elements of the overall facility. A method for apportioning overall facility availability requirements among systems and subsystems is presented. Characteristics that influence equipment reliability and maintainability are discussed. Experts, using engineering judgment, scored each characteristic for each system whose availability design goal is to be established. The Analytic Hierarchy Process (AHP) method is used to produce a set of weighted rankings for each characteristic for each alternative system. A mathematical model is derived which incorporates these weighting factors. The method imposes higher availability requirements on those systems in which an incremental increase in availability is easier to achieve, and lower availability requirements where greater availability is more difficult and costly. An example is given of applying this top-down apportionment methodology to the Spallation Neutron Source (SNS) facility.

  17. Source apportionment of airborne fine particulate matter in an underground mine.

    PubMed

    McDonald, Jacob D; Zielinska, Barbara; Sagebiel, John C; McDaniel, Mark R; Mousset-Jones, Pierre

    2003-04-01

    The chemical mass balance source apportionment technique was applied to an underground gold mine to assess the contribution of diesel exhaust, rock dust, oil mists, and cigarette smoke to airborne fine (<2.5 microm) particulate matter (PM). Apportionments were conducted in two locations in the mine, one near the mining operations and one near the exit of the mine where the ventilated mine air was exhausted. Results showed that diesel exhaust contributed 78-98% of the fine particulate mass and greater than 90% of the fine particle carbon, with rock dust making up the remainder. Oil mists and cigarette smoke contributions were below detection limits for this study. The diesel exhaust fraction of the total fine PM was higher than the recently implemented mine air quality standards based on total carbon at both sample locations in the mine.

  18. Source contributions and spatiotemporal characteristics of PAHs in sediments: Using three-way source apportionment approach.

    PubMed

    Tian, Ying-Ze; Shi, Guo-Liang; Liu, Gui-Rong; Guo, Chang-Sheng; Peng, Xing; Xu, Jian; Zhang, Yuan; Feng, Yin-Chang

    2014-08-01

    Polycyclic aromatic hydrocarbon (PAHs) were measured in sediments from 29 sites throughout Taihu Lake in China during 2 seasons to investigate spatiotemporal characteristics and source contributions using a 3-way source apportionment approach to positive matrix factorization (PMF3). Seasonal and spatial variations of levels and toxicity suggested higher individual carcinogenic PAH concentrations and toxic equivalent quantity (TEQ) in the flooding season. Three-way PAHs dataset (PAH species, spatial variability, and seasonal variability) was analyzed by PMF3, and its results were compared with a widely used 2-way model (PMF2). Consistent results were observed: vehicular emission was the most important contributor (67.08% by PMF2 and 61.83% by PMF3 for the flooding season; 54.21% by PMF2 and 52.94% by PMF3 for dry season), followed by coal combustion and wood combustion in both seasons. The PMF-cluster analysis was employed to investigate spatial variability of source contributions. Findings can introduce the 3-way approach to apportion sources of PAHs and other persistent organic pollutants (POPs) in sediments, offering the advantage of accounting for information on 3-way datasets.

  19. Application of a source apportionment model in consideration of volatile organic compounds in an urban stream

    USGS Publications Warehouse

    Asher, W.E.; Luo, W.; Campo, K.W.; Bender, D.A.; Robinson, K.W.; Zogorski, J.S.; Pankow, J.F.

    2007-01-01

    Position-dependent concentrations of trichloroethylene and methyl-tert-butyl ether are considered for a 2.81-km section of the Aberjona River in Massachusetts, USA. This river flows through Woburn and Winchester (Massachusetts, USA), an area that is highly urbanized, has a long history of industrial activities dating to the early 1800s, and has gained national attention because of contamination from chlorinated solvent compounds in Woburn wells G and H. The river study section is in Winchester and begins approximately five stream kilometers downstream from the Woburn wells superfund site. Approximately 300 toxic release sites are documented in the watershed upstream from the terminus of the study section. The inflow to the river study section is considered one source of contamination. Other sources are the atmosphere, a tributary flow, and groundwater flows entering the river; the latter are categorized according to stream zone (1, 2, 3, etc.). Loss processes considered include outflows to groundwater and water-to-atmosphere transfer of volatile compounds. For both trichloroethylene and methyl-rerf-butyl ether, degradation is neglected over the timescale of interest. Source apportionment fractions with assigned values ??inflow, ??1, ??2, ??3, etc. are tracked by a source apportionment model. The strengths of the groundwater and tributary sources serve as fitting parameters when minimizing a reduced least squares statistic between water concentrations measured during a synoptic study in July 2001 versus predictions from the model. The model fits provide strong evidence of substantial unknown groundwater sources of trichloroethylene and methyl-tert-butyl ether amounting to tens of grams per day of trichloroethylene and methyl-tert-butyl ether in the river along the study section. Modeling in a source apportionment manner can be useful to water quality managers allocating limited resources for remediation and source control. ?? 2007 SETAC.

  20. Microbial water pollution: a screening tool for initial catchment-scale assessment and source apportionment.

    PubMed

    Kay, D; Anthony, S; Crowther, J; Chambers, B J; Nicholson, F A; Chadwick, D; Stapleton, C M; Wyer, M D

    2010-11-01

    The European Union Water Framework Directive requires that Management Plans are developed for individual River Basin Districts. From the point of view of faecal indicator organisms (FIOs), there is a critical need for screening tools that can provide a rapid assessment of the likely FIO concentrations and fluxes within catchments under base- and high-flow conditions, and of the balance ('source apportionment') between agriculture- and sewage-derived sources. Accordingly, the present paper reports on: (1) the development of preliminary generic models, using water quality and land cover data from previous UK catchment studies for assessing FIO concentrations, fluxes and source apportionment within catchments during the summer bathing season; (2) the calibration of national land use data, against data previously used in the models; and (3) provisional FIO concentration and source-apportionment assessments for England and Wales. The models clearly highlighted the crucial importance of high-flow conditions for the flux of FIOs within catchments. At high flow, improved grassland (and associated livestock) was the key FIO source; FIO loadings derived from catchments with high proportions of improved grassland were shown to be as high as from urbanized catchments; and in many rural catchments, especially in NW and SW England and Wales, which are important areas of lowland livestock (especially dairy) farming, ≥ 40% of FIOs was assessed to be derived from agricultural sources. In contrast, under base-flow conditions, when there was little or no runoff from agricultural land, urban (i.e. sewerage-related) sources were assessed to dominate, and even in rural areas the majority of FIOs were attributed to urban sources. The results of the study demonstrate the potential of this type of approach, particularly in light of climate change and the likelihood of more high-flow events, in underpinning informed policy development and prioritization of investment.

  1. Fine Particle Sources and Cardiorespiratory Morbidity: An Application of Chemical Mass Balance and Factor Analytical Source-Apportionment Methods

    PubMed Central

    Sarnat, Jeremy A.; Marmur, Amit; Klein, Mitchel; Kim, Eugene; Russell, Armistead G.; Sarnat, Stefanie E.; Mulholland, James A.; Hopke, Philip K.; Tolbert, Paige E.

    2008-01-01

    Background Interest in the health effects of particulate matter (PM) has focused on identifying sources of PM, including biomass burning, power plants, and gasoline and diesel emissions that may be associated with adverse health risks. Few epidemiologic studies, however, have included source-apportionment estimates in their examinations of PM health effects. We analyzed a time-series of chemically speciated PM measurements in Atlanta, Georgia, and conducted an epidemiologic analysis using data from three distinct source-apportionment methods. Objective The key objective of this analysis was to compare epidemiologic findings generated using both factor analysis and mass balance source-apportionment methods. Methods We analyzed data collected between November 1998 and December 2002 using positive-matrix factorization (PMF), modified chemical mass balance (CMB-LGO), and a tracer approach. Emergency department (ED) visits for a combined cardiovascular (CVD) and respiratory disease (RD) group were assessed as end points. We estimated the risk ratio (RR) associated with same day PM concentrations using Poisson generalized linear models. Results There were significant, positive associations between same-day PM2.5 (PM with aero-dynamic diameter ≤ 2.5 μm) concentrations attributed to mobile sources (RR range, 1.018–1.025) and biomass combustion, primarily prescribed forest burning and residential wood combustion, (RR range, 1.024–1.033) source categories and CVD-related ED visits. Associations between the source categories and RD visits were not significant for all models except sulfate-rich secondary PM2.5 (RR range, 1.012–1.020). Generally, the epidemiologic results were robust to the selection of source-apportionment method, with strong agreement between the RR estimates from the PMF and CMB-LGO models, as well as with results from models using single-species tracers as surrogates of the source-apportioned PM2.5 values. Conclusions Despite differences among the

  2. Temporal trend and source apportionment of water pollution in different functional zones of Qiantang River, China.

    PubMed

    Su, Shiliang; Li, Dan; Zhang, Qi; Xiao, Rui; Huang, Fang; Wu, Jiaping

    2011-02-01

    The increasingly serious river water pollution in developing countries poses great threat to environmental health and human welfare. The assignment of river function to specific uses, known as zoning, is a useful tool to reveal variations of water environmental adaptability to human impact. Therefore, characterizing the temporal trend and identifying responsible pollution sources in different functional zones could greatly improve our knowledge about human impacts on the river water environment. The aim of this study is to obtain a deeper understanding of temporal trends and sources of water pollution in different functional zones with a case study of the Qiantang River, China. Measurement data were obtained and pretreated for 13 variables from 41 monitoring sites in four categories of functional zones during the period 1996-2004. An exploratory approach, which combines smoothing and non-parametric statistical tests, was applied to characterize trends of four significant parameters (permanganate index, ammonia nitrogen, total cadmium and fluoride) accounting for differences among different functional zones identified by discriminant analysis. Aided by GIS, yearly pollution index (PI) for each monitoring site was further mapped to compare the within-group variations in temporal dynamics for different functional zones. Rotated principal component analysis and receptor model (absolute principle component score-multiple linear regression, APCS-MLR) revealed that potential pollution sources and their corresponding contributions varied among the four functional zones. Variations of APCS values for each site of one functional zone as well as their annual average values highlighted the uncertainties associated with cross space-time effects in source apportionment. All these results reinforce the notion that the concept of zoning should be taken seriously in water pollution control. Being applicable to other rivers, the framework of management-oriented source apportionment

  3. An integrated approach to assess heavy metal source apportionment in peri-urban agricultural soils.

    PubMed

    Huang, Ying; Li, Tingqiang; Wu, Chengxian; He, Zhenli; Japenga, Jan; Deng, Meihua; Yang, Xiaoe

    2015-12-15

    Three techniques (Isotope Ratio Analysis, GIS mapping, and Multivariate Statistical Analysis) were integrated to assess heavy metal pollution and source apportionment in peri-urban agricultural soils. The soils in the study area were moderately polluted with cadmium (Cd) and mercury (Hg), lightly polluted with lead (Pb), and chromium (Cr). GIS Mapping suggested Cd pollution originates from point sources, whereas Hg, Pb, Cr could be traced back to both point and non-point sources. Principal component analysis (PCA) indicated aluminum (Al), manganese (Mn), nickel (Ni) were mainly inherited from natural sources, while Hg, Pb, and Cd were associated with two different kinds of anthropogenic sources. Cluster analysis (CA) further identified fertilizers, waste water, industrial solid wastes, road dust, and atmospheric deposition as potential sources. Based on isotope ratio analysis (IRA) organic fertilizers and road dusts accounted for 74-100% and 0-24% of the total Hg input, while road dusts and solid wastes contributed for 0-80% and 19-100% of the Pb input. This study provides a reliable approach for heavy metal source apportionment in this particular peri-urban area, with a clear potential for future application in other regions.

  4. Application of 14C analyses to source apportionment of carbonaceous PM 2.5 in the UK

    NASA Astrophysics Data System (ADS)

    Heal, Mathew R.; Naysmith, Philip; Cook, Gordon T.; Xu, Sheng; Duran, Teresa Raventós; Harrison, Roy M.

    2011-05-01

    Determination of the radiocarbon ( 14C) content of airborne particulate matter yields insight into the proportion of the carbonaceous material derived from fossil and contemporary carbon sources. Daily samples of PM 2.5 were collected by high-volume sampler at an urban background site in Birmingham, UK, and the fraction of 14C in both the total carbon, and in the organic and elemental carbon fractions, determined by two-stage combustion to CO 2, graphitisation and quantification by accelerator mass spectrometry. OC and EC content was also determined by Sunset Analyzer. The mean fraction contemporary TC in the PM 2.5 samples was 0.50 (range 0.27-0.66, n = 26). There was no seasonality to the data, but there was a positive trend between fraction contemporary TC and magnitude of SOC/TC ratio and for the high values of these two parameters to be associated with air-mass back trajectories arriving in Birmingham from over land. Using a five-compartment mass balance model on fraction contemporary carbon in OC and EC, the following average source apportionment for the TC in these PM 2.5 samples was derived: 27% fossil EC; 20% fossil OC; 2% biomass EC; 10% biomass OC; and 41% biogenic OC. The latter category will comprise, in addition to BVOC-derived SOC, other non-combustion contemporary carbon sources such as biological particles, vegetative detritus, humic material and tyre wear. The proportion of total PM 2.5 at this location estimated to derive from BVOC-derived secondary organic aerosol was 9-29%. The findings from this work are consistent with those from elsewhere in Europe and support the conclusion of a significant and ubiquitous contribution from non-fossil biogenic sources to the carbon in terrestrial aerosol.

  5. SOURCE APPORTIONMENT OF EXPOSURES TO VOLATILE ORGANIC COMPOUNDS: I. EVALUATION OF RECEPTOR MODELS USING SIMULATED EXPOSURE DATA. (R826788)

    EPA Science Inventory

    Four receptor-oriented source apportionment models were evaluated by applying them to simulated personal exposure data for select volatile organic compounds (VOCs) that were generated by Monte Carlo sampling from known source contributions and profiles. The exposure sources mo...

  6. Fine particulate matter source apportionment using a hybrid chemical transport and receptor model approach

    NASA Astrophysics Data System (ADS)

    Hu, Y.; Balachandran, S.; Pachon, J. E.; Baek, J.; Ivey, C.; Holmes, H.; Odman, M. T.; Mulholland, J. A.; Russell, A. G.

    2013-10-01

    A hybrid fine particulate matter (PM2.5) source apportionment approach based on a receptor-model (RM) species balance and species specific source impacts from a chemical transport model (CTM) equipped with a sensitivity analysis tool is developed to provide physically- and chemically-consistent relationships between source emissions and receptor impacts. This hybrid approach enhances RM results by providing initial estimates of source impacts from a much larger number of sources than are typically used in RMs, and provides source-receptor relationships for secondary species. Further, the method addresses issues of source collinearities, and accounts for emissions uncertainties. Hybrid method results also provide information on the resulting source impact uncertainties. We apply this hybrid approach to conduct PM2.5 source apportionment at Chemical Speciation Network (CSN) sites across the US. Ambient PM2.5 concentrations at these receptor sites were apportioned to 33 separate sources. Hybrid method results led to large changes of impacts from CTM estimates for sources such as dust, woodstove, and other biomass burning sources, but limited changes to others. The refinements reduced the differences between CTM-simulated and observed concentrations of individual PM2.5 species by over 98% when using a weighted least squared error minimization. The rankings of source impacts changed from the initial estimates, revealing that CTM-only results should be evaluated with observations. Assessment with RM results at six US locations showed that the hybrid results differ somewhat from commonly resolved sources. The hybrid method also resolved sources that typical RM methods do not capture without extra measurement information on unique tracers. The method can be readily applied to large domains and long (such as multi-annual) time periods to provide source impact estimates for management- and health-related studies.

  7. Source apportionment of PM2.5 in top polluted cities in Hebei, China using the CMAQ model

    NASA Astrophysics Data System (ADS)

    Wang, Litao; Wei, Zhe; Wei, Wei; Fu, Joshua S.; Meng, Chenchen; Ma, Simeng

    2015-12-01

    Hebei has been recognized as one of the most polluted provinces in China, characterized by extremely high concentrations of fine particulate matter (PM2.5) in many of its cities, especially those located in the southern area of the province and highly potentially northward transported to Beijing. Source apportionment of PM2.5 is the basis and prerequisite of an effective control strategy. In this study, the Mesoscale Modeling System Generation 5 (MM5) and the Models-3/Community Multiscale Air Quality (CMAQ) modeling system are applied to East Asia and North China at 36- and 12-km horizontal grid resolutions, and the source apportionment of PM2.5 in the three top polluted cities in Hebei, i.e., Shijiazhuang, Xingtai, and Handan, is performed using the Brute-Force method. It is concluded that the regional source contributions to PM2.5 are 27.9% in Shijiazhuang, 46.6% in Xingtai, and 40.4% in Handan. The major local contributors are industrial, domestic and agricultural sources in all the three cities with the contributions of 39.8%, 15.8%, and 10.6% in Shijiazhuang, 30.5%, 13.6%, and 6.9% in Xingtai, 35.9%, 13.5%, and 6.2% in Handan, respectively. As to the secondary aerosols of sulfate (SO42-), nitrate (NO3-), and ammonium (NH4+) in PM2.5, which are important chemical species in PM2.5 (about 30-40% in PM2.5) and cannot be further apportioned by receptor models, the regional source contributions to the total concentrations of SO42-, NO3-, and NH4+ are 40.9%, 62.0%, and 59.1% in Shijiazhuang, Xingtai, and Handan, respectively. The local industrial, domestic and agricultural contributions to those are 23.7%, 6.6%, and 29.8% in total in Shijiazhuang, 17.5%, 5.0%, and 17.7% in Xingtai, and 20.6%, 4.8%, and 17.8% in Handan, respectively. The regional joint controls of air pollution are more important in Xingtai and Handan than in Shijiazhuang, and the emission controls of agricultural sources need to be further considered in the future policy.

  8. Fine particulate matter source apportionment using a hybrid chemical transport and receptor model approach

    NASA Astrophysics Data System (ADS)

    Hu, Y.; Balachandran, S.; Pachon, J. E.; Baek, J.; Ivey, C.; Holmes, H.; Odman, M. T.; Mulholland, J. A.; Russell, A. G.

    2014-06-01

    A hybrid fine particulate matter (PM2.5) source apportionment approach based on a receptor model (RM) species balance and species specific source impacts from a chemical transport model (CTM) equipped with a sensitivity analysis tool is developed to provide physically and chemically consistent relationships between source emissions and receptor impacts. This hybrid approach enhances RM results by providing initial estimates of source impacts from a much larger number of sources than are typically used in RMs, and provides source-receptor relationships for secondary species. Further, the method addresses issues of source collinearities and accounts for emissions uncertainties. We apply this hybrid approach to conduct PM2.5 source apportionment at Chemical Speciation Network (CSN) sites across the US. Ambient PM2.5 concentrations at these receptor sites were apportioned to 33 separate sources. Hybrid method results led to large changes of impacts from CTM estimates for sources such as dust, woodstoves, and other biomass-burning sources, but limited changes to others. The refinements reduced the differences between CTM-simulated and observed concentrations of individual PM2.5 species by over 98% when using a weighted least-squares error minimization. The rankings of source impacts changed from the initial estimates, further demonstrating that CTM-only results should be evaluated with observations. Assessment with RM results at six US locations showed that the hybrid results differ somewhat from commonly resolved sources. The hybrid method also resolved sources that typical RM methods do not capture without extra measurement information for unique tracers. The method can be readily applied to large domains and long (such as multi-annual) time periods to provide source impact estimates for management- and health-related studies.

  9. Fine particulates over South Asia: Review and meta-analysis of PM2.5 source apportionment through receptor model.

    PubMed

    Singh, Nandita; Murari, Vishnu; Kumar, Manish; Barman, S C; Banerjee, Tirthankar

    2017-04-01

    Fine particulates (PM2.5) constitute dominant proportion of airborne particulates and have been often associated with human health disorders, changes in regional climate, hydrological cycle and more recently to food security. Intrinsic properties of particulates are direct function of sources. This initiates the necessity of conducting a comprehensive review on PM2.5 sources over South Asia which in turn may be valuable to develop strategies for emission control. Particulate source apportionment (SA) through receptor models is one of the existing tool to quantify contribution of particulate sources. Review of 51 SA studies were performed of which 48 (94%) were appeared within a span of 2007-2016. Almost half of SA studies (55%) were found concentrated over few typical urban stations (Delhi, Dhaka, Mumbai, Agra and Lahore). Due to lack of local particulate source profile and emission inventory, positive matrix factorization and principal component analysis (62% of studies) were the primary choices, followed by chemical mass balance (CMB, 18%). Metallic species were most regularly used as source tracers while use of organic molecular markers and gas-to-particle conversion were minimum. Among all the SA sites, vehicular emissions (mean ± sd: 37 ± 20%) emerged as most dominating PM2.5 source followed by industrial emissions (23 ± 16%), secondary aerosols (22 ± 12%) and natural sources (20 ± 15%). Vehicular emissions (39 ± 24%) also identified as dominating source for highly polluted sites (PM2.5>100 μgm(-3), n = 15) while site specific influence of either or in combination of industrial, secondary aerosols and natural sources were recognized. Source specific trends were considerably varied in terms of region and seasonality. Both natural and industrial sources were most influential over Pakistan and Afghanistan while over Indo-Gangetic plain, vehicular, natural and industrial emissions appeared dominant. Influence of vehicular emission was found

  10. Estimation of organic carbon blank values and error structures of the speciation trends network data for source apportionment

    SciTech Connect

    Eugene Kim; Philip K. Hopke; Youjun Qin

    2005-08-01

    Because the particulate organic carbon (OC) concentrations reported in U.S. Environment Protection Agency Speciation Trends Network (STN) data were not blank corrected, the OC blank concentrations were estimated using the intercept in particulate matter {lt} 2.5 {mu}m in aerodynamic diameter (PM2.5) regression against OC concentrations. The estimated OC blank concentrations ranged from 1 to 2.4 {mu}g/m{sup 3} showing higher values in urban areas for the 13 monitoring sites in the northeastern United States. In the STN data, several different samplers and analyzers are used, and various instruments show different method detection limit (MDL) values, as well as errors. A comprehensive set of error structures that would be used for numerous source apportionment studies of STN data was estimated by comparing a limited set of measured concentrations and their associated uncertainties. To examine the estimated error structures and investigate the appropriate MDL values, PM2.5 samples collected at a STN site in Burlington, VT, were analyzed through the application of the positive matrix factorization. A total of 323 samples that were collected between December 2000 and December 2003 and 49 species based on several variable selection criteria were used, and eight sources were successfully identified in this study with the estimated error structures and min values among different MDL values from the five instruments: secondary sulfate aerosol (41%) identified as the result of emissions from coal-fired power plants, secondary nitrate aerosol (20%), airborne soil (15%), gasoline vehicle emissions (7%), diesel emissions (7%), aged sea salt (4%), copper smelting (3%), and ferrous smelting (2%). Time series plots of contributions from airborne soil indicate that the highly elevated impacts from this source were likely caused primarily by dust storms.

  11. Source apportionment of ambient fine particulate matter in Dearborn, Michigan, using hourly resolved PM chemical composition data.

    PubMed

    Pancras, Joseph Patrick; Landis, Matthew S; Norris, Gary A; Vedantham, Ram; Dvonch, J Timothy

    2013-03-15

    High time-resolution aerosol sampling was conducted for one month during July-August 2007 in Dearborn, MI, a non-attainment area for fine particulate matter (PM2.5) National Ambient Air Quality Standards (NAAQS). Measurements of more than 30 PM2.5 species were made using a suite of semi-continuous sampling and monitoring instruments. Dynamic variations in the sub-hourly concentrations of source 'marker' elements were observed when discrete plumes from local sources impacted the sampling site. Hourly averaged PM2.5 composition data for 639 samples were used to identify and apportion PM2.5 emission sources using the multivariate receptor modeling techniques EPA Positive Matrix Factorization (PMF) v4.2 and EPA Unmix v6.0. Source contribution estimates from PMF and Unmix were then evaluated using the Sustained Wind Instance Method (SWIM), which identified plausible source origins. Ten sources were identified by both PMF and Unmix: (1) secondary sulfate, (2) secondary nitrate characterized by a significant diurnal trend, (3) iron and steel production, (4) a potassium-rich factor attributable to iron/steel slag waste processing, (5) a cadmium-rich factor attributable to incineration, (6) an oil refinery characterized by La/Ce>1 specific to south wind, (7) oil combustion, (8) coal combustion, (9) motor vehicles, and (10) road dust enriched with organic carbon. While both models apportioned secondary sulfate, oil refinery, and oil combustion PM2.5 masses closely, the mobile and industrial source apportionments differed. Analyses were also carried out to help infer time-of-day variations in the contributions of local sources.

  12. Mass closure and source apportionment of PM2.5 by Positive Matrix Factorization analysis in urban Mediterranean environment

    NASA Astrophysics Data System (ADS)

    Mantas, E.; Remoundaki, E.; Halari, I.; Kassomenos, P.; Theodosi, C.; Hatzikioseyian, A.; Mihalopoulos, N.

    2014-09-01

    A systematic monitoring of PM2.5 was carried out during a period of three years (from February 2010 to April 2013) at an urban site, at the National Technical University of Athens campus. Two types of 24-h PM2.5 samples have been collected: 271 samples on PTFE and 116 samples on quartz filters. Daily PM2.5 concentrations were determined for both types of samples. Total sulfur, crustal origin elements and elements of a major crustal component (Al, Si, Fe, Ca, K, Mg, Ti) trace elements (Zn, Pb, Cu, Ni, P, V, Cr, Mn) and water soluble ions (Cl-, NO3-, SO42-, Na+, K+, NH4+, Ca2+, Mg2+) were determined on the PTFE samples. Organic carbon (OC), elemental carbon (EC) and water soluble ions were determined on the quartz samples. For the mass closure six components were considered: Secondary Inorganic Aerosol (SIA), Organic Matter (OM), Elemental Carbon (EC), Dust, Mineral anthropogenic component (MIN) and Sea Salt (SS). SIA and OM contributed in the mass of PM2.5 almost equally: 30-36% and 30% respectively. EC, SS and MIN accounted for 5, 4 and 3% respectively of the total PM2.5 mass. Dust accounted for about 3-5% in absence of dust transport event and reached a much higher percentage in case of dust transport event. These contributions justify at least 80% of the PM2.5 mass. Source apportionment analysis has been performed by Positive Matrix Factorization. The combination of the PMF results obtained by both data sets lead to the definition of six factors: 1. SO42-, NH4+, OC (industrial/regional sources, secondary aerosol) 2. EC, OC, K and trace metals (traffic and heating by biomass burning, locally emitted aerosol). 3. Ca, EC, OC and trace metals (urban-resuspended road dust reflecting exhaust emissions), 4. Secondary nitrates 5. Na, Cl (marine source) 6. Si, Al, Ti, Ca, Fe (Dust transported from Sahara). These factors reflect not only main sources contributions but also underline the key role of atmospheric dynamics and aerosol ageing processes in this Mediterranean

  13. AIRUSE-LIFE+: a harmonized PM speciation and source apportionment in five southern European cities

    NASA Astrophysics Data System (ADS)

    Amato, Fulvio; Alastuey, Andrés; Karanasiou, Angeliki; Lucarelli, Franco; Nava, Silvia; Calzolai, Giulia; Severi, Mirko; Becagli, Silvia; Gianelle, Vorne L.; Colombi, Cristina; Alves, Celia; Custódio, Danilo; Nunes, Teresa; Cerqueira, Mario; Pio, Casimiro; Eleftheriadis, Konstantinos; Diapouli, Evangelia; Reche, Cristina; Cruz Minguillón, María; Manousakas, Manousos-Ioannis; Maggos, Thomas; Vratolis, Stergios; Harrison, Roy M.; Querol, Xavier

    2016-03-01

    The AIRUSE-LIFE+ project aims at characterizing similarities and heterogeneities in particulate matter (PM) sources and contributions in urban areas from southern Europe. Once the main PMx sources are identified, AIRUSE aims at developing and testing the efficiency of specific and non-specific measures to improve urban air quality. This article reports the results of the source apportionment of PM10 and PM2.5 conducted at three urban background sites (Barcelona, Florence and Milan, BCN-UB, FI-UB and MLN-UB), one suburban background site (Athens, ATH-SUB) and one traffic site (Porto, POR-TR). After collecting 1047 PM10 and 1116 PM2.5 24 h samples during 12 months (from January 2013 on) simultaneously at the five cities, these were analysed for the contents of OC, EC, anions, cations, major and trace elements and levoglucosan. The USEPA PMF5 receptor model was applied to these data sets in a harmonized way for each city. The sum of vehicle exhaust (VEX) and non-exhaust (NEX) contributes between 3.9 and 10.8 µg m-3 (16-32 %) to PM10 and 2.3 and 9.4 µg m-3 (15-36 %) to PM2.5, although a fraction of secondary nitrate is also traffic-related but could not be estimated. Important contributions arise from secondary particles (nitrate, sulfate and organics) in PM2.5 (37-82 %) but also in PM10 (40-71 %), mostly at background sites, revealing the importance of abating gaseous precursors in designing air quality plans. Biomass burning (BB) contributions vary widely, from 14-24 % of PM10 in POR-TR, MLN-UB and FI-UB, 7 % in ATH-SUB, to < 2 % in BCN-UB. In PM2.5, BB is the second most important source in MLN-UB (21 %) and in POR-TR (18 %), the third one in FI-UB (21 %) and ATH-SUB (11 %), but is again negligible (< 2 %) in BCN-UB. This large variability among cities is mostly due to the degree of penetration of biomass for residential heating. In Barcelona natural gas is very well supplied across the city and is used as fuel in 96 % of homes, while in other cities, PM levels

  14. Analyzing hydrocarbons in sewer to help in PAH source apportionment in sewage sludges.

    PubMed

    Mansuy-Huault, Laurence; Regier, Annette; Faure, Pierre

    2009-05-01

    A multi-molecular approach for polycyclic aromatic hydrocarbons (PAH) source apportionment in sewage sludge was tested. Three simple catchment areas with corresponding wastewater treatment plants (WWTP) were chosen. Sewage sludges of these WWTPs chronically exceeded the French guide values for PAHs. Aliphatic and aromatic hydrocarbons were quantified in sediments or wastewater suspended particulate matter sampled in different locations of the sewer as well as in sewage sludge. Various molecular indices including PAH ratios were calculated. The results showed that the ratios calculated from sewage sludge analyses provided a rather unspecific hydrocarbon fingerprint where combustion input appear as the main PAH sources. The complexity of the inputs as well as degradation occurring during wastewater treatment prevent any detailed diagnosis. Coupled to the analyses of samples collected in the sewer, the multi-molecular approach becomes more efficient especially for the identification of specific petroleum inputs such as fuel or used lubricating oils which can be important PAH sources. Indeed, the sampling in the sewer allows a spatial screening of the hydrocarbon inputs and facilitates the PAH source apportionment by avoiding the dilution of specific inputs with the whole wastewater inputs and by limiting the degradation of the molecular fingerprint that could occur during transfer and treatment in the WWTP. Then, the combination of PAH ratios and aliphatic distribution analyses is a very valuable approach that can help in sewer and WWTP management.

  15. Toxicity evaluation and source apportionment of Polycyclic Aromatic Hydrocarbons (PAHs) at three stations in Istanbul, Turkey.

    PubMed

    Hanedar, Asude; Alp, Kadir; Kaynak, Burçak; Avşar, Edip

    2014-08-01

    This paper focuses on the toxicity evaluation and source apportionment of Polycyclic Aromatic Hydrocarbons (PAHs) in three monitoring stations in Istanbul, Turkey. A total of 326 airborne samples were collected and analyzed for 16 PAHs and Total Suspended Particles (TSP) for the period of September 2006-December 2007. The total average PAH concentrations were 100.7±61.3, 84.6±46.7 and 25.1±13.3 ng m(-3) and the TSP concentrations were 101.2±53.2, 152.3±99.1, 49.8±18.6 μg m(-3) for URB1, URB2 and RUR stations, respectively. Benzo(a)Pyren (BaP) toxic equivalency factors to PAH concentration values were calculated indicating that the health risk of BaP and DiBenz(a,h)Anthracene (markers of traffic emissions) have the highest contribution compared to all of the other species measured at the sampling sites. In order to determine PAH sources, two different source apportionment techniques were applied to the measurements; diagnostic ratios (DR) and Positive Matrix Factorization (PMF). The results of the two applications were compatible indicating the vehicle emissions - especially diesel engines - as the major source for urban stations.

  16. RECENT APPLICATIONS OF SOURCE APPORTIONMENT METHODS AND RELATED NEEDS

    EPA Science Inventory

    Traditional receptor modeling studies have utilized factor analysis (like principal component analysis, PCA) and/or Chemical Mass Balance (CMB) to assess source influences. The limitations with these approaches is that PCA is qualitative and CMB requires the input of source pr...

  17. Source apportionment: findings from the US supersites program

    SciTech Connect

    John G. Watson; L.-W. Antony Chen; Judith C. Chow; Prakash Doraiswamy; Douglas H. Lowenthal

    2008-02-15

    Receptor models are used to identify and quantify source contributions to particulate matter and volatile organic compounds based on measurements of many chemical components at receptor sites. These components are selected based on their consistent appearance in some source types and their absence in others. UNMIX, positive matrix factorization (PMF), and effective variance are different solutions to the chemical mass balance (CMB) receptor model equations and are implemented on available software. In their more general form, the CMB equations allow spatial, temporal, transport, and particle size profiles to be combined with chemical source profiles for improved source resolution. Although UNMIX and PMF do not use source profiles explicitly as input data, they still require measured profiles to justify their derived source factors. The U.S. Supersites Program provided advanced datasets to apply these CMB solutions in different urban areas. Still lacking are better characterization of source emissions, new methods to estimate profile changes between source and receptor, and systematic sensitivity tests of deviations from receptor model assumptions. 154 refs.

  18. RECENT APPLICATIONS OF SOURCE APPORTIONMENT METHODS AND RELATED NEEDS

    EPA Science Inventory

    Traditional receptor modeling studies have utilized factor analysis (like principal component analysis, PCA) and/or Chemical Mass Balance (CMB) to assess source influences. The limitations with these approaches is that PCA is qualitative and CMB requires the input of source pr...

  19. Source apportionment of hydrocarbons measured in the Eagle Ford shale

    NASA Astrophysics Data System (ADS)

    Roest, G. S.; Schade, G. W.

    2016-12-01

    The rapid development of unconventional oil and gas in the US has led to hydrocarbon emissions that are yet to be accurately quantified. Emissions from the Eagle Ford Shale in southern Texas, one of the most productive shale plays in the U.S., have received little attention due to a sparse air quality monitoring network, thereby limiting studies of air quality within the region. We use hourly atmospheric hydrocarbon and meteorological data from three locations in the Eagle Ford Shale to assess their sources. Data are available from the Texas commission of environmental quality (TCEQ) air quality monitors in Floresville, a small town southeast of San Antonio and just north of the shale area; and Karnes city, a midsize rural city in the center of the shale. Our own measurements were carried out at a private ranch in rural Dimmit County in southern Texas from April to November of 2015. Air quality monitor data from the TCEQ were selected for the same time period. Non-negative matrix factorization in R (package NMF) was used to determine likely sources and their contributions above background. While the TCEQ monitor data consisted mostly of hydrocarbons, our own data include both CO, CO2, O3, and NOx. We find that rural Dimmit County hydrocarbons are dominated by oil and gas development sources, while central shale hydrocarbons at the TCEQ monitoring sites have a mix of sources including car traffic. However, oil and gas sources also dominate hydrocarbons at Floresville and Karnes City. Toxic benzene is nearly exclusively due to oil and gas development sources, including flaring, which NMF identifies as a major hydrocarbon source in Karnes City. Other major sources include emissions of light weight alkanes (C2-C5) from raw natural gas emissions and a larger set of alkanes (C2-C10) from oil sources, including liquid storage tanks.

  20. An inter-comparison of PM2.5 at urban and urban background sites: Chemical characterization and source apportionment

    NASA Astrophysics Data System (ADS)

    Cesari, D.; Donateo, A.; Conte, M.; Merico, E.; Giangreco, A.; Giangreco, F.; Contini, D.

    2016-06-01

    A measurement campaign was performed between 04/03/2013 and 17/07/2013 for simultaneous collection of PM2.5 samples in two nearby sites in southeastern Italy: an urban site and an urban background site. PM2.5 at the two sites were similar; however, the chemical composition and the contributions of the main sources were significantly different. The coefficients of divergence (CODs) showed spatial heterogeneity of EC (higher at the urban site because of traffic emissions) and of all metals. Major ions (NH4+, Na+, and SO42 -) and OC had low CODs, suggesting a homogeneous distribution of sea spray, secondary sulfate, and secondary organic matter (SOM = 1.6*OCsec, where OCsec is the secondary OC). The strong correlations between Na+ and Cl-, and the low Cl-/Na+ ratios, suggested the presence of aged sea spray with chloride depletion (about 79% of Cl-) and formation of sodium nitrate at both sites. In both sites, the non-sea-salt sulfate was about 97% of sulfate, and the strong correlation between SO42 - and NH4+ indicated that ammonium was present as ammonium sulfate. However, during advection of Saharan Dust, calcium sulfate was present rather than ammonium sulfate. The source apportionment was performed using the Positive Matrix Factorization comparing outputs of model EPA PMF 3.0 and 5.0 version. Six aerosol sources were identified at both sites: traffic, biomass burning, crustal-resuspended dust, secondary nitrate, marine aerosol, and secondary sulfate. The PMF3.0 model was not completely able, in these sites, to separate marine contribution from secondary nitrate and secondary sulfate from OC, underestimating the marine contribution and overestimating the secondary sulfate with respect to stoichiometric calculations. The application of specific constraints on PMF5.0 provided cleaner profiles, improving the comparison with stoichiometric calculations. The seasonal trends revealed larger biomass burning contributions during the cold period at both sites due to

  1. Source apportionment of PM2.5 in Incheon, Korea

    NASA Astrophysics Data System (ADS)

    Choi, J.; Ban, S.; Lee, C.; Yi, S.; Zoh, K.

    2011-12-01

    PM2.5 samples were collected at a centrally located urban monitoring site in Incheon, Korea, every third day from Jun 2009 to may 2010 and analyzed their chemical species. In this study, we investigated the source of PM2.5 using Positive Matrix Factorization(PMF), the source area from Potential Source Contribution Function (PSCF) and Conditional Probability Function(CPF), and characterized source variation among episode, non-episode, yellow sand events. Incheon, study site, is located at the mid-western tip of the Korean Peninsula with a population of 2.6 million people and area of 1029.4 km2, respectively. As a transportation hub, the city also holds the importance of meteological/geological aspect affecting the air quality of capital region, in that is prevailing westerlies zone and a air passageway from China to Japan passing through seoul, korea. In the study, the Four channel based on Annular Denuder System(ADS) were used for sample collection(URG co, USA). The filter samples were analyzed with respect to species type such as ion group, metal, and OC/EC compound using ion chromatography, ICP/MS, and NIOSH TOT method, respectively. The PM2.5 concentration was 43ug/m3 that is almost three times higher than the US NAAQS annual PM2.5 standard of 15ug/m3. Nine PM2.5 sources were resolved from PMF analysis that provided reasonable source profiles and interesting insights into the source contributions to the ambient mass concentrations. The major sources of PM2.5 were secondary nitrate(26.4%), secondary sulfate(17.3%), gasoline(16.4%), and residual oil combustion(13.5%), with lesser contributions from biomass burning (7.5%), road dust(6.9%), soil (5.5%), coal fire powerplant (4.0%), and free sea salt(2.4%). CPF results identified possible local source directions such as motor vehicles, free sea salt. PSCF results indicated that likely pollution areas increased secondary particle concentrations(sulfate and nitrate) in Incheon to be the major industrial areas in China

  2. Source apportionment of fine particles in Kuwait City.

    PubMed

    Alolayan, Mohammad A; Brown, Kathleen W; Evans, John S; Bouhamra, Walid S; Koutrakis, Petros

    2013-03-15

    This study investigated major sources of PM2.5 in the atmosphere of Kuwait based on a sampling program conducted between February 2004 and October 2005. Three source identification techniques were used in this study: (1) a positive matrix factorization model; (2) backward trajectory profiles; and (3) concentration rose plots. Five major sources of PM2.5 were estimated. These were sand dust (sand storms), oil combustion (power plants), petrochemical industry (fertilizer, nylon or catalyst regeneration facilities), traffic (vehicle emissions and road dust) and transported emissions (emissions from outside Kuwait, such as those from automobiles, road dust or smelters). The estimated contributions to PM2.5 of these sources were: 54% from sand dust, 18% from oil combustion, 12% from petrochemical industry, 11% from traffic and 5% from anthropogenic sources transported from outside the country. Oil combustion, petrochemical industry and traffic were found to emanate from local sources, whereas sand dust and some emissions from traffic, and possibly smelters, appeared to originate from sources outside of Kuwait (transported). The PM2.5 levels in Kuwait during our previous sampling study averaged 53μg/m(3). More than half of the measured PM2.5 appears to have been due to crustal material, much originating outside of the country. However, the relatively high levels of PM2.5 contributed by anthropogenic local sources, such as oil combustion, petrochemical industry emissions, and traffic indicated that there may be great opportunities for Kuwait to improve public health. The application of cost-effective emission controls and development of forward looking environmental health policies have the potential to significantly reduce emissions, population exposures to PM2.5 and the burden of mortality and morbidity from air pollution.

  3. Source apportionment of exposures to volatile organic compounds: II. Application of receptor models to TEAM study data

    NASA Astrophysics Data System (ADS)

    Anderson, Melissa J.; Daly, Eileen P.; Miller, Shelly L.; Milford, Jana B.

    Four receptor-oriented source apportionment models were applied to personal exposure measurements for toxic volatile organic compounds (VOCs). The measurements are from the total exposure assessment methodology studies conducted from 1980 to 1984 in New Jersey (NJ) and California (CA) and the 1987-1990 CA Indoor Exposure study. The receptor models applied are the Chemical Mass Balance model, Principal Component Analysis/Absolute Principal Component Scores, Positive Matrix Factorization, and Graphical Ratio Analysis for Composition Estimates/Source Apportionment by Factors with Explicit Restriction. Major sources of personal exposure to toxic VOCs appear to have been aromatic sources resembling automobile exhaust, gasoline vapor, or environmental tobacco smoke, and a 1,1,1-trichloroethane-dominated source that may be associated with solvent or pesticide use. Drycleaning chemicals, deodorizers or mothballs, and building materials or carpet emissions also appear to have been significant sources of exposure. Source apportionment results from the four models agreed reasonably well for the NJ data. The performance of the models was generally poorer for the CA data, and the corresponding source apportionment results were less consistent across the models.

  4. Atmospheric polycyclic aromatic hydrocarbons in the urban environment: Occurrence, toxicity and source apportionment.

    PubMed

    Mishra, Nitika; Ayoko, Godwin A; Morawska, Lidia

    2016-01-01

    Polycyclic Aromatic Hydrocarbons (PAHs) represent a major class of toxic pollutants because of their carcinogenic and mutagenic characteristics. People living in urban areas are regularly exposed to PAHs because of abundance of their emission sources. Within this context, this study aimed to: (i) identify and quantify the levels of ambient PAHs in an urban environment; (ii) evaluate their toxicity; and (iii) identify their sources as well as the contribution of specific sources to measured concentrations. Sixteen PAHs were identified and quantified in air samples collected from Brisbane. Principal Component Analysis - Absolute Principal Component Scores (PCA-APCS) was used in order to conduct source apportionment of the measured PAHs. Vehicular emissions, natural gas combustion, petrol emissions and evaporative/unburned fuel were the sources identified; contributing 56%, 21%, 15% and 8% of the total PAHs emissions, respectively, all of which need to be considered for any pollution control measures implemented in urban areas.

  5. Expressing lead isotopic compositions by fractional abundances for environmental source apportionment.

    PubMed

    Zhi, Yuyou; Guo, Tiantian; Shi, Jiachun; Zeng, Lingzao; Wu, Laosheng

    2016-11-01

    Lead (Pb) isotope has been extensively used to identify sources of Pb and apportion their contributions in the environment. Conventionally, isotope ratios are used to express Pb isotopic composition. However, the linear combination of Pb isotope ratios is not consistent with mass balance. Moreover, the graphical presentations based on Pb isotope ratios are always inconsistent when different Pb isotope ratios are used. In this study, we proposed to use fractional abundance to express Pb isotopic composition to achieve more accurate and reliable source apportionment. A new method (rotation-projection method) based on fractional abundance was developed in this research. The new method compared favorably to the isotopic ratio-based method and to another fractional abundance based method using default (204)Pb value (0) (Walraven's method). It allows to present four-dimensional (4-D) Pb isotope fractional abundance data in a 3-D plot. In the meantime, due to the low variation of the fractional abundance of (204)Pb in the terrestrial ecosystem, the terrestrial Pb isotope fractional abundance data fell nearly on a plane, which further allows to plot the Pb isotope fractional abundance data on a two-dimensional diagram. Proper presentation of the isotopic composition data helps to achieve more accurate and reliable source identification and apportionment. Copyright © 2016 Elsevier Ltd. All rights reserved.

  6. Heavy metal contamination status and source apportionment in sediments of Songhua River Harbin region, Northeast China.

    PubMed

    Li, Ning; Tian, Yu; Zhang, Jun; Zuo, Wei; Zhan, Wei; Zhang, Jian

    2016-07-09

    The Songhua River represents one of the seven major river systems in China. It flows through Harbin city with 66 km long, locating in the northern China with a longer winter time. This paper aimed to study concentration distributions, stability, risk assessment, and source apportionment of heavy metals including chromium (Cr), cadmium (Cd), lead (Pb), mercury (Hg), arsenic (As), copper (Cu), zinc (Zn), and nickel (Ni) in 11 selected sections of the Songhua River Harbin region. Results showed that Cr, Cd, Pb, Hg, and As exceeded their respective geochemical background values in sediments of most monitoring sections. Compared with other important rivers and lakes in China, Cr, Hg, Cd, and As pollutions in surface sediments were above medium level. Further analysis of chemical speciation indicated that Cr and As in surface sediments were relatively stable while Pb and Cd were easily bioavailable. Correlation analysis revealed sources of these metals except As might be identical. Pollution levels and ecological risks of heavy metals in surface sediments presented higher in the mainstream region (45° 47.0' N ~ 45° 53.3' N, 126° 37.0' E ~ 126° 42.1' E). Source apportionment found Hejiagou and Ashi River were the main contributors to metal pollution of this region. Thus, anthropogenic activities along the Hejiagou and Ashi River should be restricted in order to protect the Songhua River Harbin region from metal contamination.

  7. Source apportionment of trace contaminants in urban sewer catchments.

    PubMed

    Comber, Sean; Gardner, Mike; Jones, Vera; Ellor, Brian

    2015-01-01

    Sampling and analysis of Water Framework Directive priority chemicals were undertaken in nine urban catchments across the UK. Over 9000 samples were collected from a number of different catchment sources including tap water, domestic waste water, surface water runoff, trade discharges, town centre and light industrial estate wastewaters. Determinands included trace metals, polyaromatic hydrocarbons (PAHs), persistent organic pollutants and a number of common pharmaceuticals. Loads of the chemicals from each catchment entering the local wastewater treatment works (WwTW) were estimated and were shown to be relatively consistent between different catchments, after taking population into account. A Monte Carlo mixing model was used to combine the concentrations and flows from the different catchment sources and to predict concentrations and loads entering the WwTW. Based on the model output, the significance of the different sources could be evaluated. The study highlighted the importance of domestic wastewater as a source of contaminants, including metals and trace organic substances (such as ethylenediaminetetraacetic acid (EDTA), bisphenol A, nonylphenol and tributyl tin (TBT)). Concentrations in trade discharges were important in some locations in the case of nonylphenol, EDTA, TBT, as well as for some metals such as copper, zinc and nickel. Contributions to the total load from town centre and light industrial estate sources were generally less than 10% of the total.

  8. Source forensics of black carbon aerosols from China.

    PubMed

    Chen, Bing; Andersson, August; Lee, Meehye; Kirillova, Elena N; Xiao, Qianfen; Kruså, Martin; Shi, Meinan; Hu, Ke; Lu, Zifeng; Streets, David G; Du, Ke; Gustafsson, Örjan

    2013-08-20

    The limited understanding of black carbon (BC) aerosol emissions from incomplete combustion causes a poorly constrained anthropogenic climate warming that globally may be second only to CO2 and regionally, such as over East Asia, the dominant driver of climate change. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain as fossil BC is a stronger climate forcer. The source apportionment is the underpinning for targeted mitigation actions. However, technology-based "bottom-up" emission inventories are inconclusive, largely due to uncertain BC emission factors from small-scale/household combustion and open burning. We use "top-down" radiocarbon measurements of atmospheric BC from five sites including three city sites and two regional sites to determine that fossil fuel combustion produces 80 ± 6% of the BC emitted from China. This source-diagnostic radiocarbon signal in the ambient aerosol over East Asia establishes a much larger role for fossil fuel combustion than suggested by all 15 BC emission inventory models, including one with monthly resolution. Our results suggest that current climate modeling should refine both BC emission strength and consider the stronger radiative absorption associated with fossil-fuel-derived BC. To mitigate near-term climate effects and improve air quality in East Asia, activities such as residential coal combustion and city traffic should be targeted.

  9. Chemical composition and source apportionment of PM2.5 in Seoul, Korea during 2012-2013

    NASA Astrophysics Data System (ADS)

    Heo, Junghwa; Kim, Sang-Woo; Mann Kim, Bong; Kim, Jin Young

    2017-04-01

    carbonaceous component after source apportionment analysis, was the highest at 10.6% in winter. This suggests that about 10.6% of PM2.5 concentration cannot be estimated by local sources and can be attributable to the polluted aerosols transported from China. In this presentation, more detailed comparisons among CMB, Positive Matrix Factorization (PMF) and Solver for Mixture Problem (SMP) models will be presented.

  10. Isotopic Signatures for Source Apportionment of Ammonia in Urban Atmosphere

    NASA Astrophysics Data System (ADS)

    Chang, Y.; Liu, X.

    2016-12-01

    Stable nitrogen isotope composition (δ15N) offers new opportunities to address the long-standing and ongoing controversy regarding the origins of ambient ammonia (NH3), a vital precursor of PM2.5 inorganic components, in the urban atmosphere. In this study, the δ15N values of NH3 samples collected from various sources were constrained using a novel and robust chemical method coupled with standard elemental analysis procedures. Independent of the wide variation in mass concentrations (ranging from 33 (vehicle) to over 6000 (human excreta) μg m-3), different NH3 sources have generally different δ15N values (ranging from -52.0 to -9.6‰). Significantly high δ15N values are seen as a characteristic feature of all vehicle-derived NH3 samples (-14.2±2.8‰), which can be distinguished from other sources emitted at environmental temperature (-29.1±1.7, -37.8±3.6, and -50.0±1.8‰ for livestock, waste, and fertilizer, respectively). The isotope δ15N signatures for a range of NH3 emission sources were used to evaluate the contributions of the different sources within measured ambient NH3 in Beijing, using an isotope mixing model (IsoSource). The method was used to quantify the sources of ambient NH3 before, during and after the 2014 APEC summit, when a set of stringent air quality control measures were implemented. Results show that the average NH3 concentrations (the overall contributions of traffic, waste, livestock, and fertilizer) during the three periods were 9.1 (15.1, 31.2, 23.7, and 30.0%), 7.3 (8.8, 24.9, 14.3, and 52.0%), and 12.7 (29.4, 23.6, 31.7, and 15.4%) μg m-3, respectively, representing a 20.0% decrease first and then a 74.5% increase in overall NH3 mass concentrations. During (after) the summit, the contributions of traffic, waste, livestock, and fertilizer decreased (increased) by 58.7 (234.2), 0.9 (-5.0), 41.0 (120.8), and -87.6% (-70.5%) when compared with periods before (during) the summit, respectively, signifying that future NH3 control

  11. Investigating the contribution of shipping emissions to atmospheric PM2.5 using a combined source apportionment approach.

    PubMed

    Lang, Jianlei; Zhou, Ying; Chen, Dongsheng; Xing, Xiaofan; Wei, Lin; Wang, Xiaotong; Zhao, Na; Zhang, Yanyun; Guo, Xiurui; Han, Lihui; Cheng, Shuiyuan

    2017-10-01

    Many studies have been conducted focusing on the contribution of land emission sources to PM2.5 in China; however, little attention had been paid to other contributions, especially the secondary contributions from shipping emissions to atmospheric PM2.5. In this study, a combined source apportionment approach, including principle component analysis (PCA) and WRF-CMAQ simulation, was applied to identify both primary and secondary contributions from ships to atmospheric PM2.5. An intensive PM2.5 observation was conducted from April 2014 to January 2015 in Qinhuangdao, which was close to the largest energy output port of China. The chemical components analysis results showed that the primary component was the major contributor to PM2.5, with proportions of 48.3%, 48.9%, 55.1% and 55.4% in spring, summer, autumn and winter, respectively. The secondary component contributed higher fractions in summer (48.2%) and winter (36.8%), but had lower percentages in spring (30.1%) and autumn (32.7%). The hybrid source apportionment results indicated that the secondary contribution (SC) of shipping emissions to PM2.5 could not be ignored. The annual average SC was 2.7%, which was comparable to the primary contribution (2.9%). The SC was higher in summer (5.3%), but lower in winter (1.1%). The primary contributions to atmospheric PM2.5 were 3.0%, 2.5%, 3.4% and 2.7% in spring, summer, autumn and winter, respectively. As for the detailed chemical components, the contributions of shipping emissions were 2.3%, 0.5%, 0.1%, 1.0%, 1.7% and 0.1% to elements & sea salt, primary organic aerosol (POA), element carbon (EC), nitrate, sulfate and secondary organic carbon (SOA), respectively. The results of this study will further the understanding of the implications of shipping emissions in PM2.5 pollution. Copyright © 2017 Elsevier Ltd. All rights reserved.

  12. Ultrafine particles: exposure and source apportionment in 56 Danish homes.

    PubMed

    Bekö, Gabriel; Weschler, Charles J; Wierzbicka, Aneta; Karottki, Dorina Gabriela; Toftum, Jørn; Loft, Steffen; Clausen, Geo

    2013-09-17

    Particle number (PN) concentrations (10-300 nm in size) were continuously measured over a period of ~45 h in 56 residences of nonsmokers in Copenhagen, Denmark. The highest concentrations were measured when occupants were present and awake (geometric mean, GM: 22.3 × 10(3) cm(-3)), the lowest when the homes were vacant (GM: 6.1 × 10(3) cm(-3)) or the occupants were asleep (GM: 5.1 × 10(3) cm(-3)). Diary entries regarding occupancy and particle related activities were used to identify source events and apportion the daily integrated exposure among sources. Source events clearly resulted in increased PN concentrations and decreased average particle diameter. For a given event, elevated particle concentrations persisted for several hours after the emission of fresh particles ceased. The residential daily integrated PN exposure in the 56 homes ranged between 37 × 10(3) and 6.0 × 10(6) particles per cm(3)·h/day (GM: 3.3 × 10(5) cm(-3)·h/day). On average, ~90% of this exposure occurred outside of the period from midnight to 6 a.m. Source events, especially candle burning, cooking, toasting, and unknown activities, were responsible on average for ~65% of the residential integrated exposure (51% without the unknown activities). Candle burning occurred in half of the homes where, on average, it was responsible for almost 60% of the integrated exposure.

  13. Sensitivity tests to define the source apportionment performance criteria in the DeltaSA tool

    NASA Astrophysics Data System (ADS)

    Pernigotti, Denise; Belis, Claudio A.

    2017-04-01

    Identification and quantification of the contribution of emission sources to a given area is a key task for the design of abatement strategies. Moreover, European member states are obliged to report this kind of information for zones where the pollution levels exceed the limit values. At present, little is known about the performance and uncertainty of the variety of methodologies used for source apportionment and the comparability between the results of studies using different approaches. The source apportionment Delta (SA Delta) is a tool developed by the EC-JRC to support the particulate matter source apportionment modellers in the identification of sources (for factor analysis studies) and/or in the measure of their performance. The source identification is performed by the tool measuring the proximity of any user chemical profile to preloaded repository data (SPECIATE and SPECIEUROPE). The model performances criteria are based on standard statistical indexes calculated by comparing participants' source contribute estimates and their time series with preloaded references data. Those preloaded data refer to previous European SA intercomparison exercises: the first with real world data (22 participants), the second with synthetic data (25 participants) and the last with real world data which was also extended to Chemical Transport Models (38 receptor models and 4 CTMs). The references used for the model performances are 'true' (predefined by JRC) for the synthetic while they are calculated as ensemble average of the participants' results in real world intercomparisons. The candidates used for each source ensemble reference calculation were selected among participants results based on a number of consistency checks plus the similarity between their chemical profiles to the repository measured data. The estimation of the ensemble reference uncertainty is crucial in order to evaluate the users' performances against it. For this reason a sensitivity analysis on

  14. Source apportionment of volatile organic compounds measured in Edmonton, Alberta

    NASA Astrophysics Data System (ADS)

    McCarthy, Michael C.; Aklilu, Yayne-Abeba; Brown, Steven G.; Lyder, David A.

    2013-12-01

    From 2003 to 2009, whole air samples were collected at two sites in Edmonton and analyzed for over 77 volatile organic compounds (VOCs). VOCs were sampled in the downtown area (Central site) and an industrial area on the eastern side of the city (East site). Concentrations of most VOCs were highest at the East site, with an average total VOC mass concentration of 221 μg m-3. The average total VOC mass concentration at the Central site was 65 μg m-3. The United States Environmental Protection Agency's positive matrix factorization receptor model (EPA PMF) was used to apportion ambient concentrations of VOCs into eleven factors, which were associated with emissions sources. On average, 94 and 99% of the measured mass were apportioned by PMF at the East and Central site, respectively. Factors include transportation combustion (gasoline and diesel), industrial sources (industrial evaporative, industrial feedstock, gasoline production/storage, industrial chemical use), mixed mobile and industrial (gasoline evaporative, fugitive butane), a biogenic source, a natural gas related source, and a factor that was associated with global background pollutants transported into the area. Transportation sources accounted for more than half of the reconstructed VOC mass concentration at the Central site, but less than 10% of the reconstructed mass concentration at the East site. By contrast, industrial sources accounted for ten times more of the reconstructed VOC mass concentration at the East site than at the Central site and were responsible for approximately 75% of the reconstructed VOC mass concentration observed at the East site. Of the six industrial factors identified at the East site, four were linked to petrochemical industry production and storage. The two largest contributors to the reconstructed VOC mass concentration at the East site were associated with fugitive emissions of volatile species (butanes, pentanes, hexane, and cyclohexane); together, these two factors

  15. Source apportionment of polychlorinated biphenyls in the tidal Delaware River.

    PubMed

    Du, Songyan; Belton, Thomas J; Rodenburg, Lisa A

    2008-06-01

    The Delaware River, similar to many surface water bodies throughout the United States, is impaired due to polychlorinated biphenyl (PCB) concentrations that exceed the federal water quality standard. A total maximum daily load (TMDL) for PCBs in the Delaware was promulgated in 2003 after construction of a detailed water quality model that relied upon estimated PCB loadings from sources such as wastewater treatment plant effluents, contaminated sites, and tributaries. The purpose of this project was to corroborate this loading estimate by analyzing ambient water column data on PCB concentrations in the Delaware River via positive matrix factorization (PMF) in order to identify covarying congener patterns that are, in theory, associated with sources. The PMF program identified six factors (covarying congener patterns) that appear to be associated with sources, such as sediment resuspension, contaminated sites, and wastewater effluents and combined sewer overflows (CSOs). PCB 11 was found to be a useful tracer for CSO/ wastewater inputs despite the fact that no known dye manufacturers exist in the watershed. This analysis generally corroborates the PCB loading estimate used in the water quality model.

  16. Source apportionment of atmospheric PAHs in the western Balkans by natural abundance radiocarbon analysis.

    PubMed

    Zencak, Zdenek; Klanova, Jana; Holoubek, Ivan; Gustafsson, Orjan

    2007-06-01

    Progress in source apportionment of priority combustion-derived atmospheric pollutants can be made by an inverse approach to inventory emissions, namely, receptor-based compound class-specific radiocarbon analysis (CCSRA) of target pollutants. In the present study, CCSRA of the combustion-derived polycyclic aromatic hydrocarbons (PAHs) present in the atmosphere of the countries of the former republic of Yugoslavia was performed. The carbon stable isotope composition (delta13C) of PAHs varied between -27.68 and -27.19 per thousand, whereas delta14C values ranged from -568 per thousand for PAHs sampled in Kosovo to -288 per thousand for PAHs sampled in the Sarajevo area. The application of an isotopic mass balance model to these delta14C data revealed a significant contribution (35-65%) from the combustion of non-fossil material to the atmospheric PAH pollution, even in urban and industrialized areas. Furthermore, consistency was observed between the isotopic composition of PAHs obtained by high-volume sampling and those collected by passive sampling. This encourages the use of passive samplers for CCSRA applications. This marks the first time that a CCSRA investigation could be executed on a geographically wide scale, providing a quantitative field-based source apportionment, which points out that also non-fossil combustion processes should be targeted for remedial action.

  17. Source apportionment of atmospheric PAHs in the Western Balkans by natural abundance radiocarbon analysis

    SciTech Connect

    Zdenek Zencak; Jana Klanova; Ivan Holoubek; Oerjan Gustafsson

    2007-06-01

    Progress in source apportionment of priority combustion-derived atmospheric pollutants can be made by an inverse approach to inventory emissions, namely, receptor-based compound class-specific radiocarbon analysis (CCSRA) of target pollutants. In the present study, CCSRA of the combustion-derived polycyclic aromatic hydrocarbons (PAHs) present in the atmosphere of the countries of the former republic of Yugoslavia was performed. The carbon stable isotope composition ({delta}{sup 13}C) of PAHs varied between -27.68 and -27.19{per_thousand}, whereas {Delta}{sup 14}C values ranged from -568{per_thousand} for PAHs sampled in Kosovo to -288{per_thousand} for PAHs sampled in the Sarajevo area. The application of an isotopic mass balance model to these {Delta}{sup 14}C data revealed a significant contribution (35-65%) from the combustion of non-fossil material to the atmospheric PAH pollution, even in urban and industrialized areas. Furthermore, consistency was observed between the isotopic composition of PAHs obtained by high-volume sampling and those collected by passive sampling. This encourages the use of passive samplers for CCSRA applications. This marks the first time that a CCSRA investigation could be executed on a geographically wide scale, providing a quantitative field-based source apportionment, which points out that also non-fossil combustion processes should be targeted for remedial action. 36 refs., 1 fig., 3 tabs.

  18. Volatility of organic molecular markers used for source apportionment analysis: measurements and implications for atmospheric lifetime.

    PubMed

    May, Andrew A; Saleh, Rawad; Hennigan, Christopher J; Donahue, Neil M; Robinson, Allen L

    2012-11-20

    Molecular markers are organic species used to define fingerprints for source apportionment of ambient fine particulate matter. Traditionally, these markers have been assumed to be stable in the atmosphere. This work investigates the gas-particle partitioning of eight organic species used as molecular markers in receptor models for biomass burning (levoglucosan), motor vehicles (5α-cholestane, n-hexacosane, n-triacontane, 1,2-benz[a]anthracene, coronene), and meat cooking (cholesterol, oleic acid). Experiments were conducted using a thermodenuder to measure the evaporation of single component particles. The data were analyzed using the integrated volume method to determine saturation concentrations and enthalpies of vaporization for each compound. The results indicate that appreciable quantities (>10%) of most of these markers exist in the gas phase under typical atmospheric conditions. Therefore, these species should be considered semivolatile. Predictions from a chemical kinetics model indicate that gas-particle partitioning has important effects on the atmospheric lifetime of these species. The atmospheric decay of semivolatile compounds proceeds much more rapidly than nonvolatile compounds because gas-phase oxidation induces evaporation of particle-phase material. Therefore, both gas-particle partitioning and chemical reactions need to be accounted for when semivolatile molecular markers are used for source apportionment studies.

  19. Source apportionment studies on particulate matter in Beijing/China

    NASA Astrophysics Data System (ADS)

    Suppan, P.; Shen, R.; Shao, L.; Schrader, S.; Schäfer, K.; Norra, S.; Vogel, B.; Cen, K.; Wang, Y.

    2013-05-01

    More than 15 million people in the greater area of Beijing are still suffering from severe air pollution levels caused by sources within the city itself but also from external impacts like severe dust storms and long range advection from the southern and central part of China. Within this context particulate matter (PM) is the major air pollutant in the greater area of Beijing (Garland et al., 2009). PM did not serve only as lead substance for air quality levels and therefore for adverse health impact effects but also for a strong influence on the climate system by changing e.g. the radiative balance. Investigations on emission reductions during the Olympic Summer Games in 2008 have caused a strong reduction on coarser particles (PM10) but not on smaller particles (PM2.5). In order to discriminate the composition of the particulate matter levels, the different behavior of coarser and smaller particles investigations on source attribution, particle characteristics and external impacts on the PM levels of the city of Beijing by measurements and modeling are performed: a) Examples of long term measurements of PM2.5 filter sampling in 2010/2011 with the objectives of detailed chemical (source attribution, carbon fraction, organic speciation and inorganic composition) and isotopic analyses as well as toxicological assessment in cooperation with several institutions (Karlsruhe Institute of Technology (IfGG/IMG), Helmholtz Zentrum München (HMGU), University Rostock (UR), Chinese University of Mining and Technology Beijing, CUMTB) will be discussed. b) The impact of dust storm events on the overall pollution level of particulate matter in the greater area of Beijing is being assessed by the online coupled comprehensive model system COSMO-ART. First results of the dust storm modeling in northern China (2011, April 30th) demonstrates very well the general behavior of the meteorological parameters temperature and humidity as well as a good agreement between modeled and

  20. Contamination characteristics and source apportionment of trace metals in soils around Miyun Reservoir.

    PubMed

    Chen, Haiyang; Teng, Yanguo; Chen, Ruihui; Li, Jiao; Wang, Jinsheng

    2016-08-01

    Due to their toxicity and bioaccumulation, trace metals in soils can result in a wide range of toxic effects on animals, plants, microbes, and even humans. Recognizing the contamination characteristics of soil metals and especially apportioning their potential sources are the necessary preconditions for pollution prevention and control. Over the past decades, several receptor models have been developed for source apportionment. Among them, positive matrix factorization (PMF) has gained popularity and was recommended by the US Environmental Protection Agency as a general modeling tool. In this study, an extended chemometrics model, multivariate curve resolution-alternating least squares based on maximum likelihood principal component analysis (MCR-ALS/MLPCA), was proposed for source apportionment of soil metals and applied to identify the potential sources of trace metals in soils around Miyun Reservoir. Similar to PMF, the MCR-ALS/MLPCA model can incorporate measurement error information and non-negativity constraints in its calculation procedures. Model validation with synthetic dataset suggested that the MCR-ALS/MLPCA could extract acceptable recovered source profiles even considering relatively larger error levels. When applying to identify the sources of trace metals in soils around Miyun Reservoir, the MCR-ALS/MLPCA model obtained the highly similar profiles with PMF. On the other hand, the assessment results of contamination status showed that the soils around reservoir were polluted by trace metals in slightly moderate degree but potentially posed acceptable risks to the public. Mining activities, fertilizers and agrochemicals, and atmospheric deposition were identified as the potential anthropogenic sources with contributions of 24.8, 14.6, and 13.3 %, respectively. In order to protect the drinking water source of Beijing, special attention should be paid to the metal inputs to soils from mining and agricultural activities.

  1. Source apportionment of settleable particles in an impacted urban and industrialized region in Brazil.

    PubMed

    Santos, Jane Meri; Reis, Neyval Costa; Galvão, Elson Silva; Silveira, Alexsander; Goulart, Elisa Valentim; Lima, Ana Teresa

    2017-08-07

    Settleable particulate matter (SPM), especially coarser particles with diameters greater than 10 μm, has been found culprit of high deposition rates in cities affected by hinterland industrial activities. This is the case of Metropolitan Region of Vitoria (MRV), Espirito Santo, Brazil where industrial facilities are located within the urban sprawl and building constructions are intense. Frequent population complaints to the environmental protection agency (IEMA) throughout the years have triggered monitoring campaigns to determine SPM deposition rates and source apportionment. Eight different locations were monitored throughout the MRV, and SPM was quantified and chemically characterized. Sources profiles were defined either by using US EPA SPECIATE data or by experimental analysis. Atmospheric fallout in the MRV ranged between 2 and 20g/(m(2) 30-day), with only one monitoring station ranging from 6-10 g/(m(2) 30-day). EC, OC, Fe, Al, and Si were found the main constituents of dry deposition in the region. Source apportionment by the chemical mass balance (CMB) model determined that steel and iron ore pelletizing industries were the main contributor to one of the eight locations whereas resuspension, civil construction, and vehicular sources were also very important contributors to the other stations. Quarries and soil were also considered expressive SPM sources, but at the city periphery. CMB model could differentiate contributions from six industrial source groups: thermoelectric; iron ore, pellet, and pellet furnaces; coal coke and coke oven; sintering, blast furnace, and basic oxygen furnace; and soil, resuspension, and vehicles. However, the CMB model was unable to differentiate between iron ore and pellet stockpiles which are present in both steel and iron ore pelletizing industries. Further characterization of source and SPM might be necessary to aid local authorities in decision-making regarding these two industrial sources.

  2. Source apportionment and source/sink relationships of PAHs in the coastal atmosphere of Chicago and Lake Michigan

    NASA Astrophysics Data System (ADS)

    Simcik, Matt F.; Eisenreich, Steven J.; Lioy, Paul J.

    Multivariate statistical techniques were used to investigate source apportionment and source/sink relationships for polycyclic aromatic hydrocarbons (PAHs) in the urban and adjacent coastal atmosphere of Chicago/Lake Michigan in 1994-1995. The PAH signatures for the atmospheric particle phase, surface water particle phase and sediments indicate that atmospheric deposition is the major source of PAHs to the sediments and water column particulate phase of Lake Michigan. The PAH signature for the atmospheric gas phase and water dissolved phase indicate an intimate linkage between the lake and its overlying atmosphere. A modified factor analysis-multiple regression model was successfully applied to the source apportionment of atmospheric PAHs (gas+particle). Coal combustion accounted for 48±5% of the ΣPAH concentration in both the urban and adjacent coastal atmosphere, natural gas combustion accounted for 26±2%, coke ovens accounted for 14±3%, and vehicle emissions (gas+diesel) accounted for 9±4%. Each is an identified source category for the region. These results are consistent with the mix of fossil fuel combustion sources and ratios of indicator PAHs.

  3. Fine Particulate Pollution and Source Apportionment in the Urban Centers for Africa, Asia and Latin America

    NASA Astrophysics Data System (ADS)

    Guttikunda, S. K.; Johnson, T. M.; Procee, P.

    2004-12-01

    Fossil fuel combustion for domestic cooking and heating, power generation, industrial processes, and motor vehicles are the primary sources of air pollution in the developing country cities. Over the past twenty years, major advances have been made in understanding the social and economic consequences of air pollution. In both industrialized and developing countries, it has been shown that air pollution from energy combustion has detrimental impacts on human health and the environment. Lack of information on the sectoral contributions to air pollution - especially fine particulates, is one of the typical constraints for an effective integrated urban air quality management program. Without such information, it is difficult, if not impossible, for decision makers to provide policy advice and make informed investment decisions related to air quality improvements in developing countries. This also raises the need for low-cost ways of determining the principal sources of fine PM for a proper planning and decision making. The project objective is to develop and verify a methodology to assess and monitor the sources of PM, using a combination of ground-based monitoring and source apportionment techniques. This presentation will focus on four general tasks: (1) Review of the science and current activities in the combined use of monitoring data and modeling for better understanding of PM pollution. (2) Review of recent advances in atmospheric source apportionment techniques (e.g., principal component analysis, organic markers, source-receptor modeling techniques). (3) Develop a general methodology to use integrated top-down and bottom-up datasets. (4) Review of a series of current case studies from Africa, Asia and Latin America and the methodologies applied to assess the air pollution and its sources.

  4. A novel approach for apportionment between primary and secondary sources of airborne nitrated polycyclic aromatic hydrocarbons (NPAHs)

    NASA Astrophysics Data System (ADS)

    Lin, Yan; Qiu, Xinghua; Ma, Yiqiu; Wang, Junxia; Wu, Yusheng; Zeng, Limin; Hu, Min; Zhu, Tong; Zhu, Yifang

    2016-08-01

    Nitrated polycyclic aromatic hydrocarbons (NPAHs) are strong environmental mutagens and carcinogens originating from both primary emissions and secondary reactions in the atmosphere. The sources and the toxicity of different NPAH species could vary greatly; therefore a specie-specific source apportionment is essential to evaluate their health risks and to formulate controlling regulations. However, few studies have reported source apportionment of NPAHs species to date. In this study, we developed an easy-to-perform method for the apportionment of primary versus secondary sources of airborne NPAHs based on the relationship between NPAHs and NO2. After log-transformation of both NPAHs and NO2 concentrations, a slope of β between these two variables was obtained by the linear regression. When β is significantly smaller than 1, it indicates primary emissions while β significantly greater than 1 suggests secondary formation. We have validated this method with data previously collected in Beijing. A good correlation, with R value of 0.57, was observed between results produced by this new method and by Positive Matrix Factorization (PMF). The correlation could be further improved (R = 0.71) if the gas/particle partition of NPAHs is taken into consideration. This developed method enables the source apportionment for individual NPAHs species and could be used to validate the results of other receptor models.

  5. The Analysis of PM2.5 Source Apportionment Technique's Competitiveness in China

    NASA Astrophysics Data System (ADS)

    Qian, K.; Deng, L.; An, Y. B.; Liu, S. Y.; Hao, H. Z.

    Nowadays, people has paid more attention to PM2.5 in various countries of the world. PM2.5 is a kind of particulate matter whose diameter less than 2.5μm, with great damage to environment and public's health. The origin of source apportionment technique is studies of atmospheric particulate matter, it uses two mathematical models, one of them is diffusion model which study the source of pollution, and another one called receptor model which study the pollution of area. In my study, I will analyze the competitiveness of similar technology in various countries by using microscope to analyze shape characteristic, Enrichment Factor Method (EF), Factor Analyze Method (FA), EPA-CMB8.2 Model, combining with the consequence of Improved-source-analysis Technology and Orthogonal matrix decomposition Model.

  6. Comparison of multi-receptor and single-receptor trajectory source apportionment (TSA) methods using artificial sources

    NASA Astrophysics Data System (ADS)

    Lee, Stephanie; Ashbaugh, Lowell

    Two trajectory source apportionment methods were tested using an artificially generated data set to determine their ability to detect the known sources. The residence time or conditional probability method developed by Ashbaugh et al. [1985. A residence time probability analysis of sulfur concentrations at Grand Canyon National Park. Atmospheric Environment 19(8), 1263-1270] uses a single receptor at a time, whereas the new multi-receptor (MURA) method developed here uses several receptors at once in an attempt to detect the sources with higher accuracy. The methods were first tested using a simulation with a single source and then with another simulation using four sources. The ability of the methods to detect the sources was quantified for each simulation. The MURA trajectory method proved to be superior at identifying sources for these simulations.

  7. Measurement, time series analysis and source apportionment of inorganic and organic speciated PM(2.5) air pollution in Denver

    NASA Astrophysics Data System (ADS)

    Dutton, Steven James

    Particulate air pollution has demonstrated significant health effects ranging from worsening of asthma to increased rates of respiratory and cardiopulmonary mortality. These results have prompted the US-EPA to include particulate matter (PM) as one of the six criteria air pollutants regulated under the Clean Air Act. The diverse chemical make-up and physical characteristics of PM make it a challenging pollutant to characterize and regulate. Particulate matter less than 2.5 microns in diameter (PM2.5) has the ability to travel deep into the lungs and therefore has been linked with some of the more significant health effects. The toxicity of any given particle is likely dependent on its chemical composition. The goal of this project has been to chemically characterize a long time series of PM 2.5 measurements collected at a receptor site in Denver to a level of detail that has not been done before on this size data set. This has involved characterization of inorganic ions using ion chromatography, total elemental and organic carbon using thermal optical transmission, and organic molecular marker species using gas chromatography-mass spectrometry. Methods have been developed to allow for daily measurement and speciation for these compounds over a six year period. Measurement methods, novel approaches to uncertainty estimation, time series analysis, spectral and pattern analyses and source apportionment using two multivariate factor analysis models are presented. Analysis results reveal several natural and anthropogenic sources contributing to PM2.5 in Denver. The most distinguishable sources are motor vehicles and biomass combustion. This information will be used in a health effect analysis as part of a larger study called the Denver Aerosol Sources and Health (DASH) study. Such results will inform regulatory decisions and may help create a better understanding of the underlying mechanisms for the observed adverse health effects associated with PM2.5.

  8. Source apportionment of gaseous and particulate PAHs from traffic emission using tunnel measurements in Shanghai, China

    NASA Astrophysics Data System (ADS)

    Liu, Ying; Wang, Siyao; Lohmann, Rainer; Yu, Na; Zhang, Chenkai; Gao, Yi; Zhao, Jianfu; Ma, Limin

    2015-04-01

    Understanding sources and contributions of gaseous and particulate PAHs from traffic-related pollution can provide valuable information for alleviating air contamination from traffic in urban areas. On-road sampling campaigns were comprehensively conducted during 2011-2012 in an urban tunnel of Shanghai, China. 2-3 rings PAHs were abundant in the tunnel's gas and particle phases. Diagnostic ratios of PAHs were statistically described; several were significantly different between the gas and particle phases. Principal component analysis (PCA), positive matrix factorization (PMF), bivariate correlation analysis and multiple linear regression analysis (MLRA) were applied to apportion sources of gaseous and particulate PAHs in the tunnel. Main sources of the gaseous PAHs included evaporative emission of fuel, high-temperature and low-temperature combustion of fuel, accounting for 50-51%, 30-36% and 13-20%, respectively. Unburned fuel particles (56.4-78.3%), high-temperature combustion of fuel (9.5-26.1%) and gas-to-particle condensation (12.2-17.5%) were major contributors to the particulate PAHs. The result reflected, to a large extent, PAH emissions from the urban traffic of Shanghai. Improving fuel efficiency of local vehicles will greatly reduce contribution of traffic emission to atmospheric PAHs in urban areas. Source apportionment of PM10 mass was also performed based on the organic component data. The results showed that high-temperature combustion of fuel and gas-to-particle condensation contributed to 15-18% and 7-8% of PM10 mass, respectively, but 55-57% of the particle mass was left unexplained. Although the results from the PCA and PMF models were comparable, the PMF method is recommended for source apportionment of PAHs in real traffic conditions. In addition, the combination of multivariate statistical method and bivariate correlation analysis is a useful tool to comprehensively assess sources of PAHs.

  9. Source apportionment of ambient VOCS in Mumbai city

    NASA Astrophysics Data System (ADS)

    Srivastava, Anjali

    Air pollution kills almost half a million Asians every year. Most of this pollution is emitted from buses, trucks, motorcycles and other forms of transport. As Asia's cities continue to expand, the rising number of vehicles has resulted in even greater pollution. Amongst the measures available to control, vehicular emission was engine modification, catalytic converters and fuel modifications. Some of these have led to emissions of some hazardous air pollutants (HAP) like volatile organic compounds (VOCs). VOC emission is an area needing attention in air quality management. This paper discusses a study on VOC concentration at major sources like traffic junction, residential area, commercial areas, industrial areas and petrol pumps in Mumbai city. CMB8 Model has been used to apportion VOCs in Mumbai city. It was observed that evaporative emissions dominate in Mumbai. In order to control VOCs in air the management strategy should thus focus on cost effective vapor recovery systems at refueling stations and in vehicles. Effective inspection and maintenance programme can reduce evaporative and exhaust VOC emissions. Modifying certain fuel parameters, like reducing benzene content in petrol will as well reduce VOC content in air. The benzene content in petrol was 3% in the year 2001 in Mumbai. Adulteration also results in high levels of VOCs in air.

  10. SOURCE APPORTIONMENT OF PM 2.5 AND CARBON IN SEATTLE USING CHEMICAL MASS BALANCE AND POSITIVE MATRIX FACTORIZATION

    EPA Science Inventory

    Three years of PM2.5 speciated data were collected and chemically analyzed using the IMPROVE protocol at the Beacon Hill site in Seattle. The data were analyzed by the Chemical Mass Balance Version 8 (CMB8) and Positive Matrix Factorization (PMF) source apportionment models. T...

  11. SOURCE APPORTIONMENT OF PM 2.5 AND CARBON IN SEATTLE USING CHEMICAL MASS BALANCE AND POSITIVE MATRIX FACTORIZATION

    EPA Science Inventory

    Three years of PM2.5 speciated data were collected and chemically analyzed using the IMPROVE protocol at the Beacon Hill site in Seattle. The data were analyzed by the Chemical Mass Balance Version 8 (CMB8) and Positive Matrix Factorization (PMF) source apportionment models. T...

  12. SOURCE APPORTIONMENT OF EXPOSURES TO VOLATILE ORGANIC COMPOUNDS: II. APPLICATION OF RECEPTOR MODELS TO TEAM STUDY DATA. (R826788)

    EPA Science Inventory

    Four receptor-oriented source apportionment models were applied to personal exposure measurements for toxic volatile organic compounds (VOCs). The measurements are from the total exposure assessment methodology studies conducted from 1980 to 1984 in New Jersey (NJ) and Califor...

  13. Characterization and source apportionment of fine particulate sources at Rijeka, Croatia from 2013 to 2015

    NASA Astrophysics Data System (ADS)

    Ivošević, Tatjana; Stelcer, Eduard; Orlić, Ivica; Bogdanović Radović, Iva; Cohen, David

    2016-03-01

    PM2.5 daily aerosol samples were collected in Rijeka, Croatia during period from 6th August 2013 to 29th January 2015. In total, 259 samples were collected on Teflon filters and analyzed by PIXE and PIGE techniques to give information on 21 elements from Na to Pb. Additionally, black carbon was determined with the Laser Integrated Plate Method. Results were statistically evaluated using Positive Matrix Factorization (PMF). Eight major pollution sources: auto, smoke, secondary sulfates, heavy oil combustion, sea spray, road dust, industry iron and soil dust were identified together with their relative contributions in total PM2.5 pollution.

  14. [Source apportionment of soil heavy metals in Jiapigou goldmine based on the UNMIX model].

    PubMed

    Ai, Jian-chao; Wang, Ning; Yang, Jing

    2014-09-01

    The paper determines 16 kinds of metal elements' concentration in soil samples which collected in Jipigou goldmine upper the Songhua River. The UNMIX Model which was recommended by US EPA to get the source apportionment results was applied in this study, Cd, Hg, Pb and Ag concentration contour maps were generated by using Kriging interpolation method to verify the results. The main conclusions of this study are: (1)the concentrations of Cd, Hg, Pb and Ag exceeded Jilin Province soil background values and enriched obviously in soil samples; (2)using the UNMIX Model resolved four pollution sources: source 1 represents human activities of transportation, ore mining and garbage, and the source 1's contribution is 39. 1% ; Source 2 represents the contribution of the weathering of rocks and biological effects, and the source 2's contribution is 13. 87% ; Source 3 is a comprehensive source of soil parent material and chemical fertilizer, and the source 3's contribution is 23. 93% ; Source 4 represents iron ore mining and transportation sources, and the source 4's contribution is 22. 89%. (3)the UNMIX Model results are in accordance with the survey of local land-use types, human activities and Cd, Hg and Pb content distributions.

  15. Source apportionment of exposures to volatile organic compounds. I. Evaluation of receptor models using simulated exposure data

    NASA Astrophysics Data System (ADS)

    Miller, Shelly L.; Anderson, Melissa J.; Daly, Eileen P.; Milford, Jana B.

    Four receptor-oriented source apportionment models were evaluated by applying them to simulated personal exposure data for select volatile organic compounds (VOCs) that were generated by Monte Carlo sampling from known source contributions and profiles. The exposure sources modeled are environmental tobacco smoke, paint emissions, cleaning and/or pesticide products, gasoline vapors, automobile exhaust, and wastewater treatment plant emissions. The receptor models analyzed are chemical mass balance, principal component analysis/absolute principal component scores, positive matrix factorization (PMF), and graphical ratio analysis for composition estimates/source apportionment by factors with explicit restriction, incorporated in the UNMIX model. All models identified only the major contributors to total exposure concentrations. PMF extracted factor profiles that most closely represented the major sources used to generate the simulated data. None of the models were able to distinguish between sources with similar chemical profiles. Sources that contributed <5% to the average total VOC exposure were not identified.

  16. Space-time quantitative source apportionment of soil heavy metal concentration increments.

    PubMed

    Yang, Yong; Christakos, George; Guo, Mingwu; Xiao, Lu; Huang, Wei

    2017-04-01

    Assessing the space-time trends and detecting the sources of heavy metal accumulation in soils have important consequences in the prevention and treatment of soil heavy metal pollution. In this study, we collected soil samples in the eastern part of the Qingshan district, Wuhan city, Hubei Province, China, during the period 2010-2014. The Cd, Cu, Pb and Zn concentrations in soils exhibited a significant accumulation during 2010-2014. The spatiotemporal Kriging technique, based on a quantitative characterization of soil heavy metal concentration variations in terms of non-separable variogram models, was employed to estimate the spatiotemporal soil heavy metal distribution in the study region. Our findings showed that the Cd, Cu, and Zn concentrations have an obvious incremental tendency from the southwestern to the central part of the study region. However, the Pb concentrations exhibited an obvious tendency from the northern part to the central part of the region. Then, spatial overlay analysis was used to obtain absolute and relative concentration increments of adjacent 1- or 5-year periods during 2010-2014. The spatial distribution of soil heavy metal concentration increments showed that the larger increments occurred in the center of the study region. Lastly, the principal component analysis combined with the multiple linear regression method were employed to quantify the source apportionment of the soil heavy metal concentration increments in the region. Our results led to the conclusion that the sources of soil heavy metal concentration increments should be ascribed to industry, agriculture and traffic. In particular, 82.5% of soil heavy metal concentration increment during 2010-2014 was ascribed to industrial/agricultural activities sources. Using STK and SOA to obtain the spatial distribution of heavy metal concentration increments in soils. Using PCA-MLR to quantify the source apportionment of soil heavy metal concentration increments. Copyright © 2017

  17. Stream nitrogen sources apportionment and pollution control scheme development in an agricultural watershed in eastern China.

    PubMed

    Chen, Dingjiang; Lu, Jun; Huang, Hong; Liu, Mei; Gong, Dongqin; Chen, Jiabo

    2013-08-01

    A modeling system that couples a land-usebased export coefficient model, a stream nutrient transport equation, and Bayesian statistics was developed for stream nitrogen source apportionment. It divides a watershed into several sub-catchments, and then considers the major landuse categories as stream nitrogen sources in each subcatchment. The runoff depth and stream water depth are considered as the major factors influencing delivery of nitrogen from land to downstream stream node within each sub-catchment. The nitrogen sources and delivery processes are lumped into several constant parameters that were calibrated using Bayesian statistics from commonly available stream monitoring and land-use datasets. This modeling system was successfully applied to total nitrogen (TN) pollution control scheme development for the ChangLe River watershed containing six sub-catchments and four land-use categories. The temporal (across months and years) and spatial (across sub-catchments and land-use categories) variability of nonpoint source (NPS) TN export to stream channels and delivery to the watershed outlet were assessed. After adjustment for in-stream TNretention, the time periods and watershed areas with disproportionately high-TN contributions to the stream were identified. Aimed at a target stream TN level of 2 mg L-1, a quantitative TN pollution control scheme was further developed to determine which sub-catchments, which land-use categories in a sub-catchment, which time periods, and how large of NPS TN export reduction were required. This modeling system provides a powerful tool for stream nitrogen source apportionment and pollution control scheme development at the watershed scale and has only limited data requirements.

  18. Source apportionment based on an atmospheric dispersion model and multiple linear regression analysis

    NASA Astrophysics Data System (ADS)

    Fushimi, Akihiro; Kawashima, Hiroto; Kajihara, Hideo

    Understanding the contribution of each emission source of air pollutants to ambient concentrations is important to establish effective measures for risk reduction. We have developed a source apportionment method based on an atmospheric dispersion model and multiple linear regression analysis (MLR) in conjunction with ambient concentrations simultaneously measured at points in a grid network. We used a Gaussian plume dispersion model developed by the US Environmental Protection Agency called the Industrial Source Complex model (ISC) in the method. Our method does not require emission amounts or source profiles. The method was applied to the case of benzene in the vicinity of the Keiyo Central Coastal Industrial Complex (KCCIC), one of the biggest industrial complexes in Japan. Benzene concentrations were simultaneously measured from December 2001 to July 2002 at sites in a grid network established in the KCCIC and the surrounding residential area. The method was used to estimate benzene emissions from the factories in the KCCIC and from automobiles along a section of a road, and then the annual average contribution of the KCCIC to the ambient concentrations was estimated based on the estimated emissions. The estimated contributions of the KCCIC were 65% inside the complex, 49% at 0.5-km sites, 35% at 1.5-km sites, 20% at 3.3-km sites, and 9% at a 5.6-km site. The estimated concentrations agreed well with the measured values. The estimated emissions from the factories and the road were slightly larger than those reported in the first Pollutant Release and Transfer Register (PRTR). These results support the reliability of our method. This method can be applied to other chemicals or regions to achieve reasonable source apportionments.

  19. Characterization of Arctic elemental carbon in Barrow, AK using radiocarbon source apportionment

    NASA Astrophysics Data System (ADS)

    Barrett, T. E.; Usenko, S.; Robinson, E. M.; Sheesley, R. J.

    2013-12-01

    Currently, the Arctic is one of the fastest warming regions on earth with surface temperatures increasing at a rate nearly double the global mean over recent decades. Despite the fact that atmospheric concentrations of elemental carbon (EC) are lower in the Arctic than in lower latitudes, deposition of EC on snow and ice may exacerbate regional warming by simultaneously decreasing albedo and increasing melt rates. Due to the intensifying Arctic oil exploration in areas such as the Beaufort and Chukchi seas, the impact of new emission sources such as heavy fuel and heavy diesel combustion on regional carbon needs to be assessed. The first step in developing mitigation strategies for reducing current and future EC emissions in the Arctic is to determine emission source contributions. This study aims to determine the relative contributions of fossil fuel and biomass combustion and to identify major source regions of EC to the Arctic. Radiocarbon analysis of both total organic carbon (TOC) and EC combined with organic tracer and back trajectory analysis has been applied to a set of wintertime coarse particulate matter (PM10) samples from Barrow, AK. Preliminary apportionment for January 2013 indicates roughly half of TOC is from biogenic/biomass burning emissions and one third of EC is due to biomass burning emissions. The radiocarbon results will be combined with organic tracer analysis (polycyclic aromatic hydrocarbons, petroleum biomarkers and normal alkanes), increasing the specificity of the relative contribution of both the fossil and modern (biogenic/biomass burning) carbon emission sources. This research represents the first reported radiocarbon values for Arctic EC, providing highly conclusive source apportionment prior to the influence of increased drilling operations and ship traffic in the Beaufort and Chukchi seas.

  20. Source apportionment of trace metals in river sediments: A comparison of three methods.

    PubMed

    Chen, Haiyang; Teng, Yanguo; Li, Jiao; Wu, Jin; Wang, Jinsheng

    2016-04-01

    Increasing trace metal pollution in river sediment poses a significant threat to watershed ecosystem health. Identifying potential sources of sediment metals and apportioning their contributions are of key importance for proposing prevention and control strategies of river pollution. In this study, three advanced multivariate receptor models, factor analysis with nonnegative constraints (FA-NNC), positive matrix factorization (PMF), and multivariate curve resolution weighted-alternating least-squares (MCR-WALS), were comparatively employed for source apportionment of trace metals in river sediments and applied to the Le'an River, a main tributary of Poyang Lake which is the largest freshwater lake in China. The pollution assessment with contamination factor and geoaccumulation index suggested that the river sediments in Le'an River were contaminated severely by trace metals due to human activities. With the three apportionment tools, similar source profiles of trace metals in sediments were extracted. Especially, the MCR-WALS and PMF models produced essentially the same results. Comparatively speaking, the weighted schemes might give better solutions than the unweighted FA-NNC because the uncertainty information of environmental data was considered by PMF and MCR-WALS. Anthropogenic sources were apportioned as the most important pollution sources influencing the sediment metals in Le'an River with contributions of about 90%. Among them, copper tailings occupied the largest contribution (38.4-42.2%), followed by mining wastewater (29.0-33.5%), and agricultural activities (18.2-18.7%). To protect the ecosystem of Le'an River and Poyang Lake, special attention should be paid to the discharges of mining wastewater and the leachates of copper tailing ponds in that region.

  1. Monitoring and source apportionment of trace elements in PM2.5: Implications for local air quality management.

    PubMed

    Li, Yueyan; Chang, Miao; Ding, Shanshan; Wang, Shiwen; Ni, Dun; Hu, Hongtao

    2017-03-08

    Fine particulate matter (PM2.5) samples were collected simultaneously every hour in Beijing between April 2014 and April 2015 at five sites. Thirteen trace elements (TEs) in PM2.5 were analyzed by online X-ray fluorescence (XRF). The annual average PM2.5 concentrations ranged from 76.8 to 102.7 μg m(-3). TEs accounted for 5.9%-8.7% of the total PM2.5 mass with Cl, S, K, and Si as the most dominant elements. Spearman correlation coefficients of PM2.5 or TE concentrations between the background site and other sites showed that PM2.5 and some element loadings were affected by regional and local sources, whereas Cr, Si, and Ni were attributed to substantial local emissions. Temporal variations of TEs in PM2.5 were significant and provided information on source profiles. The PM2.5 concentrations were highest in autumn and lowest in summer. Mn and Cr showed similar variation. Fe, Ca, Si, and Ti tended to show higher concentrations in spring, whereas concentrations of S peaked in summer. Concentrations of Cl, K, Pb, Zn, Cu, and Ni peaked in winter. PM2.5 and TE median concentrations were higher on Saturdays than on weekdays. The diurnal pattern of PM2.5 and TE median concentrations yielded similar bimodal patterns. Five dominant sources of PM2.5 mass were identified via positive matrix factorization (PMF). These sources included the regional and local secondary aerosols, traffic, coal burning, soil dust, and metal processing. Air quality management strategies, including regional environmental coordination and collaboration, reduction in secondary aerosol precursors, restrictive vehicle emission standards, promotion of public transport, and adoption of clean energy, should be strictly implemented. High time-resolution measurements of TEs provided detailed source profiles, which can greatly improve precision in interpreting source apportionment calculations; the PMF analysis of online XRF data is a powerful tool for local air quality management.

  2. [Characteristics and source apportionment of volatile organic compounds (VOCs) in the northern suburb of Nanjing].

    PubMed

    An, Jun-lin; Zhu, Bin; Wang, Hong-lei; Yang, Hui

    2014-12-01

    Based on the data of volatile organic compounds (VOCs) collected continuously from 1st Mar, 2011 to 29th Feb, 2012 in the northern suburb of Nanjing, characteristics of their variability, differences of ratios of tracers and source apportionment by principal component analysis/absolute principal component scores (PCA/APCS) were analyzed. The results showed that the total VOCs mixing ratios were 43.52 x 10(-9), which accounted for 45.1% of alkanes, alkenes for 25.3%, alkyne for 7.3%, and aromatics for 22.3%. There was an obviously seasonal variation of VOCs, with the maximum in summer and the minimum in winter. There was an obvious seasonal variation of VOCs component, with highest alkanes in winter, highest alkenes in summer, highest aromatic in spring, and highest alkyne in winter. By using the specific pollutant ratios ( hydrocarbons/acetylene and toluene/benzene) method, it indicated that the observation site was greatly affected by the surrounding industrial areas. Source analysis of VOCs by PCA/APCS mode showed that the sources consisted of industrial production sources, automobile emission sources, combustion sources, industrial production volatilization sources, solvent use sources and biogenic emission sources. In addition, there were seasonal variations. Overall, the sources related to industrial production activities represented 45% - 63% of VOCs, and they were followed by automobile emission sources, which represented 34% - 50%.

  3. Source apportionment of mercury in dust fallout at urban residential area of Central India

    NASA Astrophysics Data System (ADS)

    Pervez, S.; Balakrishna, G.; Tiwari, S.

    2009-10-01

    The components and quantities of atmospheric dust fallout have been reported to be the pollution indicator of large urban areas. The multiplicity and complexity of sources of atmospheric dusts in urban regions (e.g. industrial complexes composed of a variety of industrial processes, automobiles, construction activities etc.) has put forward the need of source apportionment of these sources indicating their contribution to specific environmental receptor. The study presented here is focused on investigation of source contribution estimates of Mercury in urban dust fallout in an urban-industrial area, Raipur, India. Source-receptor based representative sampling plan using longitudinal study design has been adopted. Six sampling sites have been identified on the basis of land use for development plan of anthropogenic activities and factors related to the transportation and dispersion pattern of atmospheric dusts. 24 samples of dust fallout has been collected from each site (one in each month) and subjected to chemical analysis of selected chemical constituents known as markers of selected major dust emitting sources (Steel making average, Road traffic-borne dusts, construction activities, Auto mobile exhaust, and soils). Chemical composition of dust measured at sites marked for identified sources alongwith SPECIATE of USEPA has been used for the preparation of source profiles. Three classified residential receptors (ambient-outdoor, house-indoors and local street-outdoors) have been chosen for development of receptor compositional profiles. Source apportionment has been done using Chemical Mass Balance (CMB 8). Good fit parameters and relative source contribution has been analysed and documented. Dust fallout and respective mercury levels were found tobe higher compared to prescribed standards. Variation in relative contribution of selected sources from site to site within the study area has been occurred. Dominance of local line and area sources (road-traffic and

  4. Spatial distribution and source apportionment of PAHs in surficial sediments of the Yangtze Estuary, China.

    PubMed

    Li, Baohua; Feng, Chenghong; Li, Xue; Chen, Yaxin; Niu, Junfeng; Shen, Zhenyao

    2012-03-01

    Spatial distribution and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in the surface sediments of the Yangtze Estuary, especially the North Branch, have been fully investigated. PAH concentrations increased with the descending distance from the inner estuary to the adjacent sea, and varied significantly in various estuarine regions. Water currents (e.g., river runoff and ocean current) greatly affected the distribution pattern. In addition, ambient sewage and traffic also contributed to the PAH pollution in the estuary. In the adjacent sea, PAH values along the -20m isobath were higher than those along the -10m isobath due to the "marginal filter" phenomenon formed by different water currents. In most sites, PAHs had poor correlations with sediment size, but had positive correlations with total organic carbon. Based on the qualitative and quantitative analysis results, PAH sources were proved to be mainly from a mixture of petroleum combustion, biomass, and coal combustion. Copyright © 2011 Elsevier Ltd. All rights reserved.

  5. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2015-01-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9% and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/z 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ~10 years of meteorological, particle composition, and fire data.

  6. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2014-07-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9 and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/zs 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time (LST) when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ∼10 years of meteorological, particle composition, and fire data.

  7. Comparison of the MURA and an improved single-receptor (SIRA) trajectory source apportionment (TSA) method using artificial sources

    NASA Astrophysics Data System (ADS)

    Lee, Stephanie; Ashbaugh, Lowell

    Two trajectory source apportionment methods were tested using an artificially generated data set to determine their ability to detect the known sources. The forward-looking step from the multi-receptor trajectory analysis (MURA) method was added to the conditional probability (CP)method of Ashbaugh et al. [1985. A residence time probability analysis of sulfur concentrations at Grand Canyon National Park. Atmospheric Environment 19(8), 1263-1270] to develop the single-receptor forward CP (SIRA) method. The multi-receptor (MURA) and the SIRA methods were tested with three simulations using artificially generated sources. The ability of the methods to detect the sources was quantified for each simulation. The first simulation showed that the SIRA method is an improvement over the original CP method. The MURA trajectory method proved to be superior at identifying sources for the simulation located in the west and comparable to the SIRA method for the two simulations located in the east.

  8. Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties.

    PubMed

    Xie, Mingjie; Mladenov, Natalie; Williams, Mark W; Neff, Jason C; Wasswa, Joseph; Hannigan, Michael P

    2016-12-19

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites.

  9. Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

    NASA Astrophysics Data System (ADS)

    Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

    2016-12-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites.

  10. Water soluble organic aerosols in the Colorado Rocky Mountains, USA: composition, sources and optical properties

    PubMed Central

    Xie, Mingjie; Mladenov, Natalie; Williams, Mark W.; Neff, Jason C.; Wasswa, Joseph; Hannigan, Michael P.

    2016-01-01

    Atmospheric aerosols have been shown to be an important input of organic carbon and nutrients to alpine watersheds and influence biogeochemical processes in these remote settings. For many remote, high elevation watersheds, direct evidence of the sources of water soluble organic aerosols and their chemical and optical characteristics is lacking. Here, we show that the concentration of water soluble organic carbon (WSOC) in the total suspended particulate (TSP) load at a high elevation site in the Colorado Rocky Mountains was strongly correlated with UV absorbance at 254 nm (Abs254, r = 0.88 p < 0.01) and organic carbon (OC, r = 0.95 p < 0.01), accounting for >90% of OC on average. According to source apportionment analysis, biomass burning had the highest contribution (50.3%) to average WSOC concentration; SOA formation and motor vehicle emissions dominated the contribution to WSOC in the summer. The source apportionment and backward trajectory analysis results supported the notion that both wildfire and Colorado Front Range pollution sources contribute to the summertime OC peaks observed in wet deposition at high elevation sites in the Colorado Rocky Mountains. These findings have important implications for water quality in remote, high-elevation, mountain catchments considered to be our pristine reference sites. PMID:27991554

  11. Source apportionment of PAH in Hamilton Harbour suspended sediments: comparison of two factor analysis methods

    SciTech Connect

    Uwayemi M. Sofowote; Brian E. McCarry; Christopher H. Marvin

    2008-08-15

    A total of 26 suspended sediment samples collected over a 5-year period in Hamilton Harbour, Ontario, Canada and surrounding creeks were analyzed for a suite of polycyclic aromatic hydrocarbons and sulfur heterocycles. Hamilton Harbour sediments contain relatively high levels of polycyclic aromatic compounds and heavy metals due to emissions from industrial and mobile sources. Two receptor modeling methods using factor analyses were compared to determine the profiles and relative contributions of pollution sources to the harbor; these methods are principal component analyses (PCA) with multiple linear regression analysis (MLR) and positive matrix factorization (PMF). Both methods identified four factors and gave excellent correlation coefficients between predicted and measured levels of 25 aromatic compounds; both methods predicted similar contributions from coal tar/coal combustion sources to the harbor (19 and 26%, respectively). One PCA factor was identified as contributions from vehicular emissions (61%); PMF was able to differentiate vehicular emissions into two factors, one attributed to gasoline emissions sources (28%) and the other to diesel emissions sources (24%). Overall, PMF afforded better source identification than PCA with MLR. This work constitutes one of the few examples of the application of PMF to the source apportionment of sediments; the addition of sulfur heterocycles to the analyte list greatly aided in the source identification process. 41 refs., 3 figs., 2 tabs.

  12. Source apportionment of PM(2.5) and selected hazardous air pollutants in Seattle.

    PubMed

    Wu, Chang-fu; Larson, Timothy V; Wu, Szu-Ying; Williamson, John; Westberg, Hal H; Liu, L-J Sally

    2007-11-01

    The potential benefits of combining the speciated PM(2.5) and VOCs data in source apportionment analysis for identification of additional sources remain unclear. We analyzed the speciated PM(2.5) and VOCs data collected at the Beacon Hill in Seattle, WA between 2000 and 2004 with the Multilinear Engine (ME-2) to quantify source contributions to the mixture of hazardous air pollutants (HAPs). We used the 'missing mass', defined as the concentration of the measured total particle mass minus the sum of all analyzed species, as an additional variable and implemented an auxiliary equation to constrain the sum of all species mass fractions to be 100%. Regardless of whether the above constraint was implemented and/or the additional VOCs data were included with the PM(2.5) data, the models identified that wood burning (24%-31%), secondary sulfate (20%-24%) and secondary nitrate (15%-20%) were the main contributors to PM(2.5). Using only PM(2.5) data, the model distinguished two diesel features with the 100% constraint, but identified only one diesel feature without the constraint. When both PM(2.5) and VOCs data were used, one additional feature was identified as the major contributor (26%) to total VOC mass. Adding VOCs data to the speciated PM(2.5) data in source apportionment modeling resulted in more accurate source contribution estimates for combustion related sources as evidenced by the less 'missing mass' percentage in PM(2.5). Using the source contribution estimates, we evaluated the validity of using black carbon (BC) as a surrogate for diesel exhaust. We found that BC measured with an aethalometer at 370 nm and 880 nm had reasonable correlations with the estimated concentrations of diesel particulate matters (r>0.7), as well as with the estimated concentrations of wood burning particles during the heating seasons (r=0.56-0.66). This indicates that the BC is not a unique tracer for either source. The difference in BC between 370 and 880 nm, however, correlated

  13. Source apportionment of biogenic contributions to ozone formation over the United States

    NASA Astrophysics Data System (ADS)

    Zhang, Rui; Cohan, Alexander; Pour Biazar, Arastoo; Cohan, Daniel S.

    2017-09-01

    Vegetation is the leading emitter of volatile organic compounds (VOC), a key ingredient for ozone formation. The contribution of biogenic VOC (BVOC) emissions to regional ozone formation needs better quantification so that air quality regulators can effectively design emission control strategies. One of the key uncertainties for modeling BVOC emissions comes from the estimation of photosynthetically active radiation (PAR) reaching canopy. Satellite insolation retrieval data provide an alternative to prognostic meteorological models for representing the spatial and temporal variations of PAR. In this study, biogenic emission estimates generated with the MEGAN and BEIS biogenic emissions models using satellite or prognostic PAR are used to examine the contribution of BVOC to ozone in the United States. The Comprehensive Air Quality Model with Extensions (CAMx) is applied with Ozone Source Apportionment Technology (OSAT) and brute force zero-out sensitivity runs to quantify the biogenic contributions to ozone formation during May through September 2011. The satellite PAR retrievals are on average lower than modeled PAR and exhibit better agreement with SCAN and SURFRAD network measurements. Using satellite retrievals instead of modeled PAR reduces BEIS and MEGAN estimates of isoprene by an average of 3%-4% and 9%-12%, respectively. The simulations still overestimate observed ground-level isoprene concentrations by a factor of 1.1 for BEIS and 2.6 for MEGAN. The spatial pattern of biogenic ozone contribution diagnosed from OSAT differs from the brute force zero-out sensitivity results, with the former more smoothly distributed and the latter exhibiting peak impacts near metropolitan regions with intense anthropogenic NOx emissions. OSAT tends to apportion less ozone to biogenics as BVOC emissions increase, since that shifts marginal ozone formation toward more NOx-limited conditions. By contrast, zero-out source apportionment of ozone to biogenics increases with BVOC

  14. Source apportionment of fine and coarse particles at a roadside and urban background site in London during the 2012 summer ClearfLo campaign.

    PubMed

    Crilley, Leigh R; Lucarelli, Franco; Bloss, William J; Harrison, Roy M; Beddows, David C; Calzolai, Giulia; Nava, Silvia; Valli, Gianluigi; Bernardoni, Vera; Vecchi, Roberta

    2017-01-01

    London, like many major cities, has a noted air pollution problem, and a better understanding of the sources of airborne particles in the different size fractions will facilitate the implementation and effectiveness of control strategies to reduce air pollution. Thus, the trace elemental composition of the fine and coarse fraction were analysed at hourly time resolution at urban background (North Kensington, NK) and roadside (Marylebone Road, MR) sites within central London. Unlike previous work, the current study focuses on measurements during the summer providing a snapshot of contributing sources, utilising the high time resolution to improve source identification. Roadside enrichment was observed for a large number of elements associated with traffic emissions (Al, S, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Rb and Zr), while those elements that are typically from more regional sources (e.g. Na, Cl, S and K) were not found to have an appreciable increment. Positive Matrix Factorization (PMF) was applied for the source apportionment of the particle mass at both sites with similar sources being identified, including sea salt, airborne soil, traffic emissions, secondary inorganic aerosols and a Zn-Pb source. In the fine fraction, traffic emissions was the largest contributing source at MR (31.9%), whereas it was incorporated within an "urban background" source at NK, which had contributions from wood smoke, vehicle emissions and secondary particles. Regional sources were the major contributors to the coarse fraction at both sites. Secondary inorganic aerosols (which contained influences from shipping emissions and coal combustion) source factors accounted for around 33% of the PM10 at NK and were found to have the highest contributions from regional sources, including from the European mainland. Exhaust and non-exhaust sources both contribute appreciably to PM10 levels at the MR site, highlighting the continuing importance of vehicle-related air pollutants at

  15. Source apportionment of airborne particulate matter using organic compounds as tracers

    NASA Astrophysics Data System (ADS)

    Schauer, James J.; Rogge, Wolfgang F.; Hildemann, Lynn M.; Mazurek, Monica A.; Cass, Glen R.; Simoneit, Bernd R. T.

    A chemical mass balance receptor model based on organic compounds has been developed that relates source contributions to airborne fine particle mass concentrations. Source contributions to the concentrations of specific organic compounds are revealed as well. The model is applied to four air quality monitoring sites in southern California using atmospheric organic compound concentration data and source test data collected specifically for the purpose of testing this model. The contributions of up to nine primary particle source types can be separately identified in ambient samples based on this method, and approximately 85% of the organic fine aerosol is assigned to primary sources on an annual average basis. The model provides information on source contributions to fine mass concentrations, fine organic aerosol concentrations and individual organic compound concentrations. The largest primary source contributors to fine particle mass concentrations in Los Angeles are found to include diesel engine exhaust, paved road dust, gasoline-powered vehicle exhaust, plus emissions from food cooking and wood smoke, with smaller contribution from tire dust, plant fragments, natural gas combustion aerosol, and cigarette smoke. Once these primary aerosol source contributions are added to the secondary sulfates, nitrates and organics present, virtually all of the annual average fine particle mass at Los Angeles area monitoring sites can be assigned to its source.

  16. Quantitative identification and source apportionment of anthropogenic heavy metals in marine sediment of Hong Kong

    NASA Astrophysics Data System (ADS)

    Zhou, Feng; Guo, Huaicheng; Liu, Lei

    2007-10-01

    Based on ten heavy metals collected twice annually at 59 sites from 1998 to 2004, enrichment factors (EFs), principal component analysis (PCA) and multivariate linear regression of absolute principal component scores (MLR-APCS) were used in identification and source apportionment of the anthropogenic heavy metals in marine sediment. EFs with Fe as a normalizer and local background as reference values was properly tested and suitable in Hong Kong, and Zn, Ni, Pb, Cu, Cd, Hg and Cr mainly originated from anthropogenic sources, while Al, Mn and Fe were derived from rocks weathering. Rotated PCA and GIS mapping further identified two types of anthropogenic sources and their impacted regions: (1) electronic industrial pollution, riparian runoff and vehicle exhaust impacted the entire Victoria Harbour, inner Tolo Harbour, Eastern Buffer, inner Deep Bay and Cheung Chau; and (2) discharges from textile factories and paint, influenced Tsuen Wan Bay and Kwun Tong typhoon shelter and Rambler Channel. In addition, MLR-APCS was successfully introduced to quantitatively determine the source contributions with uncertainties almost less than 8%: the first anthropogenic sources were responsible for 50.0, 45.1, 86.6, 78.9 and 87.5% of the Zn, Pb, Cu, Cd and Hg, respectively, whereas 49.9% of the Ni and 58.4% of the Cr came from the second anthropogenic sources.

  17. Chemical characterization and source apportionment of fine and coarse particulate matter in Lahore, Pakistan

    NASA Astrophysics Data System (ADS)

    Stone, Elizabeth; Schauer, James; Quraishi, Tauseef A.; Mahmood, Abid

    2010-03-01

    Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM 2.5 and PM 10) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (±one standard deviation) of PM 2.5 was 194 ± 94 μg m -3 and PM 10 was 336 ± 135 μg m -3. Coarse aerosol (PM 10-2.5) was dominated by crustal sources like dust (74 ± 16%, annual average ± one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 ± 17%). Organic tracer species were used to identify sources of PM 2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 ± 19%). Lesser sources included biomass burning (10 ± 5%) and the combined source of diesel engines and residual fuel oil combustion (6 ± 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 ± 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 ± 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity.

  18. Source apportionment of airborne particulate matter using organic compounds as tracers

    NASA Astrophysics Data System (ADS)

    Schauer, James J.; Rogge, Wolfgang F.; Hildemann, Lynn M.; Mazurek, Monica A.; Cass, Glen R.; Simoneit, Bernd R. T.

    A chemical mass balance receptor model based on organic compounds has been developed that relates sours; contributions to airborne fine particle mass concentrations. Source contributions to the concentrations of specific organic compounds are revealed as well. The model is applied to four air quality monitoring sites in southern California using atmospheric organic compound concentration data and source test data collected specifically for the purpose of testing this model. The contributions of up to nine primary particle source types can be separately identified in ambient samples based on this method, and approximately 85% of the organic fine aerosol is assigned to primary sources on an annual average basis. The model provides information on source contributions to fine mass concentrations, fine organic aerosol concentrations and individual organic compound concentrations. The largest primary source contributors to fine particle mass concentrations in Los Angeles are found to include diesel engine exhaust, paved road dust, gasoline-powered vehicle exhaust, plus emissions from food cooking and wood smoke, with smaller contribution:; from tire dust, plant fragments, natural gas combustion aerosol, and cigarette smoke. Once these primary aerosol source contributions are added to the secondary sulfates, nitrates and organics present, virtually all of the annual average fine particle mass at Los Angeles area monitoring sites can be assigned to its source.

  19. Fine particulate matter (PM2.5) in Edmonton, Canada: Source apportionment and potential risk for human health.

    PubMed

    Bari, Md Aynul; Kindzierski, Warren B

    2016-11-01

    To design effective PM2.5 control strategies in urban centers, there is a need to better understand local and remote sources influencing PM2.5 levels and associated risk to public health. An investigation of PM2.5 levels, sources and potential human health risk associated with trace elements in the PM2.5 was undertaken in Edmonton over a 6-year period (September 2009-August 2015). The geometric mean PM2.5 concentration of was 7.11 μg/m(3) (interquartile range, IQR = 4.83-10.08 μg/m(3)). Positive matrix factorization (PMF) receptor modeling identified secondary organic aerosol (SOA) as the major contributor (2.2 μg/m(3), 27%), followed by secondary nitrate (1.3 μg/m(3), 17%) and secondary sulfate (1.2 μg/m(3), 15%). Other local sources included transportation (1.1 μg/m(3), 14%) and industry-related emissions (0.26 μg/m(3), 3.4%), biomass burning (1.0 μg/m(3), 13%) and soil (0.54 μg/m(3), 6.8%). Five factors (i.e., SOA, secondary nitrate, secondary sulfate, transportation and biomass burning) contributed more than 85% to PM2.5 for the 2009-2015 period. Geometric (arithmetic) mean and maximum ambient air concentrations for hazardous trace elements of public health concern in PM2.5 during the study period were below United States regulatory agency chronic and acute health risk screening criteria. Carcinogenic and non-carcinogenic risk of trace elements and source-specific risk values were well below acceptable and safe levels of risks recommended by regulatory agencies. More work is needed to understand the origin of potential SOA and wintertime wood burning sources in Edmonton and the surrounding region and to apply source-risk apportionment using all available hazardous air pollutants (HAPs) including organic compounds to better interpret the potential health risk posed by various sources in urban areas.

  20. Source apportionment of PM₂.₅ at the coastal area in Korea.

    PubMed

    Choi, Jong-Kyu; Heo, Jong-Bae; Ban, Soo-Jin; Yi, Seung-Muk; Zoh, Kyung-Duk

    2013-03-01

    In this study, we analyzed the chemical composition of fine particulate matter 2.5 μm or less (PM) collected at Incheon, the coastal area in Seoul, Korea every third day from June 2009 to May 2010. Based on the analyzed chemical species in the PM samples, the sources of PM were identified using a positive matrix factorization (PMF). Nine sources of PM were determined from PMF analysis. The major sources of PM were secondary nitrate (25.4%), secondary sulfate (19.0%), motor vehicle 1 (14.8%) with a lesser contribution from industry (8.5%), motor vehicle 2 (8.2%), biomass burning (6.1%), soil (6.1%), combustion and copper production emissions (6.1%), and sea salt (5.9%). From a paired t-test, it was found that yellow sand samples were characterized as having higher contribution from soil sources (p<0.05). Furthermore, the likely source areas of PM emissions were determined using the conditional probability function (CPF) and the potential source contribution function (PSCF). CPF analysis identified the likely local sources of PM as motor vehicles and sea salt. PSCF analysis indicated that the likely source areas for secondary particles (sulfate and nitrate) were the major industrial areas in China. Finally, using the source contribution of PM and associated organic composition data, principal component analysis (PCA) was conducted to evaluate the accuracy of the PM source apportionments by PMF. The PCA analysis confirmed eight of the nine PM sources. Our result implies that the chemical composition analysis of PM data and various modeling techniques can effectively identify the potential contributing sources. Copyright © 2012 Elsevier B.V. All rights reserved.

  1. Multiple-year black carbon measurements and source apportionment using delta-C in Rochester, New York.

    PubMed

    Wang, Yungang; Hopke, Philip K; Rattigan, Oliver V; Chalupa, David C; Utell, Mark J

    2012-08-01

    Black carbon (BC), an important component ofthe atmospheric aerosol, has climatic, environmental, and human health significance. In this study, BC was continuously measured using a two-wavelength aethalometer (370 nm and 880 nm) in Rochester; New York, from January 2007 to December 2010. The monitoring site is adjacent to two major urban highways (I-490 and I-590), where 14% to 21% of the total traffic was heavy-duty diesel vehicles. The annual average BC concentrations were 0.76 microg/m3, 0.67 microg/m3, 0.60 microg/m3, and 0.52 microg/m3 in 2007, 2008, 2009, and 2010, respectively. Positive matrix factorization (PMF) modeling was performed using PM2.5 elements, sulfate, nitrate, ammonia, elemental carbon (EC), and organic carbon (OC) data from the US. Environmental Protection Agency (EPA) speciation network and Delta-C (UVBC370nm-BC880nm) data. Delta-C has been previously shown to be a tracer of wood combustion factor It was used as an input variable in source apportionment models for the first time in this study and was found to play an important role in separating traffic (especially diesel) emissions from wood combustion emissions. The result showed the annual average PM2.5 concentrations apportioned to diesel emissions in 2007, 2008, 2009, and 2010 were 1.34 microg/m3, 1.25 microg/m3, 1.13 microg/m3, and 0.97 microg/m3, respectively. The BC conditional probability function (CPF) plots show a large contribution from the highway diesel traffic to elevated BC concentrations. The measurements and modeling results suggest an impact of the US Environmental Protection Agency (EPA) 2007 Heavy-Duty Highway Rule on the decrease ofBC and PM2.5 concentrations during the study period.

  2. Characterization and source apportionment of water pollution in Jinjiang River, China.

    PubMed

    Chen, Haiyang; Teng, Yanguo; Yue, Weifeng; Song, Liuting

    2013-11-01

    Characterizing water quality and identifying potential pollution sources could greatly improve our knowledge about human impacts on the river ecosystem. In this study, fuzzy comprehensive assessment (FCA), pollution index (PI), principal component analysis (PCA), and absolute principal component score-multiple linear regression (APCS-MLR) were combined to obtain a deeper understanding of temporal-spatial characterization and sources of water pollution with a case study of the Jinjiang River, China. Measurement data were obtained with 17 water quality variables from 20 sampling sites in the December 2010 (withered water period) and June 2011 (high flow period). FCA and PI were used to comprehensively estimate the water quality variables and compare temporal-spatial variations, respectively. Rotated PCA and receptor model (APCS-MLR) revealed potential pollution sources and their corresponding contributions. Application results showed that comprehensive application of various multivariate methods were effective for water quality assessment and management. In the withered water period, most sampling sites were assessed as low or moderate pollution with characteristics pollutants of permanganate index and total nitrogen (TN), whereas 90% sites were classified as high pollution in the high flow period with higher TN and total phosphorus. Agricultural non-point sources, industrial wastewater discharge, and domestic sewage were identified as major pollution sources. Apportionment results revealed that most variables were complicatedly influenced by industrial wastewater discharge and agricultural activities in withered water period and primarily dominated by agricultural runoff in high flow period.

  3. Development of a chemical source apportionment decision support framework for catchment management.

    PubMed

    Comber, Sean D W; Smith, Russell; Daldorph, Peter; Gardner, Michael J; Constantino, Carlos; Ellor, Brian

    2013-09-03

    EU legislation, including the Water Framework Directive, has led to the application of increasingly stringent quality standards for a wide range of chemical contaminants in surface waters. This has raised the question of how to determine and to quantify the sources of such substances so that measures can be taken to address breaches of these quality standards using the polluter pays principle. Contaminants enter surface waters via a number of diffuse and point sources. Decision support tools are required to assess the relative magnitudes of these sources and to estimate the impacts of any programmes of measures. This work describes the development and testing of a modeling framework, the Source Apportionment Geographical Information System (SAGIS). The model uses readily available national data sets to estimate contributions of a number of nutrients (nitrogen and phosphorus), metals (copper, zinc, cadmium, lead, mercury, and nickel) and organic chemicals (a phthalate and a number of polynuclear aromatic hydrocarbons) from multiple sector sources. Such a tool has not previously been available on a national scale for such a wide range of chemicals. It is intended to provide a common platform to assist stakeholders in future catchment management.

  4. Chemical mass balance source apportionment of PM 10 in an industrialized urban area of Northern Greece

    NASA Astrophysics Data System (ADS)

    Samara, C.; Kouimtzis, Th; Tsitouridou, R.; Kanias, G.; Simeonov, V.

    Ambient PM 10 were sampled at three sites in an industrialized urban area of Northern Greece during June 1997-June 1998 and analyzed for 17 chemical elements, 5 water-soluble ions and 13 polycyclic aromatic hydrocarbons. In addition, chemical source profiles consisting of the same particulate components were obtained for a number of industrial activities (cement, fertilizer and asphalt production, quarry operations, metal electroplating, metal welding and tempering, steel manufacture, lead and bronze smelters, metal scrap incineration), residential oil burning, non-catalyst and catalyst-equipped passenger cars, diesel fuelled taxis and buses, as well as for geological fugitive sources (paved road dust and soil from open lands). Ambient and source data were used in a chemical mass balance (CMB) receptor model for source identification and apportionment. Results of CMB modeling showed that major source of ambient PM 10 at all three sites was diesel vehicle exhaust. Significant contribution from industrial oil burning was also evidenced at the site located closest to the industrial area.

  5. Size-resolved source apportionment of particulate matter in urban Beijing during haze and non-haze episodes

    NASA Astrophysics Data System (ADS)

    Tian, S. L.; Pan, Y. P.; Wang, Y. S.

    2016-01-01

    Additional size-resolved chemical information is needed before the physicochemical characteristics and sources of airborne particles can be understood; however, this information remains unavailable in most regions of China due to lacking measurement data. In this study, we report observations of various chemical species in size-segregated particle samples that were collected over 1 year in the urban area of Beijing, a megacity that experiences severe haze episodes. In addition to fine particles, high concentrations of coarse particles were measured during the periods of haze. The abundance and chemical compositions of the particles in this study were temporally and spatially variable, with major contributions from organic matter and secondary inorganic aerosols. The contributions of organic matter to the particle mass decreased from 37.9 to 31.2 %, and the total contribution of sulfate, nitrate and ammonium increased from 19.1 to 33.9 % between non-haze and haze days, respectively. Due to heterogeneous reactions and hygroscopic growth, the peak concentrations of the organic carbon, cadmium and sulfate, nitrate, ammonium, chloride and potassium shifted from 0.43 to 0.65 µm on non-haze days to 0.65-1.1 µm on haze days. Although the size distributions of lead and thallium were similar during the observation period, their concentrations increased by a factor of more than 1.5 on haze days compared with non-haze days. We observed that sulfate and ammonium, which have a size range of 0.43-0.65 µm, sulfate and nitrate, which have a size range of 0.65-1.1 µm, calcium, which has a size range of 5.8-9 µm, and the meteorological factors of relative humidity and wind speed were responsible for haze pollution when the visibility was less than 10 km. Source apportionment using Positive Matrix Factorization showed six PM2.1 sources and seven PM2.1-9 common sources: secondary inorganic aerosol (25.1 % for fine particles vs. 9.8 % for coarse particles), coal combustion (17

  6. AERONET - Aerosol Climatology From Megalopolis Aerosol Source Regions

    NASA Astrophysics Data System (ADS)

    Holben, B. N.; Eck, T. F.; Dubovik, O.; Smirnov, A.; Slutsker, I.; Artaxo, P.; Leyva, A.; Lu, D.; Sano, I.; Singh, R. P.; Quel, E.; Tanre, D.; Zibordi, G.

    2002-05-01

    AERONET is a globally distributed network of ~170 identical sun and sky scanning spectral radiometers expanded by federation with collaborating investigators that contribute to the AERONET public domain data-base. We will detail the current distribution and plans for expanded collaboration. Recent products available through the project database are important for assessment of human health as well as climate forcing issues. We will illustrate a summary of aerosol optical properties measured in Indian, East Asian, North American, South American and European megalopolis source regions. We will present monthly mean fine and coarse particle aerosol optical depth, particle size distributions and single scattering albedos. Each region represents a population in excess of 10 million inhabitants within a 200 km radius of the observation site that dictate the anthropogenic aerosol sources contributing to significantly diverse aerosol properties as a function of economic development and seasonally dependent meteorological processes. The diversity of the measured optical properties of urban aerosols illustrates the need for long-term regional monitoring that contribute to comparative assessments for health and climate change investigations.

  7. Aerosol characterization of a smoldering source

    SciTech Connect

    Mulholland, G.; Ohlemiller, T.J.

    1982-01-01

    The aerosol emitted by a moderately large smoldering combustion source (16 cm in diameter) has been characterized in detail. The fuel is a permeable bed of cellulosic insulation (wood fibers) receiving its primary air supply by flow up from the bottom of the bed while the smolder wave propagates downward. The mass mean particle size of the aerosol is 2-3 ..mu..m; this shows no clear trend with smolder wave depth in the bed or with air flow velocity. The large average particle size is shown to imply that, compared to punk smoke, the present aerosol requires a sevenfold greater concentration to trigger an ionization detector. Coagulation of the aerosol in the plume above the source is shown to be minimal, but substantial coagulation can occur within the source. The apparent fractional conversion of gasified mass (60-75% of the fuel) to aerosol mass decreases with smolder wave depth in the bed and with decreasing air flow rate. The mass and number flow rate of the aerosol show these same trends. The decreasing aerosol emissions with wave depth or air flow rate are plausibly explained by filtration effects in the smolder bed.

  8. Source apportionment and organic compound characterization of ambient ultrafine particulate matter (PM) in the Los Angeles Basin

    NASA Astrophysics Data System (ADS)

    Hasheminassab, Sina; Daher, Nancy; Schauer, James J.; Sioutas, Constantinos

    2013-11-01

    In this study, quasi-UFP (PM0.25, dp < 0.25 μm) were collected for 24 h once per week from April 2008 to March 2009 at 10 different locations in the Los Angeles Basin. Samples were chemically analyzed and organic constituents of PM0.25 were grouped into polycyclic aromatic hydrocarbon (PAHs), hopanes and steranes, n-alkanes, and levoglucosan, with concentration levels ranging from 0.16 to 5.5, 0.09 to 2.2, 9.3 to 48, and 2.2 to 106.2 ng m-3 over all sites and seasons, respectively. A molecular marker-based chemical mass balance (MM-CMB) model was applied to estimate the relative contributions from the following primary sources: mobile sources (combined gasoline and diesel vehicles), wood smoke, natural gas combustion, vegetative detritus, and ship emissions. Secondary organic aerosol (SOA) tracers were not included in the model; however their contributions were estimated from non-biomass burning water soluble organic carbon (WSOCnb) and un-apportioned OC from MM-CMB model (“other OC”). High correlation (R2 = 0.8) between “other OC” and WSOCnb in summer suggests that “other OC” is highly impacted by SOA, however un-apportioned primary sources may contribute to “other OC” as well. Mobile sources were expectedly the major primary contributor to PM0.25, with seasonal average contributions of 31 ± 12% in summer and 57 ± 17% in winter. “Other organic matter” was the second largest contributor to PM0.25 in all seasons, across the basin, with substantially higher contribution during warmer spring and summer seasons (27%), while lowest during cold seasons (13%). Wood smoke was the third major contributor to PM0.25 in winter, whereas its contribution was lowest in summer. As expected, ship emissions displayed the highest contribution at the near-harbor HUD site, and their levels continually decreased as a function of distance from coast. Two other primary sources, vegetative detritus and natural gas combustion, collectively contributed to 1.3 ± 0

  9. Source apportionment of atmospheric particulate matter (PM) using a constrained US-EPA-PMF5.0 model at different urban environments in France

    NASA Astrophysics Data System (ADS)

    Salameh, Dalia; Favez, Olivier; Golly, Benjamin; Besombes, Jean Luc; Alleman, Laurent; Albinet, Alexandre; Jaffrezo, Jean Luc

    2017-04-01

    Particulate matter (PM) is one of the most studied atmospheric pollutant in urban areas due to their adverse effects on human health (Pope et al., 2009). Intrinsic properties of PM (e.g. chemical composition and morphology) are directly linked to their origins. Therefore, a harmonized and comprehensive apportionment study of PM sources in urban environments is extremely required to connect source contributions with PM concentration levels and then develop effective PM abatement strategies. Multivariate receptor models such as Positive Matrix Factorization (PMF) are very useful and have been used worldwide for PM source apportionment (Viana et al., 2008). PMF uses a weighted least-squares fit and quantitatively determines source fingerprints (factors) and their contributions to the total PM mass. However, in many cases, it could be tricky to separate two factors that co-vary due to similar seasonal variations, making unclear the physical sense of the extracted factors. To address such issues of source collinearities, additional specific constraints are incorporated into the model (i.e., constrained PMF) based on user's external knowledge allowing better apportionment results. In this work and within the framework of the SOURCES project, a harmonized source apportionment approach has been implemented and applied for the determination of PM sources on a large number of sites (up to 20) of different typologies (e.g. urban background, industrial, traffic, rural and/or alpine sites) distributed all over France and previously investigated with annual or multiannual studies (2012-2016). A constrained PMF approach (using US-EPA PMF5.0 software) was applied to the comprehensive PM-offline chemical datasets (i.e. carbonaceous fraction, major ions, metals/trace elements, specific organic markers) in a harmonized way for all the investigated sites. Different types of specific chemical constraints from well-characterized sources were defined based on external knowledge and were

  10. Source apportionment of PAHs in dated sediments from the Black River, Ohio.

    PubMed

    Gu, Sheng-He; Kralovec, Andrew C; Christensen, Erik R; Van Camp, Ryan P

    2003-05-01

    Black River, OH, is contaminated with polycyclic aromatic hydrocarbons (PAHs) from coke ovens of a US Steel Corp. Plant. Closing of a coking plant in 1983 and environmental dredging of the sediments during 1989 and 1990 has reduced the PAH levels significantly. This study quantifies the decrease, and consider source apportionment of PAHs in Black River sediments using chemical mass balance modeling. Five vibra cores collected in 1998 and dated using 210Pb and 137Cs, were analyzed for 18 PAHs. The cores had total PAH concentrations between 250 and 0.10 ppm. PAH maxima occur in 1949, 1969, in accordance with regional historical inputs (core BR4), and in 1991 due to remediation (BR6). Coke oven emissions (CO), highway dust (HWY), and wood burning (WB) are likely sources. The CO source (6-92% of total PAHs) is maximal in 1954, and again in 1992-1994 due to the exposure and redistribution of older contaminated sediments during dredging, and decreases thereafter. There is minimal CO content in 1985 (BR4), 2 yr after closure of the coking plant. The HWY contribution (2-86%) is high during 1969-1988, and increases again after 1993. The WB source is less than 23%, and exhibits a minimum (2%) around 1979 (BR4). There is evidence of aerobic biodegradation or photolysis in the sediment of phenanthrene (PhA) at PhA concentrations >500 ppb.

  11. Source apportionment for African dust outbreaks over the Western Mediterranean using the HYSPLIT model

    NASA Astrophysics Data System (ADS)

    Escudero, M.; Stein, A. F.; Draxler, R. R.; Querol, X.; Alastuey, A.; Castillo, S.; Avila, A.

    2011-03-01

    A source apportionment technique has been applied to determine the geographical distribution of emissions in Northern Africa contributing to dust outbreaks that yield high PM10 levels at Spanish regional background stations. Seven dust episodes have been analyzed in this study. Total suspended particles have been sampled and chemically analyzed for these events at La Castanya background station (Montseny, NE Spain) and differences in the composition of airborne dust have been studied. The dominant role of northern and western source areas (Tunisia, Algeria, Mauritania and the Western Sahara) contrasted with the negligible contribution of major emission source areas such as the Bodelé depression, Libya, Niger, and Sudan. During the simulated events using the dust module of the HYSPLIT model, material from the latter regions is persistently transported across the Atlantic but not towards Western Europe. As a consequence, the composition of the dust turned out to be quite homogeneous since the mixing of dust occurs from various source areas with similar chemical composition. However, differences in Ca/Al ratios have been found in a number of samples that are mainly explained by vertical transport segregation of clay minerals (relatively richer in Al) from coarser dust particles (Ca-carbonate).

  12. Source apportionment of Pb pollution in saltmarsh sediments from southwest England

    NASA Astrophysics Data System (ADS)

    Iurian, Andra-Rada; Millward, Geoffrey; Taylor, Alex; Marshall, William; Rodríguez, Javier; Gil Ibarguchi, José Ignacio; Blake, William H.

    2017-04-01

    The local availability of metal resources played a crucial role in Britain's development during the industrial revolution, but centuries of mining within Cornwall and Devon (UK) have left a legacy of contamination in river basin and estuary sediments. Improved knowledge of historical heavy metal sources, emissions and pathways will result in a better understanding of the contemporary pollution conditions and a better protection of the environment from legacy contaminants. Our study aims to trace historical sources of Pb pollution in the area of east Cornwall and west Devon, UK, using a multi proxy approach for contaminants stored in saltmarsh sediment columns from 3 systems characterized by different contamination patterns. Source apportionment investigations included the determination of Pb concentration and Pb isotopic composition (204Pb, 206Pb, 207Pb, and 208Pb) for selected down-core sediment samples, and for local ore and parent rock materials. General trends in pollutant loading (e.g. Pb) could be identified, with maximum inputs occurring in the middle of the 19th century and decreasing towards the present day, while an increase in the catchment disturbance was apparent for the last decades. The isotopic ratios of Pb further indicate that sediments with higher Pb content have a less radiogenic signature, these particular inputs being derived from Pb mining and smelting sources in the catchment area. Acknowledgements: Andra-Rada Iurian acknowledges the support of a Marie Curie Fellowship (H2020-MSCA-IF-2014, Grant Agreement number: 658863) within the Horizon 2020.

  13. Source apportionment of traffic emissions of particulate matter using tunnel measurements

    NASA Astrophysics Data System (ADS)

    Lawrence, Samantha; Sokhi, Ranjeet; Ravindra, Khaiwal; Mao, Hongjun; Prain, Hunter Douglas; Bull, Ian D.

    2013-10-01

    This study aims to quantify exhaust/non-exhaust emissions and the uncertainties associated with them by combining innovative motorway tunnel sampling and source apportionment modelling. Analytical techniques ICP-AES and GC-MS were used to identify the metallic and organic composition of PM10, respectively. Good correlation was observed between Fe, Cu, Mn, Ni, Pb and Sb and change in traffic volume. The concentration of polycyclic aromatic hydrocarbons and other organics varies significantly at the entrance and exit site of the tunnel, with fluoranthene, pyrene, benzo[a]pyrene, chrysene and benzothiazole having the highest incremented concentrations. The application of Principal Component Analysis and Multiple Linear Regression Analysis helped to identify the emission sources for 82% of the total PM10 mass inside the tunnel. Identified sources include resuspension (27%), diesel exhaust emissions (21%), petrol exhaust emissions (12%), brake wear emissions (11%) and road surface wear (11%). This study shows that major health related chemical species of PM10 originate from non-exhaust sources, further signifying the need for legislation to reduce these emissions.

  14. Source apportionment of atmospheric PAHs and their toxicity using PMF: Impact of gas/particle partitioning

    NASA Astrophysics Data System (ADS)

    Gao, Bo; Wang, Xin-Ming; Zhao, Xiu-Ying; Ding, Xiang; Fu, Xiao-Xin; Zhang, Yan-Li; He, Quan-Fu; Zhang, Zhou; Liu, Teng-Yu; Huang, Zou-Zhao; Chen, Lai-Guo; Peng, Yan; Guo, Hai

    2015-02-01

    24-h PM2.5 samples were simultaneously collected at six sites in a subtropical city of South China during November-December, 2009. Particle-phase concentrations of polycyclic aromatic hydrocarbons (PAHs) and organic tracers such as hopanes for vehicular emissions (VE), levoglucosan for biomass burning (BB) and picene for coal combustion (CC) were determined. Meanwhile, their gas-phase concentrations were calculated from gas/particle (G/P) partitioning theory using the particle-phase concentrations. The 4 ring PAHs (fluoranthene to chrysene) had lower particle-phase fractions (10%-79%) than other species. Estimated BaPeq and lifetime cancer risk for particle-only (P-only) vs gas + particle (G + P) data sets showed similar values, indicating PAHs with 5-7 rings dominated the carcinogenicity of PAHs. Positive Matrix Factorization (PMF) was applied on both P-only and G + P data sets to estimate the source contributions to PAHs and their toxicity. Three common sources were identified: VE, BB and CC, with CC as the most significant source for both particulate (58%) and total (G + P, 40%) PAHs. While CC exhibited consistent contributions to BaPeq for P-only (66%) vs G + P (62%) solutions, VE and BB contributions were under- and overestimated by 68% and 47%, respectively by the P-only solution, as compared to the G + P solution. The results provide an insight on the impact of G/P partitioning on the source apportionment of PAHs and their toxicity.

  15. Thia-arenes as source apportionment tracers for urban air particulate

    SciTech Connect

    McCarry, B.E.; Allan, L.M.; Mehta, S.; Marvin, C.H.

    1995-12-31

    Over sixty respirable air particulate samples were selected from a large number of filters collected in Hamilton, Ontario, Canada. Depending on the wind direction these sites were either predominantly upwind or predominantly downwind of the industrial sources. The sixty filters were extracted and analyzed using GC-MS for a range of PAH and sulfur-containing PAH (thia-arenes). Various reference standards (coal tar, diesel exhaust, urban air particulate) and source samples (coke oven condensate) were analyzed as well. A set of air particulate samples collected in another city alongside a highway provided an urban vehicular air sample. Unique thia-arene profiles were noted in the reference and source samples which provided the basis for this source apportionment work; two main approaches were used: (1) analysis of alkylated derivatives of thia-arenes with a molecular mass of 184 amu and (2) analysis of 234 amu isomers. The diesel exhaust and urban vehicular samples gave identical profiles while the coal tar and coke oven samples also had identical profiles but in different respects. The air samples collected at samplers located upwind of the coke ovens showed thia-arene profiles which were similar to the profile observed with a diesel exhaust reference material. However, air samples collected downwind of the coke ovens were heavily loaded samples and resembled the coal tar coke and oven condensate samples.

  16. Source apportionment of PM2.5 for supporting control strategies in the Monterrey Metropolitan Area, Mexico.

    PubMed

    Martínez-Cinco, Marco; Santos-Guzmán, Jesús; Mejía-Velázquez, Gerardo

    2016-06-01

    The Monterrey Metropolitan Area (MMA) in Northeast Mexico has shown high PM2.5 concentrations since 2003. The data shows that the annual average concentration exceeds from 2 to 3 times the Mexican PM2.5 annual air quality standard of 12 µg/m(3). In a previous work we studied the chemical characterization of PM2.5 in two sites of the MMA during the winter season. Among the most important components we found ammonium sulfate and nitrate, elemental and organic carbon, and crustal matter. In this work we present the results of a second chemical characterization study performed during the summer time and the application of the chemical mass balance (CMB) model to determine the source apportionment of air pollutants in the region. The chemical analysis results show that the chemical composition of PM2.5 is similar in both sites and periods of the year. The results of the chemical analysis and the CMB model show that industrial, traffic, and combustion activities in the area are the major sources of primary PM2.5 and precursor gases of secondary inorganic and organic aerosol (SO2, NOx, NH3, and volatile organic compounds [VOCs]). We also found that black carbon and organic carbon are important components of PM2.5 in the MMA. These results are consistent with the MMA emission inventory that reports as major sources of particles and SO2 a refinery and fuel combustion, as well as nitrogen oxides and ammonium from transportation and industrial activities in the MMA and ammonium form agricultural activities in the state. The results of this work are important to identify and support effective actions to reduce direct emissions of PM2.5 and its precursor gases to improve air quality in the MMA. The Monterrey Metropolitan Area (MMA) has been classified as the most air-polluted area in Mexico by the World Health Organization (WHO). Effective actions need to be taken to control primary sources of PM2.5 and its precursors, reducing health risks on the population exposed and their

  17. Source apportionment of size-fractionated particles during the 2013 Asian Youth Games and the 2014 Youth Olympic Games in Nanjing, China.

    PubMed

    Chen, Pulong; Wang, Tijian; Lu, Xiaobo; Yu, Yiyong; Kasoar, Matthew; Xie, Min; Zhuang, Bingliang

    2017-02-01

    In this study, samples of size-fractionated particulate matter were collected continuously using a 9-size interval cascade impactor at an urban site in Nanjing, before, during and after the Asian Youth Games (AYG), from July to September of 2013, and the Youth Olympic Games (YOG), from July to September of 2014. First, elemental concentrations, water-soluble ions including Cl(-), NO3(-), SO4(2-), NH4(+), K(+), Na(+) and Ca(2+), organic carbon (OC) and elemental carbon (EC) were analysed. Then, the source apportionment of the fine and coarse particulate matter was carried out using the chemical mass balance (CMB) model. The average PM10 concentrations were 90.4±20.0μg/m(3) during the 2013 AYG and 70.6±25.3μg/m(3) during the 2014 YOG. For PM2.1, the average concentrations were 50.0±12.8μg/m(3) in 2013 and 34.6±17.0μg/m(3) in 2014. Investigations showed that the average concentrations of particles declined significantly from 2013 to 2014, and concentrations were at the lowest levels during the events. Results indicated that OC, EC, sulfate and crustal elements have significant monthly and size-based variations. The major components, including crustal elements, water-soluble ions and carbonaceous aerosol accounted for 75.3-91.9% of the total particulate mass concentrations during the sampling periods. Fugitive dust, coal combustion dust, iron dust, construction dust, soil dust, vehicle exhaust, secondary aerosols and sea salt have been classified as the main emissions in Nanjing. The source apportionment results indicate that the emissions from fugitive dust, which was the most abundance emission source during the 2013 AYG, contributed to 23.0% of the total particle mass. However, fugitive dust decreased to 6.2% of the total particle mass during the 2014 YOG. Construction dust (14.7% versus 7.8% for the AYG and the YOG, respectively) and secondary sulfate aerosol (9.3% versus 8.0% for the AYG and the YOG, respectively) showed the same trend as fugitive dust

  18. Use of synthetic data to evaluate positive matrix factorization as a source apportionment tool for PM2.5 exposure data.

    PubMed

    Brinkman, Gregory; Vance, Gary; Hannigan, Michael P; Milford, Jana B

    2006-03-15

    Positive matrix factorization (PMF) was applied to synthetic datasets that simulate personal exposures to airborne PM2.5 from 12 sources. Three differentfilter analysis scenarios using different analytical chemistry techniques were considered. The full suite scenario quantified elemental carbon, organic carbon, inorganic ions, trace elements, and trace organic species including carboxylic acids and organic compounds with -OH functionality. A second scenario excluded trace elements and a third assumed that derivatization steps to quantify polar organic compounds were not performed. Similar errors in source apportionment were seen with all three scenarios. In most cases, PMF failed to separate out factors corresponding to road dust and vegetative debris, two sources that made relatively uniform contributions to the synthetic exposures. Factors representing wood smoke, natural gas combustion, and meat cooking sources were difficult to identify due to a lack of unique tracers with concentrations reliably above the detection limits assumed in the study. Factors representing cigarette smoke, candle smoke, gasoline exhaust, and secondary aerosols were comparatively easy to identify. When contributions from a pair of sources, such as diesel and gasoline exhaust, were highly correlated in the synthetic datasets, a single factor corresponding to both sources was usually found.

  19. Connecting Organic Aerosol Climate-Relevant Properties to Chemical Mechanisms of Sources and Processing

    SciTech Connect

    Thornton, Joel

    2015-01-26

    The research conducted on this project aimed to improve our understanding of secondary organic aerosol (SOA) formation in the atmosphere, and how the properties of the SOA impact climate through its size, phase state, and optical properties. The goal of this project was to demonstrate that the use of molecular composition information to mechanistically connect source apportionment and climate properties can improve the physical basis for simulation of SOA formation and properties in climate models. The research involved developing and improving methods to provide online measurements of the molecular composition of SOA under atmospherically relevant conditions and to apply this technology to controlled simulation chamber experiments and field measurements. The science we have completed with the methodology will impact the simulation of aerosol particles in climate models.

  20. Source apportionment of VOCs in the Los Angeles area using positive matrix factorization

    NASA Astrophysics Data System (ADS)

    Brown, Steven G.; Frankel, Anna; Hafner, Hilary R.

    Eight 3-h speciated hydrocarbon measurements were collected daily by the South Coast Air Quality Management District (SCAQMD) as part of the Photochemical Assessment Monitoring Stations (PAMS) program during the summers of 2001-03 at two sites in the Los Angeles air basin, Azusa and Hawthorne. Over 30 hydrocarbons from over 500 samples at Azusa and 600 samples at Hawthorne were subsequently analyzed using the multivariate receptor model positive matrix factorization (PMF). At Azusa and Hawthorne, five and six factors were identified, respectively, with a good comparison between predicted and measured mass. At Azusa, evaporative emissions (a median of 31% of the total mass), motor vehicle exhaust (22%), liquid/unburned gasoline (27%), coatings (17%), and biogenic emissions (3%) factors were identified. Factors identified at Hawthorne were evaporative emissions (a median of 34% of the total mass), motor vehicle exhaust (24%), industrial process losses (15%), natural gas (13%), liquid/unburned gasoline (13%), and biogenic emissions (1%). Together, the median contribution from mobile source-related factors (exhaust, evaporative emissions, and liquid/unburned gasoline) was 80% and 71% at Azusa and Hawthorne, respectively, similar to previous source apportionment results using the chemical mass balance (CMB) model. There is a difference in the distribution among mobile source factors compared to the CMB work, with an increase in the contribution from evaporative emissions, though the cause (changes in emissions or differences between models) is unknown.

  1. Source Apportionment of Atmospheric Polychlorinated Biphenyls in New Jersey 1997-2011.

    PubMed

    Praipipat, Pornsawai; Meng, Qingyu; Miskewitz, Robert J; Rodenburg, Lisa A

    2017-02-07

    Concentrations of polychlorinated biphenyls (PCBs) in the Delaware River currently exceed the Water Quality Criteria of 16 pg/L for the sum of PCBs due in part to atmospheric deposition. The purpose of this work was to use a source apportionment tool called Positive Matrix Factorization (PMF) to identify the sources of PCBs to the atmosphere in this area and determine whether their concentrations are declining over time. The data set was compiled by the Delaware Atmospheric Deposition Network (DADN) from samples taken in Camden, NJ from 1999 to 2011 and New Brunswick, NJ from 1997 to 2011. The PMF analysis revealed four resolved factors at each site. The factors that dominate the PCB burden in the atmosphere at both Camden and New Brunswick resemble Aroclor 1242. These factors declined in concentration during some portions of the monitoring period, but this decline slowed or stopped during 2003-2011. None of the factors displayed consistent declines in concentration throughout the monitoring periods, and some factors actually increased in concentration during some periods. This suggests natural attenuation alone will not control atmospheric PCB concentrations, and additional efforts are needed to control PCB atmospheric emissions as well as the numerous other sources of PCBs to the estuary.

  2. Source apportionment of particulate organic matter using infrared spectra at multiple IMPROVE sites

    NASA Astrophysics Data System (ADS)

    Kuzmiakova, A.; Dillner, A. M.; Takahama, S.

    2016-12-01

    As organic aerosol is a dominant contributor to air pollution and radiative forcing in many regions in the United States, characterizing its composition and apportioning the organic mass to its major sources provides insight into atmospheric processes and guidance for decreasing its abundance. National networks, such as Interagency Monitoring of Protected Visual Environment (IMPROVE), provide multi-site and multi-year particulate matter samples useful for evaluating sources over all four seasons. To this end, our study focuses on apportioning the particulate organic matter (OM) to specific anthropogenic and biological processes from year-long infrared aerosol measurements collected at six IMPROVE sites (five national park sites and one urban site) during 2011. Pooling these organic aerosol samples into one dataset, we apply factor and cluster analyses to extract four chemical factors (two dominated by processed emissions, one dominated by hydroxyl groups, and one by hydrocarbons) and ascribe each factor to a specific source depending on the site and season. We also present a method to characterize measurement uncertainty in infrared instrumental analysis and investigate sensitivity analysis in generated factors. In Phoenix (the urban site) we find the majority (80-95%) of the OM consisted of anthropogenic activities, such as traffic emissions, fossil fuel combustion (both all year long), and residential wood burning (fall to winter). Mineral dust emissions accounted for the rest of OM (5-20%). At the National Park sites the OM concentration was lower on average and consisted of marine and dust aerosols, summertime biomass burning and biogenic aerosols, processed fossil fuel combustion, and emissions from ships and oil refineries. Our study highlights the potential for further site-specific or multi-year aerosol characterization in the context of a long-term atmospheric sampling program to quantify sources of organic particles impacting air quality, aid in policy

  3. Measurement of greenhouse gases (GHGs) and source apportionment in Bakersfield, CA during CALNEX 2010

    NASA Astrophysics Data System (ADS)

    Guha, A.; Gentner, D. R.; Goldstein, A.; Provencal, R. A.; Gardner, A.; Calnex Bakersfield Science Team

    2010-12-01

    The California Global Warming Solutions Act 2006 creates a need to validate and improve the GHG inventory of the State, which has been largely based on activity and emission factor based estimates. As part of CALNEX 2010, we conducted measurements at the Bakersfield supersite of CO2, CH4, and N2O using fast response laser analyzers (LGR Inc.) to document the ambient mixing ratios of GHGs and analyze their major sources in the region, with an emphasis on understanding emissions of methane (CH4) and nitrous oxide (N2O). The site was located downwind of the urban center during the day and usually experienced a reversal of wind direction at night. Bakersfield is an urban area with heavy industrialization including petroleum refineries, oilfields, manufacturing, and cogeneration plants, all of which can be sources of the abovementioned GHGs. The site was close to a highway and potentially subject to vehicular CH4 and N2O emissions. Hence, CO and a broad variety of VOCs, which can serve as tracers (particularly for vehicle emissions), were included in the measurements to help with source apportionment. In addition to typical urban and industrial sources, Kern County is a rich agricultural region and includes a large number of cattle feedlots, dairies, settling ponds and landfills which are assumed to be some of the largest anthropogenic sources of methane in the State. Additionally, the agricultural industry uses significant amounts of fertilizers, which can lead to production of N2O from the soils along with emissions from controlled biomass burning of agricultural waste. The three GHGs studied show a strong diurnal pattern with concentrations building up in the night-time as the planetary boundary layer (PBL) becomes smaller and reversal in wind direction causes the site to become downwind of some GHG sources like landfills and feedlots. The mean background concentrations at the site (CNO2= 323 ppb; CCO2 = 390 ppm) during the day were consistent with those from the

  4. Determination of buffering capacity of total suspended particle and its source apportionment using the chemical mass balance approach.

    PubMed

    Bi, Xiao-Hui; Feng, Yin-Chang; Zhu, Tan; Zhang, Yu-Fen; Wu, Jian-Hui; Li, Xiang

    2011-01-01

    The samples of total suspended particle (TSP) from sources and TSP in the ambient atmosphere were collected in 2006 at Tianjin, People's Republic of China and analyzed for 16 chemical elements, two water-soluble ions, total carbon, and organic carbon. On the basis of the chemical mass balance (CMB) model, the contributions of different TSP sources to the ambient TSP were identified. The results showed that resuspended dust has the biggest contributions to the concentration of ambient TSP. The buffering capacity of each TSP source was also determined by an analytical chemistry method, and the result showed that the constructive dust (the dust emitted from construction work) had the strongest buffering capacity among the measured sources, whereas the coal combustion dust had the weakest buffering capacity. A calculation formula of the source of buffering capacity of ambient TSP was developed based on the result of TSP source apportionment and the identification of the buffering capacity of each TSP source in this study. The results of the source apportionment of the buffering capacity of ambient TSP indicated that open sources (including soil dust, resuspended dust, and constructive dust) were the dominant sources of the buffering capacity of the ambient TSP. Acid rain pollution in cities in Northern China might become serious with a decrease of open source pollution without reducing acidic sources. More efforts must be made to evaluate this potential risk, and countermeasures should be proposed as early as possible.

  5. Source apportionment of fluorine pollution in regional shallow groundwater at You'xi County southeast China.

    PubMed

    Lü, Jian; Qiu, Haiyuan; Lin, Huangbin; Yuan, Yuan; Chen, Zhi; Zhao, Rurong

    2016-09-01

    Source apportionment of fluorine pollution in the regional shallow groundwater at You'xi County, southeast China, has been analyzed by means of monitoring F(-) ion change characteristics in this area. Meanwhile, pollution sources and influencing factors of the shallow groundwater have been uncovered by studying the correlation between F(-) and other related ions such as Na(+), Ca(2+), Cl(-), NO3(-), HCO3(-), as well as (K(+) + Na(+))/Ca(2+) ratio (R) and pH effect. The results show that F(-) ions in shallow groundwater at the study area come mainly from the dissolution of fluorinated minerals in a form of fluorite (CaF2), the so-called water-rock interaction, and there is a higher possibility for the occurrence of fluorine water where the ratio of (K(+) + Na(+))/Ca(2+) exceeds a value of 2.1. Moreover, the release and migration of F(-) ions have been favored by the alkaline environment in this study area. Copyright © 2016 Elsevier Ltd. All rights reserved.

  6. Application of hierarchical Bayesian unmixing models in river sediment source apportionment

    NASA Astrophysics Data System (ADS)

    Blake, Will; Smith, Hugh; Navas, Ana; Bodé, Samuel; Goddard, Rupert; Zou Kuzyk, Zou; Lennard, Amy; Lobb, David; Owens, Phil; Palazon, Leticia; Petticrew, Ellen; Gaspar, Leticia; Stock, Brian; Boeckx, Pacsal; Semmens, Brice

    2016-04-01

    Fingerprinting and unmixing concepts are used widely across environmental disciplines for forensic evaluation of pollutant sources. In aquatic and marine systems, this includes tracking the source of organic and inorganic pollutants in water and linking problem sediment to soil erosion and land use sources. It is, however, the particular complexity of ecological systems that has driven creation of the most sophisticated mixing models, primarily to (i) evaluate diet composition in complex ecological food webs, (ii) inform population structure and (iii) explore animal movement. In the context of the new hierarchical Bayesian unmixing model, MIXSIAR, developed to characterise intra-population niche variation in ecological systems, we evaluate the linkage between ecological 'prey' and 'consumer' concepts and river basin sediment 'source' and sediment 'mixtures' to exemplify the value of ecological modelling tools to river basin science. Recent studies have outlined advantages presented by Bayesian unmixing approaches in handling complex source and mixture datasets while dealing appropriately with uncertainty in parameter probability distributions. MixSIAR is unique in that it allows individual fixed and random effects associated with mixture hierarchy, i.e. factors that might exert an influence on model outcome for mixture groups, to be explored within the source-receptor framework. This offers new and powerful ways of interpreting river basin apportionment data. In this contribution, key components of the model are evaluated in the context of common experimental designs for sediment fingerprinting studies namely simple, nested and distributed catchment sampling programmes. Illustrative examples using geochemical and compound specific stable isotope datasets are presented and used to discuss best practice with specific attention to (1) the tracer selection process, (2) incorporation of fixed effects relating to sample timeframe and sediment type in the modelling

  7. Source apportionment of surface ozone in the Yangtze River Delta, China in the summer of 2013

    NASA Astrophysics Data System (ADS)

    Li, L.; An, J. Y.; Shi, Y. Y.; Zhou, M.; Yan, R. S.; Huang, C.; Wang, H. L.; Lou, S. R.; Wang, Q.; Lu, Q.; Wu, J.

    2016-11-01

    We applied ozone source apportionment technology (OSAT) with tagged tracers coupled within the Comprehensive Air Quality Model with Extensions (CAMx) to study the region and source category contribution to surface ozone in the Yangtze River Delta area in summer of 2013. Results indicate that the daytime ozone concentrations in the YRD region are influenced by emissions both locally, regionally and super-regionally. At urban Shanghai, Hangzhou and Suzhou receptors, the ozone formation is mainly VOC-limited, precursor emissions form Zhejiang province dominate their O3 concentrations. At the junction area among two provinces and Shanghai city, the ozone is usually influenced by all the three areas. The daily max O3 at the Dianshan Lake in July are contributed by Zhejiang (48.5%), Jiangsu (11.7%), Anhui (11.6%) and Shanghai (7.4%), long-range transport constitutes around 20.9%. At Chongming site, the BVOC emissions rate is higher than urban region. Regional contribution results show that Shanghai constitutes 15.6%, Jiangsu contributes 16.2% and Zhejiang accounts for 25.5% of the daily max O3. The analysis of the source category contribution to high ozone in the Yangtze River Delta region indicates that the most significant anthropogenic emission source sectors contributing to O3 pollution include industry, vehicle exhaust, although the effects vary with source sector and selected pollution episodes. Emissions of NOx and VOCs emitted from the fuel combustion of industrial boilers and kilns, together with VOCs emissions from industrial process contribute a lot to the high concentrations in urban Hangzhou, Suzhou and Shanghai. The contribution from regional elevated power plants cannot be neglected, especially to Dianshan Lake. Fugitive emissions of volatile pollution sources also have certain contribution to regional O3. These results indicate that the regional collaboration is of most importance to reduce ambient ozone pollution, particularly during high ozone episodes.

  8. Apportionment of primary and secondary organic aerosols in southern California during the 2005 study of organic aerosols in riverside (SOAR-1).

    PubMed

    Docherty, Kenneth S; Stone, Elizabeth A; Ulbrich, Ingrid M; DeCarlo, Peter F; Snyder, David C; Schauer, James J; Peltier, Richard E; Weber, Rodney J; Murphy, Shane M; Seinfeld, John H; Grover, Brett D; Eatough, Delbert J; Jimenez, Jose L

    2008-10-15

    Ambient sampling was conducted in Riverside, California during the 2005 Study of Organic Aerosols in Riverside to characterize the composition and sources of organic aerosol using a variety of state-of-the-art instrumentation and source apportionmenttechniques. The secondary organic aerosol (SOA) mass is estimated by elemental carbon and carbon monoxide tracer methods, water soluble organic carbon content, chemical mass balance of organic molecular markers, and positive matrix factorization of high-resolution aerosol mass spectrometer data. Estimates obtained from each ofthese methods indicate that the organic fraction in ambient aerosol is overwhelmingly secondary in nature during a period of several weeks with moderate ozone concentrations and that SOA is the single largest component of PM1 aerosol in Riverside. Average SOA/OA contributions of 70-90% were observed during midday periods, whereas minimum SOA contributions of approximately 45% were observed during peak morning traffic periods. These results are contraryto previous estimates of SOAthroughout the Los Angeles Basin which reported that, other than during severe photochemical smog episodes, SOA was lower than primary OA. Possible reasons for these differences are discussed.

  9. Source apportionment of atmospheric polycyclic aromatic hydrocarbons (PAHs) in Palm Beach County, Florida.

    PubMed

    Afshar-Mohajer, Nima; Wilson, Christina; Wu, Chang-Yu; Stormer, James E

    2016-04-01

    Due to concerns about adverse health effects associated with inhalation of atmospheric polycyclic aromatic hydrocarbons (PAHs), 30 ambient air samples were obtained at an air quality monitoring station in Palm Beach County, Florida, from March 2013 to March 2014. The ambient PAH concentration measurements and fractional emission rates of known sources were incorporated into a chemical mass balance model, CMB8.2, developed by EPA, to apportion contributions of three major PAH sources including preharvest sugarcane burning, mobile vehicles, and wildland fires. Strong association between the number of benzene rings and source contribution was found, and mobile vehicles were identified to be the prevailing source (contribution≥56%) for the observed PAHs concentration with lower molecular weights (four or fewer benzene rings) throughout the year. Preharvest sugarcane burning was the primary contributing source for PAHs with relatively higher molecular weights (five or more benzene rings) during the sugarcane burning season (from October to May of the next year). Source contribution of wildland fires varied among PAH compounds but was consistently lower than for sugarcane burning during the sugarcane harvest season. Determining the major sources responsible for ground-level PAHs serves as a tool to improving management strategies for PAH emitting sources and a step toward better protection of the health of residents in terms of exposure to PAHs. The results obtain insight into temporal dominance of PAH polluting sources for those residential areas located near sugarcane burning facilities and have implications beyond Palm Beach County, in areas with high concerns of PAHs and their linked sources. Source apportionment of atmospheric polycyclic hydrocarbons (PAHs) in Palm Beach County, Florida, meant to estimate contributions of major sources in PAH concentrations measured at Belle Glade City of Palm Beach County. Number of benzene rings was found to be the key parameter

  10. Source apportionment of single particles sampled at the industrially polluted town of Port Talbot, United Kingdom by ATOFMS

    NASA Astrophysics Data System (ADS)

    Taiwo, Adewale M.; Harrison, Roy M.; Beddows, David C. S.; Shi, Zongbo

    2014-11-01

    Single particle analysis of an industrially polluted atmosphere in Port Talbot, South Wales, United Kingdom was conducted using Aerosol-Time-of-Flight Mass Spectrometry (ATOFMS). During the four week sampling campaign, a total of 5,162,018 particles were sized in the size range 0.2-1.9 μm aerodynamic diameter. Of these, 580,798 were successfully ionized generating mass spectra. K-means clustering employed for analysing ATOFMS data utilized 96% of the hit particles to generate 20 clusters. Similar clusters were merged together and 17 clusters were generated from which 7 main particle groups were identified. The particle classes include: K-rich particles (K-CN, K-NO3, K-EC, K-Cl-PO3 and K-HSO4), aged sea salt (Na-NO3), silicate dust (Na-HSiO2), sulphate rich particles (K-HSO4), nitrate rich particles (AlO-NO3), Ca particles (Ca-NO3), carbon-rich particles (Mn-OC, Metallic-EC, EC, EC-NO3 and OC-EC), and aromatic hydrocarbon particles (Arom-CN, Fe-PAH-NO3 and PAH-CN). With the aid of wind sector plots, the K-Cl-PO3 and Na-HSiO2 particle clusters were related to the steelworks blast furnace/sinter plant while Ca-rich particles arose from blast furnace emissions. K-CN, K-EC, Na-HSiO2, K-HSO4, Mn-OC, Arom-CN, Fe-PAH-NO3, and PAH-CN particles were closely linked with emissions from the cokemaking and mills (hot and cold) steelworks sections. The source factors identified by the ATOFMS were compared with those derived from multivariate analysis using Multilinear Engine (ME-2) applied to filter samples analysed off-line. Both methods of source apportionment identified common source factors including those within the steelworks (blast furnace, sinter, cokemaking), as well as marine, traffic and secondary particles, but quantitative attribution of mass is very different.

  11. Application of a tagged-species method to source apportionment of primary PM 2.5 components in a regional air quality model

    NASA Astrophysics Data System (ADS)

    Samaali, Mehrez; Bouchet, Véronique S.; Moran, Michael D.; Sassi, Mourad

    2011-07-01

    %) in all five cities. At this smaller scale, it was found that the tagged sources' relative contributions to emissions may not scale proportionally with the tagged sources' relative contributions to concentrations due to transport from neighboring areas. With this new source-apportionment capability, AURAMS can be used to accurately and efficiently track the contribution of selected emissions sources of carbonaceous aerosols for longer simulations at regional or continental scales. This capability will also provide the foundation for the development of tagging for secondary PM species to allow the apportionment of PM component concentrations across all sources.

  12. Aerosol deposited in East Antarctica over the last glacial cycle: Detailed apportionment of continental and sea-salt contributions

    NASA Astrophysics Data System (ADS)

    Bigler, Matthias; RöThlisberger, Regine; Lambert, Fabrice; Stocker, Thomas F.; Wagenbach, Dietmar

    2006-04-01

    The major ions, sodium (Na+), calcium (Ca2+), and chloride (Cl-), deposited in central Antarctica and preserved in ice cores originate from both marine and continental sources. They provide important proxy records, helping to reconstruct past climatic processes. However, it is difficult to clearly separate the individual contributions from the two sources, particularly the continental one during glacial periods. On the basis of Na+ and Ca2+ records at an unprecedented resolution from the European Project for Ice Coring in Antarctica (EPICA) Dome C ice core back to the penultimate glacial period, mean ion mass ratios were deduced for the continental and the sea-salt aerosol body over East Antarctica. The sea-salt ion mass ratios are in the range predicted for both wind-induced bubble bursting of breaking waves on the open ocean and sea ice brine-derived aerosols, respectively, thus allowing no clear decision on the contribution of sea ice to the central Antarctic sea-salt aerosol. The continental ion mass ratios point to a substantial contribution by halide aerosols, which is in agreement with the source properties in southern South America, although these ratios do not rule out the continental shelf exposed during glacial stages as an additional source. While during cold glacial periods continental sources accounted for more than 90% of the total Ca2+ input, this contribution was highly variable during the remaining glacial periods covarying with the Antarctic warm events. During the Holocene it was less than 50%, but it was significantly higher during the last interglacial period. The sea-salt aerosol contribution to the total Na+ input, which was mostly dominant and higher than 90%, was reduced to only two thirds during the last two glacial maxima and the period around 60 ka. Thus the glacial continental Na+ contribution appears to be more important than previously assumed, implying that Na+ records not corrected for continental Na+ do not represent a pure marine

  13. Chemical composition, sources and secondary processes of aerosols in Baoji city of northwest China

    NASA Astrophysics Data System (ADS)

    Wang, Y. C.; Huang, R.-J.; Ni, H. Y.; Chen, Y.; Wang, Q. Y.; Li, G. H.; Tie, X. X.; Shen, Z. X.; Huang, Y.; Liu, S. X.; Dong, W. M.; Xue, P.; Fröhlich, R.; Canonaco, F.; Elser, M.; Daellenbach, K. R.; Bozzetti, C.; El Haddad, I.; Prévôt, A. S. H.; Canagaratna, M. R.; Worsnop, D. R.; Cao, J. J.

    2017-06-01

    Particulate air pollution is a severe environmental problem in China, affecting visibility, air quality, climate and human health. However, previous studies focus mainly on large cities such as Beijing, Shanghai, and Guangzhou. In this study, an Aerodyne Aerosol Chemical Speciation Monitor was deployed in Baoji, a middle size inland city in northwest China from 26 February to 27 March 2014. The non-refractory submicron aerosol (NR-PM1) was dominated by organics (55%), followed by sulfate (16%), nitrate (15%), ammonium (11%) and chloride (3%). A source apportionment of the organic aerosol (OA) was performed with the Sofi (Source Finder) interface of ME-2 (Multilinear Engine), and six main sources/factors were identified and classified as hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), coal combustion OA (CCOA), less oxidized oxygenated OA (LO-OOA) and more oxidized oxygenated OA (MO-OOA), which contributed 20%, 14%, 13%, 9%, 23% and 21% of total OA, respectively. The contribution of secondary components shows increasing trends from clean days to polluted days, indicating the importance of secondary aerosol formation processes in driving particulate air pollution. The formation of LO-OOA and MO-OOA is mainly driven by photochemical reactions, but significantly influenced by aqueous-phase chemistry during periods of low atmospheric oxidative capacity.

  14. Reactive oxygen species associated with water-soluble PM2.5 in the southeastern United States: spatiotemporal trends and source apportionment

    NASA Astrophysics Data System (ADS)

    Verma, V.; Fang, T.; Guo, H.; King, L.; Bates, J. T.; Peltier, R. E.; Edgerton, E.; Russell, A. G.; Weber, R. J.

    2014-12-01

    We assess the potential of the water-soluble fraction of atmospheric fine aerosols in the southeastern United States to generate reactive oxygen species (ROS) and identify major ROS-associated emission sources. ROS-generation potential of particles was quantified by the dithiothreitol (DTT) assay and involved analysis of fine particulate matter (PM) extracted from high-volume quartz filters (23 h integrated samples) collected at various sites in different environmental settings in the southeast, including three urban-Atlanta sites, in addition to a rural site. Paired sampling was conducted with one fixed site in Atlanta (Jefferson Street), representative of the urban environment, with the others rotating among different sites, for ~250 days between June 2012 and September 2013 (N=483). A simple linear regression between the DTT activity and aerosol chemical components revealed strong associations between PM ROS-generation potential and secondary organic aerosol (WSOC - water-soluble organic carbon) in summer, and biomass burning markers in winter. Redox-active metals were also somewhat correlated with the DTT activity, but mostly at urban and roadside sites. Positive matrix factorization (PMF) was applied to apportion the relative contribution of various sources to the ROS-generation potential of water-soluble PM2.5 in urban Atlanta. PMF showed that vehicular emissions contribute uniformly throughout the year (12-25%), while secondary oxidation processes dominated the DTT activity in summer (46%) and biomass burning in winter (47%). Road dust was significant only during drier periods (~12% in summer and fall). Source apportionment by chemical mass balance (CMB) was reasonably consistent with PMF, but with higher contribution from vehicular emissions (32%). Given the spatially large data set of PM sampled over an extended period, the study reconciles the results from previous work that showed only region- or season-specific aerosol components or sources contributing

  15. Reactive oxygen species associated with water-soluble PM2.5 in the southeastern United States: spatiotemporal trends and source apportionment

    NASA Astrophysics Data System (ADS)

    Verma, V.; Fang, T.; Guo, H.; King, L.; Bates, J. T.; Peltier, R. E.; Edgerton, E.; Russell, A. J.; Weber, R. J.

    2014-07-01

    We assess the potential of the water-soluble fraction of atmospheric fine aerosols in the southeastern US to generate reactive oxygen species (ROS) and identify major ROS-associated emission sources. ROS-generation potential of particles was quantified by the dithiothreitol (DTT) assay and involved analysis of fine particulate matter (PM) extracted from high-volume quartz filters (23 h integrated samples) collected at various sites in different environmental settings in the southeast, including three urban Atlanta sites, in addition to a rural site. Paired sampling was conducted with one fixed site in Atlanta (Jefferson Street), representative of the urban environment, with the others rotating among different sites, for ~250 days between June 2012 and September 2013 (N = 483). A simple linear regression between the DTT activity and aerosol chemical components revealed strong associations between PM ROS generation potential and secondary organic aerosol (WSOC) in summer, and biomass burning markers in winter. Redox-active metals were also correlated with the DTT activity, but mostly at urban and roadside sites. Positive matrix factorization (PMF) was applied to apportion the relative contribution of various sources to the ROS generation potential of water-soluble PM2.5 in urban Atlanta. PMF showed that vehicular emissions contribute uniformly throughout the year (12 to 25%), while secondary oxidation processes dominated the DTT activity in summer (46%) and biomass burning in winter (47%). Mineral dust was significant only during drier periods (~12% in summer and fall). Source apportionment by chemical mass balance (CMB) was reasonably consistent with PMF, but with higher contribution from vehicular emissions (32%). Given the spatially large data set of PM sampled over an extended period, the study reconciles the results from previous work that showed only region- or season-specific aerosol components or sources contributing to PM ROS activity, possibly due to

  16. Source apportionment of arsenic in atmospheric dust fall out in an urban residential area, Raipur, Central India

    NASA Astrophysics Data System (ADS)

    Balakrishna, G.; Pervez, S.; Bisht, D. S.

    2011-06-01

    The components and quantities of atmospheric dust fallout have been reported to be the pollution indicator of large urban areas. The multiplicity and complexity of sources of atmospheric dusts in urban regions has put forward the need of source apportionment of these sources indicating their contribution to specific environmental receptor. The study presented here is focused on investigation of source contribution estimates of Arsenic in urban dust fallout in an urban-industrial area, Raipur, India. Source-receptor based representative sampling plan using longitudinal study design has been adopted. Six sampling sites have been identified on the basis of land use for development plan of anthropogenic activities and factors related to the transportation and dispersion pattern of atmospheric dusts. Source apportionment has been done using Chemical Mass Balance (CMB 8). Good fit parameters and relative source contribution has been analyzed and documented. Dominance of coal fired industries sources on arsenic levels measured at selected ambient residential receptors compared to line sources has been observed. Road-traffic has shown highest contribution of dust at indoor houses and out door-street automobile exhaust has shows highest contribution for arsenic. The results of CMB output and regression data of source-receptor dust matrices have shown comparable pattern.

  17. Chemical characteristics and source apportionment of fine particulate organic carbon in Hong Kong during high particulate matter episodes in winter 2003

    NASA Astrophysics Data System (ADS)

    Li, Yun-Chun; Yu, Jian Zhen; Ho, Steven Sai Hang; Schauer, James J.; Yuan, Zibing; Lau, Alexis K. H.; Louie, Peter K. K.

    2013-02-01

    PM2.5 samples were collected at six general stations and one roadside station in Hong Kong in two periods of high particulate matter (PM) in 2003 (27 October-4 November and 30 November-13 December). The highest PM2.5 reached 216 μg m- 3 during the first high PM period and 113 μg m- 3 during the second high PM period. Analysis of synoptic weather conditions identified individual sampling days under dominant influence of one of three types of air masses, that is, local, regional and long-range transported (LRT) air masses. Roadside samples were discussed separately due to heavy influences from vehicular emissions. This research examines source apportionment of fine organic carbon (OC) and contribution of secondary organic aerosol on high PM days under different synoptic conditions. Six primary OC (POC) sources (vehicle exhaust, biomass burning, cooking, cigarette smoke, vegetative detritus, and coal combustion) were identified on the basis of characteristic organic tracers. Individual POC source contributions were estimated using chemical mass balance model. In the roadside and the local samples, OC was dominated by the primary sources, accounting for more than 74% of OC. In the samples influenced by regional and LRT air masses, secondary OC (SOC), which was approximated to be the difference between the total measured OC and the apportioned POC, contributed more than 54% of fine OC. SOC was highly correlated with water-soluble organic carbon and sulfate, consistent with its secondary nature.

  18. Source apportionment of atmospheric water over East Asia - a source tracer study in CAM5.1

    NASA Astrophysics Data System (ADS)

    Pan, Chen; Zhu, Bin; Gao, Jinhui; Kang, Hanqing

    2017-02-01

    The atmospheric water tracer (AWT) method is implemented in the Community Atmosphere Model version 5.1 (CAM5.1) to quantitatively identify the contributions of various source regions to precipitation and water vapour over East Asia. Compared to other source apportionment methods, the AWT method was developed based on detailed physical parameterisations, and can therefore trace the behaviour of atmospheric water substances directly and exactly. According to the simulation, the northern Indian Ocean (NIO) is the dominant oceanic moisture source region for precipitation over the Yangtze River valley (YRV) and southern China (SCN) in summer, while the north-western Pacific (NWP) dominates during other seasons. Evaporation over the South China Sea (SCS) is responsible for only 2.7-3.7 % of summer precipitation over the YRV and SCN. In addition, the Indo-China Peninsula is an important terrestrial moisture source region (annual contribution of ˜ 10 %). The overall relative contribution of each source region to the water vapour amount is similar to the corresponding contribution to precipitation over the YRV and SCN. A case study for the SCS shows that only a small part ( ≤ 5.5 %) of water vapour originates from local evaporation, whereas much more water vapour is supplied by the NWP and NIO. In addition, because evaporation from the SCS represents only a small contribution to the water vapour over the YRV and SCN in summer, the SCS mainly acts as a water vapour transport pathway where moisture from the NIO and NWP meet.

  19. Source regional contributions to PM2.5 in a megacity in China using an advanced source regional apportionment method.

    PubMed

    Tian, Ying-Ze; Chen, Gang; Wang, Hai-Ting; Huang-Fu, Yan-Qi; Shi, Guo-Liang; Han, Bo; Feng, Yin-Chang

    2016-03-01

    To quantify contributions of individual source categories from diverse regions to PM2.5, PM2.5 samples were collected in a megacity in China and analyzed through a newly developed source regional apportionment (SRA) method. Levels, compositions and seasonal variations of speciated PM2.5 dataset were investigated. Sources were determined by Multilinear Engine 2 (ME2) model, and results showed that the PM2.5 in Tianjin was mainly influenced by secondary sulphate & secondary organic carbon SOC (percent contribution of 26.2%), coal combustion (24.6%), crustal dust & cement dust (20.3%), secondary nitrate (14.9%) and traffic emissions (14.0%). The SRA method showed that northwest region R2 was the highest regional contributor to secondary sources, with percent contributions to PM2.5 being 9.7% for secondary sulphate & SOC and 6.0% for secondary nitrates; the highest coal combustion was from local region R1 (6.2%) and northwest R2 (8.0%); the maximum contributing region to crustal & cement dust was southeast region R4 (5.0%); and contributions of traffic emissions were relatively spatial homogeneous. The seasonal variation of regional source contributions was observed: in spring, the crustal and cement dust contributed a higher percentage and the R4 was an important contributor; the secondary process attributed an increase fraction in summer; the mixed coal combustion from southwest R5 enhanced in autumn.

  20. Measurement and apportionment of radon source terms for modeling indoor environments

    SciTech Connect

    Harley, N.H.

    1992-01-01

    During the present 2 1/2 year contract period, we have made significant Progress in modeling the source apportionment of indoor [sup 222]Rn and in [sup 222]Rn decay product dosimetry. Two additional areas were worked on which we believe are useful for the DOE Radon research Program. One involved an analysis of the research house data, grouping the hourly house [sup 222]Rn measurements into 2 day, 7 day and 90 day intervals to simulate the response of passive monitors. Another area requiring some attention resulted in a publication of 3 years of our indoor/outdoor measurements in a high-rise apartment. Little interest has been evinced in apartment measurements yet 20% of the US population lives in multiple-family dwellings, not in contact with the ground. These data together with a summary of all other published data on apartments showed that apartments have only about 50% greater [sup 222]Rn concentration than the measured outdoor [sup 222]Rn. Apartment dwellers generally represent a low risk group regarding [sup 222]Rn exposure. The following sections describe the main projects in some detail.

  1. Receptor model-based source apportionment of particulate pollution in Hyderabad, India.

    PubMed

    Guttikunda, Sarath K; Kopakka, Ramani V; Dasari, Prasad; Gertler, Alan W

    2013-07-01

    Air quality in Hyderabad, India, often exceeds the national ambient air quality standards, especially for particulate matter (PM), which, in 2010, averaged 82.2 ± 24.6, 96.2 ± 12.1, and 64.3 ± 21.2 μg/m(3) of PM10, at commercial, industrial, and residential monitoring stations, respectively, exceeding the national ambient standard of 60 μg/m(3). In 2005, following an ordinance passed by the Supreme Court of India, a source apportionment study was conducted to quantify source contributions to PM pollution in Hyderabad, using the chemical mass balance (version 8.2) receptor model for 180 ambient samples collected at three stations for PM10 and PM2.5 size fractions for three seasons. The receptor modeling results indicated that the PM10 pollution is dominated by the direct vehicular exhaust and road dust (more than 60%). PM2.5 with higher propensity to enter the human respiratory tracks, has mixed sources of vehicle exhaust, industrial coal combustion, garbage burning, and secondary PM. In order to improve the air quality in the city, these findings demonstrate the need to control emissions from all known sources and particularly focus on the low-hanging fruits like road dust and waste burning, while the technological and institutional advancements in the transport and industrial sectors are bound to enhance efficiencies. Andhra Pradesh Pollution Control Board utilized these results to prepare an air pollution control action plan for the city.

  2. Overview of receptor-based source apportionment studies for speciated atmospheric mercury

    NASA Astrophysics Data System (ADS)

    Cheng, I.; Xu, X.; Zhang, L.

    2015-07-01

    Receptor-based source apportionment studies of speciated atmospheric mercury are not only concerned with source contributions but also with the influence of transport, transformation, and deposition processes on speciated atmospheric mercury concentrations at receptor locations. Previous studies applied multivariate receptor models including principal components analysis and positive matrix factorization, and back trajectory receptor models including potential source contribution function, gridded frequency distributions, and concentration-back trajectory models. Combustion sources (e.g., coal combustion, biomass burning, and vehicular, industrial and waste incineration emissions), crustal/soil dust, and chemical and physical processes, such as gaseous elemental mercury (GEM) oxidation reactions, boundary layer mixing, and GEM flux from surfaces were inferred from the multivariate studies, which were predominantly conducted at receptor sites in Canada and the US. Back trajectory receptor models revealed potential impacts of large industrial areas such as the Ohio River valley in the US and throughout China, metal smelters, mercury evasion from the ocean and the Great Lakes, and free troposphere transport on receptor measurements. Input data and model parameters specific to atmospheric mercury receptor models are summarized and model strengths and weaknesses are also discussed. Multivariate models are suitable for receptor locations with intensive air monitoring because they require long-term collocated and simultaneous measurements of speciated atmospheric Hg and ancillary pollutants. The multivariate models provide more insight about the types of Hg emission sources and Hg processes that could affect speciated atmospheric Hg at a receptor location, whereas back trajectory receptor models are mainly ideal for identifying potential regional Hg source locations impacting elevated Hg concentrations. Interpretation of the multivariate model output to sources can be

  3. Source apportionment of NMVOCs in the Kathmandu Valley during the SusKat-ABC international field campaign using positive matrix factorization

    NASA Astrophysics Data System (ADS)

    Sarkar, Chinmoy; Sinha, Vinayak; Sinha, Baerbel; Panday, Arnico K.; Rupakheti, Maheswar; Lawrence, Mark G.

    2017-07-01

    A positive matrix factorization model (US EPA PMF version 5.0) was applied for the source apportionment of the dataset of 37 non-methane volatile organic compounds (NMVOCs) measured from 19 December 2012 to 30 January 2013 during the SusKat-ABC international air pollution measurement campaign using a proton-transfer-reaction time-of-flight mass spectrometer in the Kathmandu Valley. In all, eight source categories were identified with the PMF model using the new constrained model operation mode. Unresolved industrial emissions and traffic source factors were the major contributors to the total measured NMVOC mass loading (17.9 and 16.8 %, respectively) followed by mixed industrial emissions (14.0 %), while the remainder of the source was split approximately evenly between residential biofuel use and waste disposal (10.9 %), solvent evaporation (10.8 %), biomass co-fired brick kilns (10.4 %), biogenic emissions (10.0 %) and mixed daytime factor (9.2 %). Conditional probability function (CPF) analyses were performed to identify the physical locations associated with different sources. Source contributions to individual NMVOCs showed that biomass co-fired brick kilns significantly contribute to the elevated concentrations of several health relevant NMVOCs such as benzene. Despite the highly polluted conditions, biogenic emissions had the largest contribution (24.2 %) to the total daytime ozone production potential, even in winter, followed by solvent evaporation (20.2 %), traffic (15.0 %) and unresolved industrial emissions (14.3 %). Secondary organic aerosol (SOA) production had approximately equal contributions from biomass co-fired brick kilns (28.9 %) and traffic (28.2 %). Comparison of PMF results based on the in situ data versus REAS v2.1 and EDGAR v4.2 emission inventories showed that both the inventories underestimate the contribution of traffic and do not take the contribution of brick kilns into account. In addition, the REAS inventory overestimates the

  4. Seasonal variability and source apportionment of volatile organic compounds (VOCs) in the Paris megacity (France)

    NASA Astrophysics Data System (ADS)

    Baudic, Alexia; Gros, Valérie; Sauvage, Stéphane; Locoge, Nadine; Sanchez, Olivier; Sarda-Estève, Roland; Kalogridis, Cerise; Petit, Jean-Eudes; Bonnaire, Nicolas; Baisnée, Dominique; Favez, Olivier; Albinet, Alexandre; Sciare, Jean; Bonsang, Bernard

    2016-09-01

    Within the framework of air quality studies at the megacity scale, highly time-resolved volatile organic compound (C2-C8) measurements were performed in downtown Paris (urban background sites) from January to November 2010. This unique dataset included non-methane hydrocarbons (NMHCs) and aromatic/oxygenated species (OVOCs) measured by a GC-FID (gas chromatograph with a flame ionization detector) and a PTR-MS (proton transfer reaction - mass spectrometer), respectively. This study presents the seasonal variability of atmospheric VOCs being monitored in the French megacity and their various associated emission sources. Clear seasonal and diurnal patterns differed from one VOC to another as the result of their different origins and the influence of environmental parameters (solar radiation, temperature). Source apportionment (SA) was comprehensively conducted using a multivariate mathematical receptor modeling. The United States Environmental Protection Agency's positive matrix factorization tool (US EPA, PMF) was used to apportion and quantify ambient VOC concentrations into six different sources. The modeled source profiles were identified from near-field observations (measurements from three distinct emission sources: inside a highway tunnel, at a fireplace and from a domestic gas flue, hence with a specific focus on road traffic, wood-burning activities and natural gas emissions) and hydrocarbon profiles reported in the literature. The reconstructed VOC sources were cross validated using independent tracers such as inorganic gases (NO, NO2, CO), black carbon (BC) and meteorological data (temperature). The largest contributors to the predicted VOC concentrations were traffic-related activities (including motor vehicle exhaust, 15 % of the total mass on the annual average, and evaporative sources, 10 %), with the remaining emissions from natural gas and background (23 %), solvent use (20 %), wood-burning (18 %) and a biogenic source (15 %). An important finding of

  5. GIS-based source identification and apportionment of diffuse water pollution: perfluorinated compound pollution in the Tokyo Bay basin.

    PubMed

    Zushi, Yasuyuki; Masunaga, Shigeki

    2011-11-01

    To efficiently reduce perfluorinated compound (PFC) pollution, it is important to have an understanding of PFC sources and their contribution to the pollution. In this study, source identification of diffuse water pollution by PFCs was conducted using a GIS-based approach. Major components of the source identification were collection of the monitoring data and preparation of the corresponding geographic information that was extracted from a constructed GIS database. The spatially distributed pollution factors were then explored by multiple linear regression analysis, after which they were visually expressed using GIS. Among the 35 PFC homologues measured in a survey of the Tokyo Bay basin, 18 homologues were analyzed. Pollution by perfluorooctane sulfonate (PFOS) was explained well by the percentage of arterial traffic area in the basin, and the 84% variance of the measured PFOS concentration was explained by two geographic variables, arterial traffic area and population. Source apportionment between point and nonpoint sources was conducted based on the results of the analysis. The contribution of PFOS from nonpoint sources was comparable to that from point sources in several major rivers flowing into Tokyo Bay. Source identification and apportionment using the GIS-based approach was shown to be effective, especially for ubiquitous types of pollution, such as PFC pollution.

  6. Integrating Source Apportionment Tracers into a Bottom-up Inventory of Methane Emissions in the Barnett Shale Hydraulic Fracturing Region.

    PubMed

    Townsend-Small, Amy; Marrero, Josette E; Lyon, David R; Simpson, Isobel J; Meinardi, Simone; Blake, Donald R

    2015-07-07

    A growing dependence on natural gas for energy may exacerbate emissions of the greenhouse gas methane (CH4). Identifying fingerprints of these emissions is critical to our understanding of potential impacts. Here, we compare stable isotopic and alkane ratio tracers of natural gas, agricultural, and urban CH4 sources in the Barnett Shale hydraulic fracturing region near Fort Worth, Texas. Thermogenic and biogenic sources were compositionally distinct, and emissions from oil wells were enriched in alkanes and isotopically depleted relative to natural gas wells. Emissions from natural gas production varied in δ(13)C and alkane ratio composition, with δD-CH4 representing the most consistent tracer of natural gas sources. We integrated our data into a bottom-up inventory of CH4 for the region, resulting in an inventory of ethane (C2H6) sources for comparison to top-down estimates of CH4 and C2H6 emissions. Methane emissions in the Barnett are a complex mixture of urban, agricultural, and fossil fuel sources, which makes source apportionment challenging. For example, spatial heterogeneity in gas composition and high C2H6/CH4 ratios in emissions from conventional oil production add uncertainty to top-down models of source apportionment. Future top-down studies may benefit from the addition of δD-CH4 to distinguish thermogenic and biogenic sources.

  7. Evaluation of Particulate Matter Source Apportionment Forecasts during the MAPS-Seoul Field Campaign

    NASA Astrophysics Data System (ADS)

    Bae, C.; Kim, S.; Kim, H. C.; Kim, B. U.

    2015-12-01

    We report forecasting model performance analysis results of Comprehensive Air quality Model with extensions (CAMx) simulation evaluated with flight measurements during Megacity Air Pollution Studies-Seoul (MAPS-Seoul) field campaign. The primary focus of this study is two-fold: (1) the air quality forecasting model performance for O3, PM10/2.5 and their precursors over the Yellow Sea to measure the model's ability to account for the transport process and (2) the utilization of modeled source-receptor relationship to understand the root of systematic model under-prediction for PM10 and PM2.5 forecasts. MAPS-Seoul, conducted in the Seoul Metropolitan Area (SMA) in the summer of 2015, was an integrated research program covering ground monitoring and aloft measurement with aircrafts. To support this field campaign, air quality forecasting was performed with Weather Research and Forecasting (WRF) - Sparse Matrix Operator Kernel Emissions (SMOKE) - CAMx modeling framework. WRF model simulations initialized with National Centers for Environmental Prediction Global Forecasting System (NOAA/NCEP-GFS) were prepared for daily meteorological forecasts. Emission inventories used in this study are Model Inter-Comparison Study-Asia (MICS-Asia) 2010 for Asia and Clean Air Policy Support System (CAPSS) 2010 for South Korea. Simulated PM10 concentrations were evaluated with observed PM10 concentrations at ground monitoring sites of the AirKorea network in SMA. During the campaign period, average simulated PM10 concentrations showed significant underprediction, over 30% (~35 ㎍/㎥) lower than those observed at sites. To examine source-receptor relationship as a way to identify the cause of underprediction, we ran CAMx with Particulate matter Source Apportionment Technology (PSAT). The air quality forecasting model is based on the with 27-km horizontal grid resolution over Northeast Asia.

  8. Successful application of lead isotopes in source apportionment, legal proceedings, remediation and monitoring

    SciTech Connect

    Gulson, Brian; Korsch, Michael; Winchester, Wayne; Devenish, Matthew; Hobbs, Thad; Main, Cleve; Smith, Gerard; Rosman, Kevin; Howearth, Lynette; Burn-Nunes, Laurie; Seow, Jimmy; Oxford, Cameron; Yun, Gracie; Gillam, Lindsay; Crisp, Michelle

    2012-01-15

    In late 2006, the seaside community in Esperance Western Australia was alerted to thousands of native bird species dying. The source of the lead (Pb) was determined by Pb isotopes to derive from the handling of Pb carbonate concentrate through the Port, which began in July 2005. Concern was expressed for the impact of this on the community. Our objectives were to employ Pb isotope ratios to evaluate the source of Pb in environmental samples for use in legal proceedings, and for use in remediation and monitoring. Isotope measurements were undertaken of bird livers, plants, drinking water, soil, harbour sediments, air, bulk ceiling dust, gutter sludge, surface swabs and blood. The unique lead isotopic signature of the contaminating Pb carbonate enabled diagnostic apportionment of lead in samples. Apart from some soil and water samples, the proportion of contaminating Pb was >95% in the environmental samples. Lead isotopes were critical in resolving legal proceedings, are being used in the remediation of premises, were used in monitoring of workers involved in the decontamination of the storage facility, and monitoring transport of the concentrate through another port facility. Air samples show the continued presence of contaminant Pb, more than one year after shipping of concentrate ceased, probably arising from dust resuspension. Brief details of the comprehensive testing and cleanup of the Esperance community are provided along with the role of the Community. Lead isotopic analyses can provide significant benefits to regulatory agencies, interested parties, and the community where the signature is able to be characterised with a high degree of certainty. - Highlights: Black-Right-Pointing-Triangle Lead carbonate concentrate. Black-Right-Pointing-Triangle Successful use of Pb isotopes in identifying sources of Pb arising from transport and shipping. Black-Right-Pointing-Triangle Use of Pb isotopes in legal proceedings and their use in cleanup of residences. Black

  9. Fine particulate matter and visibility in the Lake Tahoe Basin: chemical characterization, trends, and source apportionment.

    PubMed

    Green, Mark C; Chen, L W Antony; DuBois, David W; Molenar, John V

    2012-08-01

    Speciated PM2.5 (particulate matter with an aerodynamic diameteraerosol dominated reconstructedfine mass at both sites, with 58% at Bliss State Park (BLIS) and 68% at South Lake Tahoe (SOLA). Fine mass at SOLA is 2.5 times that at BLIS, mainly due to enhanced organic and elemental carbon (OC and EC). SOLA experiences a winter peak in PM25 mainly due to OC and EC from residential wood combustion, whereas BLIS experiences a summer peak in PM2.5 mainly due to OC and ECfrom wildfires. Carbonaceous aerosol dominates visibility impairment, causing about 1/2 the reconstructed aerosol light extinction at BLIS and 70% at SOLA. Trend analysis (1990-2009) showed statistically significant decreases in aerosol extinction at BLIS on 20% best and 60% middle visibility days and statistically insignificant upward trends on 20% worst days. SOLA (1990-2003) showed statistically significant decreases in aerosol extinction for all day categories, driven by decreasing OC and EC. From the regional haze rule baseline period of 2000-2004 until 2005-2009, BLIS saw 20% best days improving and 20% worst days getting worse due to increased wildfire effects. Receptor modeling was performed using positive matrix factorization (PMF) and chemical mass balance (CMB). It confirmed that (1) biomass burning dominanted PM25 sources at both sites with increasing importance over time; (2) low combustion efficiency burning accounts for most of the biomass burning contribution; (3) road dust and traffic contributions were much higher at SOLA than at BLIS; and (4) industrial combustion and salting were minor sources.

  10. Development, testing, and application of a new Multi-Receptor (MURA) Trajectory Source Apportionment (TSA) method

    NASA Astrophysics Data System (ADS)

    Lee, Stephanie J.

    Trajectory Source Apportionment (TSA) methods are statistical techniques used to identify sources of pollution at a sampling site (receptor). TSA methods have traditionally been applied to a single receptor (Ashbaugh et al., 1985; Seibert et al., 1994; Lui et al., 2003) with some exploration of using more than one receptor (Stohl, 1996; Zeng and Hopke, 1989). A new Multi-Receptor (MURA) method was developed here. It utilizes a two step process to first identify Potential Source Regions (PSRs), and then examine them to see how often they affect each receptor. The MURA method was first tested against the conditional probability method developed by Ashbaugh et al. (1985) to determine each method's ability to detect known sources. Two artificial data sets were used; one containing a single source and one that contained four sources. The MURA method outperformed the conditional probability method. Next, the MURA method was compared to an improved version of the conditional probability method (SIRA). This test utilized three sets of artificial data in the western and eastern U.S. Although the SIRA method was an improvement over the conditional probability method, the MURA method still performed better in the four-source simulation located in the western United States. In the two eastern simulations both the MURA and SIRA methods performed similarly. The third test evaluated the impact of trajectory starting heights from 10m to 500m on the MURA method using the three simulations from the SIRA comparison. In the western simulation, the starting height had little to no impact on the accuracy of the method. In the two eastern simulations, the 10m, 50m, and 250m starting heights performed more consistently over both simulations. The MURA method was then applied to two groups of IMPROVE receptors to identify sources of sulfate and nitrate. The southwest, the western Great Plains, and the eastern Midwest affect the south central United States group for high sulfate or nitrate

  11. Source apportionment of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) in ambient air of an industrial region in Turkey

    NASA Astrophysics Data System (ADS)

    Aydin, Yagmur Meltem; Kara, Melik; Dumanoglu, Yetkin; Odabasi, Mustafa; Elbir, Tolga

    2014-11-01

    Source apportionment is generally applied to a time series of data collected at a single site. However, in a complex airshed containing several different sources, it may be helpful to collect samples from multiple sites to ensure that some of them have low contributions from specific sources, thus the boundaries can be properly defined. Ambient air polycyclic aromatic hydrocarbon (PAH) and polychlorinated biphenyls (PCB) samples (n = 160) were collected at 40 sites during four seasons (summer, fall, winter, and spring) between July 2009 and April 2010 in the heavily industrialized Aliaga region in Turkey to investigate their spatial, seasonal variations and to identify possible PAH and PCB sources. The newest version of EPA PMF (V5.0) having the capability of handling multiple site data was used for source apportionment. Five PAH sources were identified as biomass and coal combustion, iron-steel production, unburned crude oil and petroleum products, and diesel and gasoline exhaust emissions with contributions of 40, 27, 27, 3, and 3%, respectively. The sources of PCBs were identified as iron-steel production (consisting of steel-making and ship breaking activities), coal and wood combustion, and evaporative emissions from technical PCB mixtures with contributions of 57, 31, and 12%, respectively.

  12. Improved source apportionment and speciation of low-volume particulate matter samples.

    PubMed

    Schauer, James J; Majestic, Brian J; Sheesley, Rebecca J; Shafer, Martin M; Deminter, Jeffrey T; Mieritz, Mark

    2010-12-01

    New chemical analysis methods for the characterization of atmospheric particulate matter (PM)* samples were developed and demonstrated in order to expand the number of such methods for use in future health studies involving PM. Three sets of methods were, developed, for the analysis (1) of organic tracer compounds in low-volume personal exposure samples (for source apportionment), (2) of trace metals and other trace elements in low-volume personal exposure samples, and (3) of the speciation of the oxidation states of water-soluble iron (Fe), manganese (Mn), and chromium (Cr) in PM samples. The development of the second set of methods built on previous work by the project team, which had in the past used similar methods in atmospheric source apportionment studies. The principal challenges in adapting these methods to the analysis of personal exposure samples were the improvement of detection limits (DLs) and control of the low-level contamination that can compromise personal exposure samples. A secondary goal of our development efforts was to reduce the cost and complexity of the three sets of methods in order to help facilitate their broader use in future health studies. The goals of the project were achieved, and the ability to integrate the methods into existing health studies was demonstrated by way of conducting two pilot studies. The first study involved analysis of trace elements in size-resolved PM samples that had been collected to represent study subjects' personal exposures along with simultaneous measures of indoor and outdoor PM concentrations. The second study involved analysis of the speciation of organic tracer compounds in personal exposure samples, indoor samples, and outdoor samples in order to understand the diesel PM exposure of study subjects in various job classifications in an occupational setting. Both pilot studies used existing samples from. large multi-year health studies and were intended to demonstrate the feasibility and value of using

  13. Source apportionment of fine particulate matter in Phoenix, AZ, using positive matrix factorization

    SciTech Connect

    Steven G. Brown; Anna Frankel; Sean M. Raffuse; Paul T. Roberts; Hilary R. Hafner; Darcy J. Anderson

    2007-06-15

    Speciated particulate matter PM2.5 data collected as Part. of the Interagency Monitoring of Protected Visual Environments (IMPROVE) program in Phoenix, AZ, from April 2001 through October 2003 were analyzed using the multivariate receptor model, positive matrix factorization (PMF). Over 250 samples and 24 species were used, including the organic carbon and elemental carbon analytical temperature fractions from the thermal optical reflectance method. A two-step approach was used. First, the species excluding the carbon fractions were used, and initially eight factors were identified; non-soil potassium was calculated and included to better refine the burning factor. Next, the mass associated with the burning factor was removed, and the data set rerun with the carbon fractions. Results were very similar (i.e., within a few percent), but this step enabled a separation of the mobile factor into gasoline and diesel vehicle emissions. The identified factors were burning (on average 2% of the mass), secondary transport (7%), regional power generation (13%), dust (25%), nitrate (9%), industrial As/Pb/Se (2%), Cu/Ni/V (7%), diesel (9%), and general mobile (26%). Most of the long-range transport of emissions emanates from south of Phoenix in Southeastern Arizona, West Texas, and Mexico, which are significant source regions of SO{sub 2} emissions from coal- and oil-fired power plants. The overall contribution from mobile sources also increased, as some mass (OC and nitrate) from the nitrate and regional power generation factors were apportioned with the mobile factors. This approach allowed better apportionment of carbon as well as total mass. Additionally, the use of multiple supporting analyses, including air mass trajectories, activity trends, and emission inventory information, helped increase confidence in factor identification. 86 refs., 10 figs., 2 tabs.

  14. Successful application of lead isotopes in source apportionment, legal proceedings, remediation and monitoring.

    PubMed

    Gulson, Brian; Korsch, Michael; Winchester, Wayne; Devenish, Matthew; Hobbs, Thad; Main, Cleve; Smith, Gerard; Rosman, Kevin; Howearth, Lynette; Burn-Nunes, Laurie; Seow, Jimmy; Oxford, Cameron; Yun, Gracie; Gillam, Lindsay; Crisp, Michelle

    2012-01-01

    In late 2006, the seaside community in Esperance Western Australia was alerted to thousands of native bird species dying. The source of the lead (Pb) was determined by Pb isotopes to derive from the handling of Pb carbonate concentrate through the Port, which began in July 2005. Concern was expressed for the impact of this on the community. Our objectives were to employ Pb isotope ratios to evaluate the source of Pb in environmental samples for use in legal proceedings, and for use in remediation and monitoring. Isotope measurements were undertaken of bird livers, plants, drinking water, soil, harbour sediments, air, bulk ceiling dust, gutter sludge, surface swabs and blood. The unique lead isotopic signature of the contaminating Pb carbonate enabled diagnostic apportionment of lead in samples. Apart from some soil and water samples, the proportion of contaminating Pb was >95% in the environmental samples. Lead isotopes were critical in resolving legal proceedings, are being used in the remediation of premises, were used in monitoring of workers involved in the decontamination of the storage facility, and monitoring transport of the concentrate through another port facility. Air samples show the continued presence of contaminant Pb, more than one year after shipping of concentrate ceased, probably arising from dust resuspension. Brief details of the comprehensive testing and cleanup of the Esperance community are provided along with the role of the Community. Lead isotopic analyses can provide significant benefits to regulatory agencies, interested parties, and the community where the signature is able to be characterised with a high degree of certainty.

  15. Source apportionment of elevated wintertime PAHs by compound-specific radiocarbon analysis

    NASA Astrophysics Data System (ADS)

    Sheesley, R. J.; Kruså, M.; Krecl, P.; Johansson, C.; Gustafsson, Ã.-.

    2008-12-01

    Natural abundance radiocarbon analysis facilitates distinct source apportionment between contemporary biomass/biofuel (14C "alive") versus fossil fuel (14C "dead") combustion. Here, the first compound-specific radiocarbon analysis (CSRA) of atmospheric polycylic aromatic hydrocarbons (PAHs) was demonstrated for a set of samples collected in Lycksele, Sweden a small town with frequent episodes of severe atmospheric pollution in the winter. Renewed interest in residential wood combustion means than this type of seasonal pollution is of increasing concern in many areas. Five individual/paired PAH isolates from three pooled fortnight-long filter collections were analyzed by CSRA: phenanthrene, fluoranthene, pyrene, benzo[b+k]fluoranthene and indeno[cd]pyrene plus benzo[ghi]perylene; phenanthrene was the only compound also analyzed in the gas phase. The measured Δ14C for PAHs spanned from -138.3‰ to 58.0‰. A simple isotopic mass balance model was applied to estimate the fraction biomass (fbiomass) contribution that was constrained to a range of 71% for indeno[cd]pyrene+benzo[ghi]perylene to 87% for the gas phase phenanthrene and particulate fluoranthene, respectively. Indeno[cd]pyrene plus benzo[ghi]perylene, known to be enhanced in gasoline-powered motor vehicle exhaust compared to diesel exhaust, had the lowest contribution of biomass combustion of the measured PAHs by 9%. The total organic carbon (TOC, defined as carbon remaining after removal of inorganic carbon) fbiomass was estimated to be 77%, which falls within the range for PAHs. This CSRA data of atmospheric PAHs demonstrate the non-uniformity of biomass combustion contribution to different PAHs even in a location with limited local emission sources and illustrates that regulatory efforts would not evenly reduce all PAHs.

  16. Source apportionment of elevated wintertime PAHs by compound-specific radiocarbon analysis

    NASA Astrophysics Data System (ADS)

    Sheesley, R. J.; Kruså, M.; Krecl, P.; Johansson, C.; Gustafsson, Ã.-.

    2009-05-01

    Natural abundance radiocarbon analysis facilitates distinct source apportionment between contemporary biomass/biofuel (14C "alive") versus fossil fuel (14C "dead") combustion. Here, the first compound-specific radiocarbon analysis (CSRA) of atmospheric polycyclic aromatic hydrocarbons (PAHs) was demonstrated for a set of samples collected in Lycksele, Sweden a small town with frequent episodes of severe atmospheric pollution in the winter. Renewed interest in using residential wood combustion (RWC) means that this type of seasonal pollution is of increasing concern in many areas. Five individual/paired PAH isolates from three pooled fortnight-long filter collections were analyzed by CSRA: phenanthrene, fluoranthene, pyrene, benzo[b+k]fluoranthene and indeno[cd]pyrene plus benzo[ghi]perylene; phenanthrene was the only compound also analyzed in the gas phase. The measured Δ14C for PAHs spanned from -138.3‰ to 58.0‰. A simple isotopic mass balance model was applied to estimate the fraction biomass (fbiomass) contribution, which was constrained to 71-87% for the individual PAHs. Indeno[cd]pyrene plus benzo[ghi]perylene had an fbiomass of 71%, while fluoranthene and phenanthrene (gas phase) had the highest biomass contribution at 87%. The total organic carbon (TOC, defined as carbon remaining after removal of inorganic carbon) fbiomass was estimated to be 77%, which falls within the range for PAHs. This CSRA data of atmospheric PAHs established that RWC is the dominating source of atmospheric PAHs to this region of the boreal zone with some variations among RWC contributions to specific PAHs.

  17. Characteristics and source apportionment of organic matter in PM(2.5) from cities in different climatic zones of China

    NASA Astrophysics Data System (ADS)

    Feng, Jialiang

    For the first time, the dependency of the characteristics of organic matter in PM2.5 on geographical and climatic zones in three metropolitan cities of China was studied. Seasonal samples were collected at suburban and urban sites in Beijing, Shanghai and Guangzhou in 2002 and 2003. To further support the above study, seasonal samples were also collected at Changdao Island, a remote island, in Bohai Sea/Yellow Sea. Concentrations of organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and solvent-extractable organic compounds (SEOC) were analyzed. The characteristics of the n-alkanes, polycyclic aromatic hydrocarbons, n-fatty acids, n-alkanols and molecular markers such as triterpanes were determined and used for source identification. Source apportionment was complemented by Chemical Mass Balance (CMB) modeling using the measured organic species as tracers. The impact of wind speed and wind direction on air quality was studied by back trajectory calculations and analysis. In general, traffic emissions were the largest contributors of OC followed by coal burning, kitchen emissions, vegetative detritus and biomass burning. However, in the space-heating season in Northern China, coal burning was the most important contributor of OC in the suburban areas of Beijing and at Changdao. Beijing had the highest concentration of organic aerosol followed by Guangzhou and Shanghai, while seasonal variation was in reverse order. Dispersion conditions determined by local topographies and meteorology were responsible for this trend. Contrary to common understanding, pollutant concentrations at the suburban sites were higher than the urban sites in all three cities. The main reason was the rapid urbanization of the suburban areas in the immediate vicinity of urban centers since China opened up for economic development, in addition, large numbers of manufacturing plants were relocated from the cities to the countryside in an attempt to clean up the urban

  18. Winter-time size distribution and source apportionment of total suspended particulate matter and associated metals in Delhi

    NASA Astrophysics Data System (ADS)

    Srivastava, Arun; Gupta, Sandeep; Jain, V. K.

    2009-03-01

    A study of the winter time size distribution and source apportionment of total suspended particulate matter (TSPM) and associated heavy metal concentrations have been carried out for the city of Delhi. This study is important from the point of view of implementation of compressed natural gas (CNG) as alternate of diesel fuel in the public transport system in 2001 to reduce the pollution level. TSPM were collected using a five-stage cascade impactor at six sites in the winters of 2005-06. The results of size distribution indicate that a major portion (~ 40%) of TSPM concentration is in the form of PM0.7 (< 0.7 μm). Similar trends were observed with most of the heavy metals associated with various size fractions of TSPM. A very good correlation between coarse and fine size fraction of TSPM was observed. It was also observed that the metals associated with coarse particles have more chances of correlation with other metals; rather they are associated with fine particles. Source apportionment was carried out separately in coarse and fine size modes of TSPM by Chemical Mass Balance Receptor Model (CMB8) as well as by Principle Component Analysis (PCA) of SPSS. Source apportionment by PCA reveals that there are two major sources (possibly vehicular and crustal re-suspension) in both coarse and fine size fractions. Results obtained by CMB8 show the dominance of vehicular pollutants and crustal dust in fine and coarse size mode respectively. Noticeably the dominance of vehicular pollutants are now confined to fine size only whilst during pre CNG era it dominated both coarse and fine size mode. An increase of 42.5, 44.4, 48.2, 38.6 and 38.9% in the concentrations of TSPM, PM10.9, coarse particles, fine particles and lead respectively was observed during pre (2001) to post CNG (2005-06) period.

  19. Spatial distribution, potential risk assessment, and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in sediments of Lake Chaohu, China.

    PubMed

    Li, Chaocan; Huo, Shouliang; Yu, Zhiqiang; Xi, Beidou; Zeng, Xiangying; Wu, Fengchang

    2014-10-01

    Twenty-nine sediment samples were collected from Lake Chaohu, a shallow eutrophic lake in Eastern China, and were analyzed for 15 priority polycyclic aromatic hydrocarbons (PAHs) to determine the spatial distribution and exposure risks of PAHs. Three receptor models, the principal component analysis-multiple linear regression (PCA-MLR) model, the positive matrix factorization (PMF) model, and the Unmix model, were used in combination with the PAHs diagnostic ratios to investigate the potential source apportionment of PAHs. A clear gradient in the spatial distribution and the potential toxicity of PAHs was observed from west to east in the sediments of Lake Chaohu. ∑15PAH concentrations and the TEQ were in the range of 80.82-30 365.01 ng g(-1) d.w. and 40.77-614.03, respectively. The highest values of the aforementioned variables were attributed to urban-industrial pollution sources in the west lake region, and the levels decreased away from the river inlets. The three different models yielded excellent correlation coefficients between the predicted and measured levels of the 15 PAH compounds. Similarly, source apportionment results were derived from the three receptor models and the PAH diagnostic ratios, suggesting that the highest contribution to the PAHs was from coal combustion and wood combustion, followed by vehicular emissions. The PMF model yielded the following contributions to the PAHs from gasoline combustion, diesel combustion, unburned petroleum emissions, and wood combustion: 34.49, 24.61, 16.11, 13.01, and 11.78 %, respectively. The PMF model produced more detailed source apportionment results for the PAHs than the PCA-MLR and Unmix models.

  20. Comparison of receptor models for source apportionment of volatile organic compounds in Beijing, China.

    PubMed

    Song, Yu; Dai, Wei; Shao, Min; Liu, Ying; Lu, Sihua; Kuster, William; Goldan, Paul

    2008-11-01

    Identifying the sources of volatile organic compounds (VOCs) is key to reducing ground-level ozone and secondary organic aerosols (SOAs). Several receptor models have been developed to apportion sources, but an intercomparison of these models had not been performed for VOCs in China. In the present study, we compared VOC sources based on chemical mass balance (CMB), UNMIX, and positive matrix factorization (PMF) models. Gasoline-related sources, petrochemical production, and liquefied petroleum gas (LPG) were identified by all three models as the major contributors, with UNMIX and PMF producing quite similar results. The contributions of gasoline-related sources and LPG estimated by the CMB model were higher, and petrochemical emissions were lower than in the UNMIX and PMF results, possibly because the VOC profiles used in the CMB model were for fresh emissions and the profiles extracted from ambient measurements by the two-factor analysis models were "aged".

  1. Background PM2.5 source apportionment in the remote Northwestern United States

    NASA Astrophysics Data System (ADS)

    Hadley, Odelle L.

    2017-10-01

    This study used the Environmental Protection Agency's positive matrix factorization model (EPA PMF5.0) to identify five primary source factors contributing to the ambient PM2.5 concentrations at Cheeka Peak Atmospheric Observatory (CPO), Neah Bay WA between January 2011 and December 2014. CPO is home to both an IMPROVE (Interagency Monitoring for Protected Visual Environments) and a NCore multi-pollutant monitoring site. Chemically resolved particulate data from the IMPROVE site was the input data to EPA PMF5.0 and the resulting source factors were derived solely from these data. Solutions from the model were analyzed in context with trace gas and meteorological data collected at the NCore site located roughly 10 m away. Seasonal and long-term trends were analyzed for all five factors and provide the first complete source apportionment analysis of PM2.5 at this remote location. The first factor, identified as marine-traffic residual fuel oil (RFO), was the highest contributor to PM2.5 during late summer. Over the 4-year analysis, the RFO percent contribution to total PM2.5 declined. This is consistent with previous studies and may be attributed to regulations restricting the sulfur content of ship fuel. Biomass combustion emissions (BMC) and sea salt were the largest PM2.5 sources observed at CPO in winter, accounting for over 80% of the fine particulate. BMC accounted for a large percent of the fine particulate pollution when winds were easterly, or continental. Sea salt was the dominant winter factor when winds blew from the west. Measured trace carbon monoxide (CO) and reactive nitrogen species (NOy) were most strongly correlated with the BMC factor and continental winds. The fourth factor was identified as aged crustal material, or dust. In all three years, dust peaked in the spring and was associated exclusively with north-easterly winds. The last factor was identified as aged sea salt mixed with nitrate, sulfate, and other components common to RFO and BMC

  2. Chemical Characterization and Source Apportionment of Indoor and Outdoor Fine Particulate Matter (PM2.5) in Retirement Communities of the Los Angeles Basin

    PubMed Central

    Hasheminassab, Sina; Daher, Nancy; Shafer, Martin M.; Schauer, James J.; Delfino, Ralph J.; Sioutas, Constantinos

    2014-01-01

    Concurrent indoor and outdoor measurements of fine particulate matter (PM2.5) were conducted at three retirement homes in the Los Angeles Basin during two separate phases (cold and warm) between 2005 and 2006. Indoor-to-outdoor relationships of PM2.5 chemical constituents were determined and sources of indoor and outdoor PM2.5 were evaluated using a molecular marker-based chemical mass balance (MM-CMB) model. Indoor levels of elemental carbon (EC) along with metals and trace elements were found to be significantly affected by outdoor sources. EC, in particular, displayed very high indoor-to-outdoor (I/O) mass ratios accompanied by strong I/O correlations, illustrating the significant impact of outdoor sources on indoor levels of EC. Similarly, indoor levels of polycyclic aromatic hydrocarbons (PAHs), hopanes, and steranes were strongly correlated with their outdoor components and displayed I/O ratios close to unity. On the other hand, concentrations of n-alkanes and organic acids inside the retirement communities were dominated by indoor sources (e.g. food cooking and consumer products), as indicated by their I/O ratios, which exceeded unity. Source apportionment results revealed that vehicular emissions were the major contributor to both indoor and outdoor PM2.5, accounting for 39 and 46% of total mass, respectively. Moreover, the contribution of vehicular sources to indoor levels was generally comparable to its corresponding outdoor estimate. Other water-insoluble organic matter (other WIOM), which accounts for emissions from uncharacterized primary biogenic sources, displayed a wider range of contributions, varying from 2 to 73% of PM2.5, across all sites and phases of the study. Lastly, higher indoor than outdoor contribution of other water-soluble organic matter (other WSOM) was evident at some of the sites, suggesting the production of secondary aerosols as well as direct emissions from primary sources (including cleaning or other consumer products) at the

  3. Source apportionment of atmospheric pollutants based on the online data by using PMF and ME2 models at a megacity, China

    NASA Astrophysics Data System (ADS)

    Liu, Baoshuang; Yang, Jiamei; Yuan, Jie; Wang, Jiao; Dai, Qili; Li, Tingkun; Bi, Xiaohui; Feng, Yinchang; Xiao, Zhimei; Zhang, Yufen; Xu, Hong

    2017-03-01

    From 1st June to 31st August 2015, the online datasets (the water soluble inorganic ions (WSIIs), OC and EC in PM2.5, and SO2, NO2, NO) were measured continuously at Tianjin. Source apportionment of atmospheric pollutants was carried out by using PMF and ME2 models based on the online datasets. During summer in Tianjin, the ammonium sulfate/ammonium hydrogen sulfate might be major forms of sulfate in the atmospheric aerosol, while the ammonium nitrate might be major forms of nitrate. The poor correlation between OC and EC might be caused by the changes of emission sources and the production of secondary organic carbon (SOC). Five source-categories that contributed to atmospheric pollutants were extracted by PMF and ME2 models, respectively. The profiles calculated by PMF and ME2 models were consistent, and the source contributions estimated by the two models were also similar. The correlations (R2 = 0.84-0.94) were better on the time series of the contributed concentrations for the same source-category calculated from PMF and ME2 models. The source-categories were identified as secondary sources (the contribution of 25.4-26.1%), vehicle exhaust (23.3-25.4%), coal combustion (16.5-18.2%), crustal dust (13.2-14.0%) and biomass burning (9.1-10.2%). For the same source-category identified from PMF and ME2 models, the differences of profiles might be attributed to the differences of calculated methods from the two models and the uncertainties of the online datasets.

  4. Background concentrations and source apportionment of polycyclic aromatic hydrocarbons in south-eastern Finland

    NASA Astrophysics Data System (ADS)

    Vestenius, Mika; Leppänen, Sirkka; Anttila, Pia; Kyllönen, Katriina; Hatakka, Juha; Hellén, Heidi; Hyvärinen, Antti-Pekka; Hakola, Hannele

    2011-07-01

    Polycyclic aromatic hydrocarbons (PAH compounds) were measured in the PM 10 fraction [from ambient air] at Virolahti, Finland. The sampling site is located in a rural area in the south-eastern corner of Finland, near the Russian border. Altogether, 51 daily and 85 weekly filter samples were collected in 2007-2008. The yearly average concentration of benzo(a)pyrene at Virolahti in 2007 was 0.21 ng m -3, which is well below the annual target value of 1 ng m -3 set by the European Union. The positive matrix factorization (PMF) method was applied in source apportionment for daily PAH data combined with other pollutant data. A three-factor solution of the PMF analysis with 28 components was chosen. These three factors were identified as long-range transported secondary particles (F1), combustion (F2) and a sea-salt factor (F3). The conditional probability function (CPF) was used to combine wind direction sectors with the PMF factors. In cases F1 and F2, pollutants mainly originated from the south-east, whereas pollutants in F3 came from the south-western sector. PAHs entered into the combustion factor 2 together with SO 2, NO x, black carbon and potassium. This suggests that the PAHs at Virolahti originated from traffic and industrial pollution, as well as biomass burning. Elevated concentrations occurred throughout the winter period and most frequently originated from the south-eastern sector between 90°-135°. This sector includes, among other transboundary areas, the metropolis of St. Petersburg at a distance of 160 km.

  5. [Tracing Sources of Sulfate Aerosol in Nanjing Northern Suburb Using Sulfur and Oxygen Isotopes].

    PubMed

    Wei, Ying; Guo, Zhao-bing; Ge, Xin; Zhu, Sheng-nan; Jiang, Wen-juan; Shi, Lei; Chen, Shu

    2015-04-01

    Abstract: To trace the sources of sulfate contributing to atmospheric aerosol, PM2.5 samples for isotopic analysis were collected in Nanjing northern suburb during January 2014. The sulfur and oxygen isotopic compositions of sulfate from these samples were determined by EA-IRMS. Source identification and apportionment were carried out using stable isotopic and chemical evidences, combined with absolute principal component analysis (APCA) method. The Δ34S values of aerosol sulfate ranged from 2.7 per thousand to 6.4 per thousand, with an average of 5.0 per thousand ± 0.9 per thousand, while the Δ18O values ranged from 10.6 per thousand to 16.1 per thousand, with an average of 12.5 per thousand ± 1.37 per thousand. In conjunction with air mass trajectories, the results suggested that aerosol sulfates were controlled by a dominance of local anthropogenic sulfate, followed by the contributions of long-distance transported sulfate. There was a minor effect of some other low-Δ34S valued sulfates, which might be expected from biogenic sources. Absolute principal component analysis results showed that the contributions of anthropogenic sulfate and long-distance transported sulfate were 46.74% and 31.54%, respectively.

  6. The Denver Aerosol Sources and Health (DASH) study: Overview and early findings

    NASA Astrophysics Data System (ADS)

    Vedal, S.; Hannigan, M. P.; Dutton, S. J.; Miller, S. L.; Milford, J. B.; Rabinovitch, N.; Kim, S.-Y.; Sheppard, L.

    Improved understanding of the sources of air pollution that are most harmful could aid in developing more effective measures for protecting human health. The Denver Aerosol Sources and Health (DASH) study was designed to identify the sources of ambient fine particulate matter (PM 2.5) that are most responsible for the adverse health effects of short-term exposure to PM 2.5. Daily 24-h PM 2.5 sampling began in July 2002 at a residential monitoring site in Denver, Colorado, using both Teflon and quartz filter samplers. Sampling is planned to continue through 2008. Chemical speciation is being carried out for mass, inorganic ionic compounds (sulfate, nitrate and ammonium), and carbonaceous components, including elemental carbon, organic carbon, temperature-resolved organic carbon fractions and a large array of organic compounds. In addition, water-soluble metals were measured daily for 12 months in 2003. A receptor-based source apportionment approach utilizing positive matrix factorization (PMF) will be used to identify PM 2.5 source contributions for each 24-h period. Based on a preliminary assessment using synthetic data, the proposed source apportionment should be able to identify many important sources on a daily basis, including secondary ammonium nitrate and ammonium sulfate, diesel vehicle exhaust, road dust, wood combustion and vegetative debris. Meat cooking, gasoline vehicle exhaust and natural gas combustion were more challenging for PMF to accurately identify due to high detection limits for certain organic molecular marker compounds. Measurements of these compounds are being improved and supplemented with additional organic molecular marker compounds. The health study will investigate associations between daily source contributions and an array of health endpoints, including daily mortality and hospitalizations and measures of asthma control in asthmatic children. Findings from the DASH study, in addition to being of interest to policymakers, by

  7. Atmospheric Aerosol Source-Receptor Relationships: The Role of Coal-Fired Power Plants

    SciTech Connect

    Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

    2005-12-01

    This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of March 2005 through August 2005. Significant progress was made this project period on the source characterization, source apportionment, and deterministic modeling activities. This report highlights new data on road dust, vegetative detritus and motor vehicle emissions. For example, the results show significant differences in the composition in urban and rural road dust. A comparison of the organic of the fine particulate matter in the tunnel with the ambient provides clear evidence of the significant contribution of vehicle emissions to ambient PM. The source profiles developed from this work are being used by the source-receptor modeling activities. The report presents results on the spatial distribution of PMF-factors. The results can be grouped into three different categories: regional sources, local sources, or potentially both regional and local sources. Examples of the regional sources are the sulfate and selenium PMF-factors which most likely-represent coal fired power plants. Examples of local sources are the specialty steel and lead factors. There is reasonable correspondence between these apportionments and data from the EPA TRI and AIRS emission inventories. Detailed comparisons between PMCAMx predictions and measurements by the STN and IMPROVE measurements in the Eastern US are presented. Comparisons were made for the major aerosol components and PM{sub 2.5} mass in July 2001, October 2001, January 2002, and April 2002. The results are encouraging with average fraction biases for most species less than 0.25. The improvement of the model performance during the last two years was mainly due to the comparison of the model predictions with the continuous measurements in the Pittsburgh Supersite. Major improvements have included the descriptions: of ammonia emissions (CMU inventory), night time nitrate chemistry, EC emissions and their diurnal

  8. The Denver Aerosol Sources and Health (DASH) Study: Overview and Early Findings.

    PubMed

    Vedal, S; Hannigan, M P; Dutton, S J; Miller, S L; Milford, J B; Rabinovitch, N; Kim, S-Y; Sheppard, L

    2009-03-01

    Improved understanding of the sources of air pollution that are most harmful could aid in developing more effective measures for protecting human health. The Denver Aerosol Sources and Health (DASH) study was designed to identify the sources of ambient fine particulate matter (PM(2.5)) that are most responsible for the adverse health effects of short-term exposure to PM (2.5). Daily 24-hour PM(2.5) sampling began in July 2002 at a residential monitoring site in Denver, Colorado, using both Teflon and quartz filter samplers. Sampling is planned to continue through 2008. Chemical speciation is being carried out for mass, inorganic ionic compounds (sulfate, nitrate and ammonium), and carbonaceous components, including elemental carbon, organic carbon, temperature-resolved organic carbon fractions and a large array of organic compounds. In addition, water soluble metals were measured daily for 12 months in 2003. A receptor-based source apportionment approach utilizing positive matrix factorization (PMF) will be used to identify PM (2.5) source contributions for each 24-hour period. Based on a preliminary assessment using synthetic data, the proposed source apportionment should be able to identify many important sources on a daily basis, including secondary ammonium nitrate and ammonium sulfate, diesel vehicle exhaust, road dust, wood combustion and vegetative debris. Meat cooking, gasoline vehicle exhaust and natural gas combustion were more challenging for PMF to accurately identify due to high detection limits for certain organic molecular marker compounds. Measurements of these compounds are being improved and supplemented with additional organic molecular marker compounds. The health study will investigate associations between daily source contributions and an array of health endpoints, including daily mortality and hospitalizations and measures of asthma control in asthmatic children. Findings from the DASH study, in addition to being of interest to policymakers

  9. Source apportionment and water solubility of metals in size segregated particles in urban environments.

    PubMed

    Jiang, Sabrina Yanan; Kaul, Daya S; Yang, Fenhuan; Sun, Li; Ning, Zhi

    2015-11-15

    Metals in atmospheric particulate matter (PM) have been associated with various adverse health effects. Different factors contributing to the characterization and distribution of atmospheric metals in urban environments lead to uncertainty of the understanding of their impact on public health. However, few studies have provided a comprehensive picture of the spatial and seasonal variability of metal concentration, solubility and size distribution, all of which have important roles in their contribution to health effects. This study presents an experimental investigation on the characteristics of metals in PM2.5 and coarse PM in two seasons from four urban sites in Hong Kong. The PM samples were extracted separately with aqua regia and water, and a total of sixteen elements were analyzed using ICP-MS and ICP-OES to determine the size segregated concentration and solubility of metals. The concentrations of major metals were distributed in similar patterns with the same order of magnitude among different urban sites. Source apportionment using Positive Matrix Factorization (PMF) indicated that three sources namely road dust, vehicular exhaust and ship emission are major contributors to the urban atmospheric metal concentrations in Hong Kong with distinctly different profiles between coarse PM and PM2.5 fractions. The individual metals were assigned to different sources, consistent with literature documentation, except potassium emerging with substantial contribution from vehicle exhaust emission. Literature data from past studies on both local and other cities were compared to the results from the present study to investigate the impact of different emission sources and control policies on metal distribution in urban atmosphere. A large variation of solubility among the metals reflected that the majority of metals in PM2.5 were more soluble than those in coarse PM indicating size dependent chemical states of metals. The data from this study provides a rich dataset of

  10. Triple-Isotope-Based Source Apportionment of Methane in Waters of the Outer Laptev Sea

    NASA Astrophysics Data System (ADS)

    Steinbach, J.; Holmstrand, H.; Shcherbakova, K.; Kosmach, D.; Sapart, C. J.; Panova, E.; Bruchert, V.; Semiletov, I. P.; Shakhova, N. E.; Gustafsson, O.

    2015-12-01

    The East Siberian Arctic Shelf (ESAS) hosts large methane (CH4) deposits in the form of gas hydrates, gas pockets within subsea permafrost and in deeper reservoirs. For over a decade, annual expeditions have documented methane releases into the water column in large parts of this region. However, there is still insufficient knowledge of which pools are releasing the methane - one important piece of information required for a deeper understanding of the system and towards predicting future releases. A powerful tool for quantifying the relative contribution of releases from different sources is multi-dimensional isotope analysis of CH4 in the water column. Using the full triple isotope characterization (δ13C-CH4, δD-CH4, Δ14C-CH4) allows deconvolution of CH4 sources between thermogenic and biogenic origins and of different reservoir ages.During the SWERUS-C3 expedition in summer 2014 we investigated the distribution of dissolved methane and its isotope signatures in the water column along the outer ESAS and its adjacent slope and ridges. Over 1500 samples for CH4 concentration from high-resolution vertical profiles (up to 12 depths) were analyzed onboard; 900 samples were taken for stable isotopes analysis; and a total of 80 larger water samples were taken at selected locations for Δ14C-CH4 analysis. CH4 was extracted from these samples onboard using custom-built CH4-stripping systems and stored in absorbent traps for further processing and radiocarbon analysis onshore. One focus was to probe CH4 sources in seep areas, identified by a combination of geophysical features in the sediment, observation of bubbles in the water column and measured CH4 profiles. Here we present triple isotope data from inside and outside seep areas of the outer Laptev Sea and source-apportionment for this region. Dissolved methane concentration there reached up to 1400nM. Stable isotopes results in near bottom waters are rather enriched: Initial results show -142 to -133‰ vs SMOW for

  11. Seasonal effect and source apportionment of polycyclic aromatic hydrocarbons in PM2.5

    NASA Astrophysics Data System (ADS)

    Khan, Md Firoz; Latif, Mohd Talib; Lim, Chee Hou; Amil, Norhaniza; Jaafar, Shoffian Amin; Dominick, Doreena; Mohd Nadzir, Mohd Shahrul; Sahani, Mazrura; Tahir, Norhayati Mohd

    2015-04-01

    This study aims to investigate distribution and sources of 16 polycyclic aromatic hydrocarbons (PAHs) bound to fine particulate matter (PM2.5) captured in a semi-urban area in Malaysia during different seasons, and to assess their health risks. PM2.5 samples were collected using a high volume air sampler on quartz filter paper at a flow rate of 1 m3 min-1 for 24 h. PAHs on the filter paper were extracted with dichloromethane (DCM) using an ultrasonic centrifuge solid-phase extraction method and measured by gas chromatography-mass spectroscopy. The results showed that the range of PAHs concentrations in the study period was between 0.21 and 12.08 ng m-3. The concentrations of PAHs were higher during the south-west monsoon (0.21-12.08 ng m-3) compared to the north-east monsoon (0.68-3.80 ng m-3). The high molecular weight (HMW) PAHs (≥5 ring) are significantly prominent (>70%) compared to the low molecular weight (LMW) PAHs (≤4 ring) in PM2.5. The Spearman correlation indicates that the LMW and HMW PAHs correlate strongly among themselves. The diagnostic ratios (DRs) of I[c]P/I[c]P + BgP and B[a]P/B[g]P suggest that the HMW PAHs originated from fuel combustion sources. The source apportionment analysis of PAHs was resolved using DRs-positive matrix factorization (PMF)-multiple linear regression (MLR). The main sources identified were (a) gasoline combustion (65%), (b) diesel and heavy oil combustion (19%) and (c) natural gas and coal burning (15%). The health risk evaluation, by means of the lifetime lung cancer risk (LLCR), showed no potential carcinogenic risk from the airborne BaPeq (which represents total PAHs at the present study area in Malaysia). The seasonal LLCR showed that the carcinogenic risk of total PAHs were two fold higher during south-westerly monsoon compared to north-easterly monsoon.

  12. Source apportionment of organic and light-absorbing carbon using receptor modeling techniques

    NASA Astrophysics Data System (ADS)

    Malm, William C.; Gebhart, Kristi A.

    An intensive field-monitoring program designed to attribute visibility reducing aerosols to their sources or source regions was carried out in the western half of Washington state. Because of the perceived concern over the contribution of carbonaceous material from prescribed and wildfires to visibility impairment, this paper focuses on attribution of organic and light-absorbing carbon to known sources and source regions. A variety of receptor-oriented models was successfully exercised and reconciled with each other. It is shown that much of the organic and light-absorbing carbon is associated with urban emissions of the Seattle-Tacoma area. Fire tracers were not strongly linked to either organic or light-absorbing carbon; however, the fire-related tracers were shown to be primarily associated with transport from south of the Washington-Oregon state border.

  13. Chemical characterization of atmospheric particles and source apportionment in the vicinity of a steelmaking industry.

    PubMed

    Almeida, S M; Lage, J; Fernández, B; Garcia, S; Reis, M A; Chaves, P C

    2015-07-15

    The objective of this work was to provide a chemical characterization of atmospheric particles collected in the vicinity of a steelmaking industry and to identify the sources that affect PM10 levels. A total of 94 PM samples were collected in two sampling campaigns that occurred in February and June/July of 2011. PM2.5 and PM2.5-10 were analyzed for a total of 22 elements by Instrumental Neutron Activation Analysis and Particle Induced X-ray Emission. The concentrations of water soluble ions in PM10 were measured by Ion Chromatography and Indophenol-Blue Spectrophotometry. Positive Matrix Factorization receptor model was used to identify sources of particulate matter and to determine their mass contribution to PM10. Seven main groups of sources were identified: marine aerosol identified by Na and Cl (22%), steelmaking and sinter plant represented by As, Cr, Cu, Fe, Ni, Mn, Pb, Sb and Zn (11%), sinter plant stack identified by NH4(+), K and Pb (12%), an unidentified Br source (1.8%), secondary aerosol from coke making and blast furnace (19%), fugitive emissions from the handling of raw material, sinter plant and vehicles dust resuspension identified by Al, Ca, La, Si, Ti and V (14%) and sinter plant and blast furnace associated essentially with Fe and Mn (21%). Copyright © 2015 Elsevier B.V. All rights reserved.

  14. Source apportionment of ambient fine particle size distribution using positive matrix factorization in Erfurt, Germany

    PubMed Central

    Yue, Wei; Stölzel, Matthias; Cyrys, Josef; Pitz, Mike; Heinrich, Joachim; Kreyling, Wolfgang G.; Wichmann, H.-Erich; Peters, Annette; Wang, Sheng; Hopke, Philip K.

    2008-01-01

    Particle size distribution data collected between September 1997 and August 2001 in Erfurt, Germany were used to investigate the sources of ambient particulate matter by positive matrix factorization (PMF). A total of 29,313 hourly averaged particle size distribution measurements covering the size range of 0.01 to 3.0 μm were included in the analysis. The particle number concentrations (cm−3) for the 9 channels in the ultrafine range, and mass concentrations (ng m−3) for the 41 size bins in the accumulation mode and particle up to 3 μm in aerodynamic diameter were used in the PMF. The analysis was performed separately for each season. Additional analyses were performed including calculations of the correlations of factor contributions with gaseous pollutants (O3, NO, NO2, CO and SO2) and particle composition data (sulfate, organic carbon and elemental carbon), estimating the contributions of each factor to the total number and mass concentration, identifying the directional locations of the sources using the conditional probability function, and examining the diurnal patterns of factor scores. These results were used to assist in the interpretation of the factors. Five factors representing particles from airborne soil, ultrafine particles from local traffic, secondary aerosols from local fuel combustion, particles from remote traffic sources, and secondary aerosols from multiple sources were identified in all seasons. PMID:18433834

  15. Primary sources of PM2.5 organic aerosol in an industrial Mediterranean city, Marseille

    NASA Astrophysics Data System (ADS)

    El Haddad, I.; Marchand, N.; Wortham, H.; Piot, C.; Besombes, J.-L.; Cozic, J.; Chauvel, C.; Armengaud, A.; Robin, D.; Jaffrezo, J.-L.

    2010-11-01

    Marseille, the most important port of the Mediterranean Sea, represents a challenging case study for source apportionment exercises, combining an active photochemistry and multiple emission sources, including fugitive emissions from industrial sources and shipping. This paper presents a Chemical Mass Balance (CMB) approach based on organic markers and metals to apportion the primary sources of organic aerosol in Marseille, with a special focus on industrial emissions. Overall, the CMB model accounts for the major primary anthropogenic sources including motor vehicles, biomass burning, and the aggregate emissions from three industrial processes (HFO combustion/shipping, coke production and steel manufacturing) as well as some primary biogenic emissions. This source apportionment exercise is well corroborated by 14C measurements. Primary OC estimated by the CMB accounts on average for 22% and is dominated by the vehicular emissions that contribute on average for 17% of OC mass concentration (17% of PM2.5). Even though, industrial emissions contribute for only 2.3% of the total OC (7% of PM2.5), they are associated with ultrafine particles (Dp<80 nm) and high concentrations of Polycyclic Aromatic Hydrocarbons (PAH) and heavy metals such as Pb, Ni and V. On one hand, given that industrial emissions governed key primary markers, their omission would lead to substantial uncertainties in the CMB analysis performed in areas heavily impacted by such sources, hindering accurate estimation of non-industrial primary sources and secondary sources. This result implies that CMB modelling should not be a straightforward exercise and one have to carefully investigate the marker behaviours and trends beforehand, especially in complex environments such as Marseille. On the other hand, being associated with bursts of submicron particles and carcinogenic and mutagenic components such as PAH, these emissions are most likely related with acute health outcomes and should be regulated

  16. Primary sources of PM2.5 organic aerosol in an industrial Mediterranean city, Marseille

    NASA Astrophysics Data System (ADS)

    El Haddad, I.; Marchand, N.; Wortham, H.; Piot, C.; Besombes, J.-L.; Cozic, J.; Chauvel, C.; Armengaud, A.; Robin, D.; Jaffrezo, J.-L.

    2011-03-01

    Marseille, the most important port of the Mediterranean Sea, represents a challenging case study for source apportionment exercises, combining an active photochemistry and multiple emission sources, including fugitive emissions from industrial sources and shipping. This paper presents a Chemical Mass Balance (CMB) approach based on organic markers and metals to apportion the primary sources of organic aerosol in Marseille, with a special focus on industrial emissions. Overall, the CMB model accounts for the major primary anthropogenic sources including motor vehicles, biomass burning and the aggregate emissions from three industrial processes (heavy fuel oil combustion/shipping, coke production and steel manufacturing) as well as some primary biogenic emissions. This source apportionment exercise is well corroborated by 14C measurements. Primary OC estimated by the CMB accounts on average for 22% of total OC and is dominated by the vehicular emissions that contribute on average for 17% of OC mass concentration (vehicular PM contributes for 17% of PM2.5). Even though industrial emissions contribute only 2.3% of the total OC (7% of PM2.5), they are associated with ultrafine particles (Dp<80 nm) and high concentrations of Polycyclic Aromatic Hydrocarbons (PAH) and heavy metals such as Pb, Ni and V. On one hand, given that industrial emissions governed key primary markers, their omission would lead to substantial uncertainties in the CMB analysis performed in areas heavily impacted by such sources, hindering accurate estimation of non-industrial primary sources and secondary sources. On the other hand, being associated with bursts of submicron particles and carcinogenic and mutagenic components such as PAH, these emissions are most likely related with acute ill-health outcomes and should be regulated despite their small contributions to OC. Another important result is the fact that 78% of OC mass cannot be attributed to the major primary sources and, thus, remains un

  17. Simultaneous monitoring and compositions analysis of PM1 and PM2.5 in Shanghai: Implications for characterization of haze pollution and source apportionment.

    PubMed

    Qiao, Ting; Zhao, Mengfei; Xiu, Guangli; Yu, Jianzhen

    2016-07-01

    A year-long simultaneous observation of PM1 and PM2.5 were conducted at ECUST campus in Shanghai, the compositions were analyzed and compared. Results showed that PM2.5 was dominated by PM1 on clear days while the contribution of PM1-2.5 to PM2.5 increased on haze days, indicating that PM2.5 should be given priority to characterize or predict haze pollution. On haze days, accumulation of organic carbon (OC), elemental carbon (EC) and primary organic carbon (POC) in PM1-2.5 was faster than that in PM1. Humic-like substances carbon (Hulis-C) in both PM2.5 and PM1 formed faster than water soluble organic carbon (WSOC) on haze days, hence Hulis-C/WSOC increased with the intensification of haze pollution. In terms of water soluble ions, NO3(-)/SO4(2-) in PM1 increased with the aggravation of haze pollution, implying that mobile sources dominated on haze days, so is nitrogen oxidation ratio (NOR). Liquid water content (LWC) in both PM1 and PM2.5 had positive correlations with relative humidity (RH) but negative correlations with visibility, implying that hygroscopic growth might be a factor for visibility impairment, especially LWC in PM1. By comparison with multi-linear equations of LWC in PM1 and PM2.5, NO3(-) exerted a higher influence on hygroscopicity of PM1 than PM2.5, while RH, WSOC, SO4(2-) and NH4(+) had higher effects on PM2.5, especially WSOC. Source apportionment of PM2.5 was also investigated to provide reference for policy making. Cluster analysis by HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) model showed that PM2.5 originated from marine aerosols, middle-scale transportation and large-scale transportation. Furthermore, PM2.5 on haze days was dominated by middle-scale transportation. In line with source apportionment by positive matrix factorization (PMF) model, PM2.5 was attributed to secondary inorganics, aged sea salt, combustion emissions, hygroscopic growth and secondary organics. Secondary formation was the principle source of

  18. Characterization and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in Sediments from the Bohai Sea, China

    NASA Astrophysics Data System (ADS)

    Liu, Jihua; Hu, Ningjing; Shi, Xuefa

    2015-04-01

    Characterization and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in Sediments from the Bohai Sea, China Liu Jihua, Hu Ningjing, Shi Xuefa First Institute of Oceanography, State Oceanic Administration, Qingdao 266061, China Polycyclic aromatic hydrocarbons (PAHs) are a class of ubiquitous organic contaminants in the environment. Indeed, 16 PAH compounds have been listed as priority pollutants by the United States Environmental Protection Agency and the European Union because of their potential toxicity to humans and ecosystems. As POPs are released or escape into the environment, their global accumulation in marine sediments generates a complex balance between inputs and outputs. Furthermore, PAHs in coastal sediments can serve as effective tracers of materials transport from land-to-sea (Fang et al., 2009). Hence, investigations of PAHs in sediments can provide useful information for further understanding of environmental processes and material transport. In this study, sixteen polycyclic aromatic hydrocarbons (PAHs) were extracted from a total of 112 surface sediment samples collected across the entire territory of the Bohai Sea. The detectable concentrations of PAHs ranged from 97.2 to 300.7 ng/g across all samples, indicating low contamination levels of PAHs compared with reported values for other coastal sediments in China and developed countries. The highest concentrations were found within three belts in the vicinity of Luan River Estuary-Qinhuangdao Harbor, the Cao River Estuary-Bohai Sea Center, and north of the Yellow River Estuary. The distribution patterns of PAHs and source identification implied that PAH contamination in the Bohai Sea mainly originates from offshore oil exploration, sewage discharge from rivers and shipping activities. Further Principal components analysis (PCA)/multivariate linear regression (MLR) analysis suggested that the contributions of spilled oil products (petrogenic), coal combustion and traffic

  19. Source apportionment of particulate matter in a South Asian Mega City: A case study of Karachi

    NASA Astrophysics Data System (ADS)

    Shahid, imran

    2016-04-01

    PM2.5 and PM10-2.5. In order to make air quality better and risk free in South Asian cities a comprehensive and integrated regional effort is required that include continuous air quality monitoring, source apportionment and implementation of regional air quality policies.

  20. Source apportionment of particulate matter in Chinese megacities: the implication for emission control strategies

    NASA Astrophysics Data System (ADS)

    Huang, Ru-Jin; Elser, Miriam; Wang, Qiyuan Wang; Bozzetti, Carlo; Wolf, Robert; Wang, Yichen; Ni, Haiyan; Wang, Meng; Ho, Kin-Fai; Han, Yongming; Dällenbach, Kaspar; Canonaco, Francesco; Slowik, Jay; El Haddad, Imad; Baltensperger, Urs; Cao, Junji; Prévôt, André S. H.

    2015-04-01

    The rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. A quantitative understanding of these effects has proven extremely challenging due to spatial and temporal variability in the sources of aerosols and their precursors, the complexity of particle composition, and uncertainties associated with the atmospheric aging of existing particles (Pöschl 2005; Hallquist et al., 2009; Huang et al., 2014). Nowadays the average PM2.5 concentrations in China are approximately one to two orders of magnitude higher than those observed in urban areas in the US and European countries (Cao 2012). This has forced the Chinese government to announce its first national environmental standard for PM2.5 in 2012 and to make highly ambitious plans for emission control. The Chinese aim to reduce the PM2.5 concentrations by up to 25% of the 2012 levels by 2017, backed by 277 billion investments from the central government. To achieve this ambitious aim, a better understanding of the aerosol composition, sources, and atmospheric processing is required. In this study, we present the results from intensive field measurement campaigns carried out in Chinese megacities in 2013/2014. The sources of PM2.5 and the organic aerosol (OA) were investigated by applying the multi-linear engine (ME-2) receptor model (Canonaco et al., 2013) to a comprehensive dataset. Primary sources including vehicle emissions, biomass burning, coal burning, and dust-related emissions were identified and quantified. The contributions from secondary aerosol formation processes to total PM2.5 mass and OA mass were evaluated. Detailed results will be presented and discussed. References Cao, J. J. (2012) J. Earth Environ., 3, 1030

  1. Source Apportionment of PM10 by Positive Matrix Factorization in Urban Area of Mumbai, India

    PubMed Central

    Gupta, Indrani; Salunkhe, Abhaysinh; Kumar, Rakesh

    2012-01-01

    Particulate Matter (PM10) has been one of the main air pollutants exceeding the ambient standards in most of the major cities in India. During last few years, receptor models such as Chemical Mass Balance, Positive Matrix Factorization (PMF), PCA–APCS and UNMIX have been used to provide solutions to the source identification and contributions which are accepted for developing effective and efficient air quality management plans. Each site poses different complexities while resolving PM10 contributions. This paper reports the variability of four sites within Mumbai city using PMF. Industrial area of Mahul showed sources such as residual oil combustion and paved road dust (27%), traffic (20%), coal fired boiler (17%), nitrate (15%). Residential area of Khar showed sources such as residual oil combustion and construction (25%), motor vehicles (23%), marine aerosol and nitrate (19%), paved road dust (18%) compared to construction and natural dust (27%), motor vehicles and smelting work (25%), nitrate (16%) and biomass burning and paved road dust (15%) in Dharavi, a low income slum residential area. The major contributors of PM10 at Colaba were marine aerosol, wood burning and ammonium sulphate (24%), motor vehicles and smelting work (22%), Natural soil (19%), nitrate and oil burning (18%). PMID:22645437

  2. Source apportionment of PM10 at a small industrial area using Positive Matrix Factorization

    NASA Astrophysics Data System (ADS)

    Lim, Jong-Myoung; Lee, Jin-Hong; Moon, Jong-Hwa; Chung, Yong-Sam; Kim, Ki-Hyun

    2010-01-01

    In this study, PM10-bound concentrations of 28 trace metals and 3 ionic components were measured from samples collected at Daejeon Industrial Complexes I and II, Korea from April 2000 to December 2002. Positive matrix factorization (PMF) and conditional probability function (CPF) were applied to these PM data sets to identify the diverse sources in the industrial area. A total of nine source types were identified to be important which include: secondary aerosol, cement/construction, soil dust, road dust, vehicle exhaust, incineration/Pb-related industry, metal smelting, fossil fuel combustion, and field burning. Results of our study suggest that there are competing relationships between anthropogenic and natural source processes in this industrial area.

  3. COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

    SciTech Connect

    Thornton, Joel A.; Worsnop, Douglas

    2016-09-22

    This project was part of a collaborative campaign, including the participation of scientists from seven research groups as part of the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London to study wintertime sources of urban particulate matter. The UW contribution by PI Thornton’s group was to make the first deployment of a chemical ionization mass spectrometer instrument (MOVI-CI-ToFMS) to measure both particle and gas phase organic acids. The new instrument ran nearly continuously during the ClearfLo WINTER IOP at the Detling site, producing a first-ever data set of molecular composition information that can be used for source apportionment and process studies. The UW group published a paper in Environmental Science and Technology and contributed to another (Bohnenstengel et al BAMS 2015) detailing a direct molecular connection between biomass/biofuel burning particles and aerosol light absorption. The ES&T paper (Mohr, et al ES&T 2013) has received 42 citations in just 3 years indicative of its significant impact on the field. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal.

  4. High Contribution of Nonfossil Sources to Submicrometer Organic Aerosols in Beijing, China.

    PubMed

    Zhang, Yanlin; Ren, Hong; Sun, Yele; Cao, Fang; Chang, Yunhua; Liu, Shoudong; Lee, Xuhui; Agrios, Konstantinos; Kawamura, Kimitaka; Liu, Di; Ren, Lujie; Du, Wei; Wang, Zifa; Prévôt, André S H; Szidat, Sönke; Fu, Pingqing

    2017-07-18

    Source apportionment of organic carbon (OC) and elemental carbon (EC) from PM1 (particulate matter with a diameter equal to or smaller than 1 μm) in Beijing, China was carried out using radiocarbon ((14)C) measurement. Despite a dominant fossil-fuel contribution to EC due to large emissions from traffic and coal combustion, nonfossil sources are dominant contributors of OC in Beijing throughout the year except during the winter. Primary emission was the most important contributor to fossil-fuel derived OC for all seasons. A clear seasonal trend was found for biomass-burning contribution to OC with the highest in autumn and spring, followed by winter and summer. (14)C results were also integrated with those from positive matrix factorization (PMF) of organic aerosols from aerosol mass spectrometer (AMS) measurements during winter and spring. The results suggest that the fossil-derived primary OC was dominated by coal combustion emissions whereas secondary OC was mostly from fossil-fuel emissions. Taken together with previous (14)C studies in Asia, Europe and USA, a ubiquity and dominance of nonfossil contribution to OC aerosols is identified not only in rural/background/remote regions but also in urban regions, which may be explained by cooking contributions, regional transportation or local emissions of seasonal-dependent biomass burning emission. In addition, biogenic and biomass burning derived SOA may be further enhanced by unresolved atmospheric processes.

  5. Concentration levels and source apportionment of ultrafine particles in road microenvironments

    NASA Astrophysics Data System (ADS)

    Argyropoulos, G.; Samara, C.; Voutsa, D.; Kouras, A.; Manoli, E.; Voliotis, A.; Tsakis, A.; Chasapidis, L.; Konstandopoulos, A.; Eleftheriadis, K.

    2016-03-01

    A mobile laboratory unit (MOBILAB) with on-board instrumentation (Scanning Mobility Particle Sizer, SMPS; Ambient NOx analyzer) was used to measure size-resolved particle number concentrations (PNCs) of quasi-ultrafine particles (UFPs, 9-372 nm), along with NOx, in road microenvironments. On-road measurements were carried out in and around a large Greek urban agglomeration, the Thessaloniki Metropolitan Area (TMA). Two 2-week measurement campaigns were conducted during the warm period of 2011 and the cold period of 2012. During each sampling campaign, MOBILAB was driven through a 5-day inner-city route and a second 5-day external route covering in total a wide range of districts (urban, urban background, industrial and residential), and road types (major and minor urban roads, freeways, arterial and interurban roads). All routes were conducted during working days, in morning and in afternoon hours under real-world traffic conditions. Spatial classification of MOBILAB measurements involved the assignment of measurement points to location bins defined by the aspect ratio of adjacent urban street canyons (USCs). Source apportionment was further carried out, by applying Positive Matrix Factorization (PMF) to particle size distribution data. Apportioned PMF factors were interpreted, by employing a two-step methodology, which involved (a) statistical association of PMF factor contributions with 12 h air-mass back-trajectories ending at the TMA during MOBILAB measurements, and (b) Multiple Linear Regression (MLR) using PMF factor contributions as the dependent variables, while relative humidity, solar radiation flux, and vehicle speed were used as the independent variables. The applied data analysis showed that low-speed cruise and high-load engine operation modes are the two dominant sources of UFPs in most of the road microenvironments in the TMA, with significant contributions from background photochemical processes during the warm period, explaining the reversed

  6. AIRUSE-LIFE+: a harmonized PM speciation and source apportionment in 5 Southern European cities

    NASA Astrophysics Data System (ADS)

    Amato, F.; Alastuey, A.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Severi, M.; Becagli, S.; Gianelle, V. L.; Colombi, C.; Alves, C.; Custódio, D.; Nunes, T.; Cerqueira, M.; Pio, C.; Eleftheriadis, K.; Diapouli, E.; Reche, C.; Minguillón, M. C.; Manousakas, M.; Maggos, T.; Vratolis, S.; Harrison, R. M.; Querol, X.

    2015-09-01

    The AIRUSE-LIFE+ project aims at characterising similarities and heterogeneities in PM sources and contributions in urban areas from the Southern Europe. Once the main PMx sources are identified, AIRUSE aims at developing and testing the efficiency of specific and non-specific measures to improve urban air quality. This article reports the results of the source apportionment of PM10 and PM2.5 conducted at three urban background sites (Barcelona, Florence and Milan, BCN-UB, FI-UB, MLN-UB) one sub-urban background site (Athens, ATH-SUB) and one traffic site (Porto, POR-TR). After collecting 1047 PM10 and 1116 PM2.5 24 h samples from January 2013 to February 2014 simultaneously at the 5 cities, these were analysed for the contents of OC, EC, anions, cations, major and trace elements and levoglucosan. The USEPA PMF5 receptor model was applied to these datasets in a harmonised way for each city. The sum of vehicle exhaust and non-exhaust contributes within 3.9-10.8 μg m-3 (16-32 %) to PM10 and 2.3-9.4 μg m-3 (15-36 %) to PM2.5, although a fraction of secondary nitrate is also traffic-related but could not be estimated. Important contributions arise from secondary particles (nitrate, sulphate and organics) in PM2.5 (37-82 %) but also in PM10 (40-71 %) mostly at background sites, revealing the importance of abating gaseous precursors in designing air quality plans. Biomass burning (BB) contributions vary widely, from 14-24 % of PM10 in POR-TR, MLN-UB and FI-UB, 7 % in ATH-SUB to < 2 % in BCN-UB. In PM2.5, BB is the second most important source in MLN-UB (21 %) and in POR-TR (18 %), the third one in FI-UB (21 %) and ATH-SUB (11 %), but again negligible (< 2 %) in BCN-UB. This large variability among cities is mostly due to the degree of penetration of biomass for residential heating. In Barcelona natural gas is very well supplied across the city and used as fuel in 96 % of homes, while, in other cities, PM levels increase on an annual basis by 1-9 μg m-3 due to this

  7. Nanoelectrospray aerosols from microporous polymer wick sources

    NASA Astrophysics Data System (ADS)

    Tepper, Gary; Kessick, Royal

    2009-02-01

    Nanoelectrospray aerosols were formed from microporous polymer wick sources. Current-voltage characteristics were measured as a function of solution electrical conductivity and surface tension and two distinct electrospray modes were observed. In the first mode, when the maximum capillary flow rate through the wick exceeds the electrospray flow rate, a single electrospray forms from a droplet at the end of the wick. In the second mode, when the maximum capillary flow rate is less than the electrospray flow rate, a multitude of microscopic nanoelectrospray sources are formed from within the surface of the wick tip.

  8. Sources of nitrogen and phosphorus emissions to Irish rivers: estimates from the Source Load Apportionment Model (SLAM)

    NASA Astrophysics Data System (ADS)

    Mockler, Eva; Deakin, Jenny; Archbold, Marie; Daly, Donal; Bruen, Michael

    2017-04-01

    More than half of the river and lake water bodies in Europe are at less than good ecological status or potential, and diffuse pollution from agriculture remains a major, but not the only, cause of this poor performance. In Ireland, it is evident that agri-environmental policy and land management practices have, in many areas, reduced nutrient emissions to water, mitigating the potential impact on water quality. However, additional measures may be required in order to further decouple the relationship between agricultural productivity and emissions to water, which is of vital importance given the on-going agricultural intensification in Ireland. Catchment management can be greatly supported by modelling, which can reduce the resources required to analyse large amounts of information and can enable investigations and measures to be targeted. The Source Load Apportionment Model (SLAM) framework was developed to support catchment management in Ireland by characterising the contributions from various sources of phosphorus (P) and nitrogen (N) emissions to water. The SLAM integrates multiple national spatial datasets relating to nutrient emissions to surface water, including land use and physical characteristics of the sub-catchments to predict emissions from point (wastewater, industry discharges and septic tank systems) and diffuse sources (agriculture, forestry, peatlands, etc.). The annual nutrient emissions predicted by the SLAM were assessed against nutrient monitoring data for 16 major river catchments covering 50% of the area of Ireland. At national scale, results indicate that the total average annual emissions to surface water in Ireland are over 2,700 t yr-1 of P and 80,000 t yr-1 of N. The SLAM results include the proportional contributions from individual sources at a range of scales from sub-catchment to national, and show that the main sources of P are from wastewater and agriculture, with wide variations across the country related to local anthropogenic

  9. Marine submicron aerosol gradients, sources and sinks

    NASA Astrophysics Data System (ADS)

    Ceburnis, Darius; Rinaldi, Matteo; Ovadnevaite, Jurgita; Martucci, Giovanni; Giulianelli, Lara; O'Dowd, Colin D.

    2016-10-01

    Aerosol principal sources and sinks over eastern North Atlantic waters were studied through the deployment of an aerosol chemistry gradient sampling system. The chemical gradients of primary and secondary aerosol components - specifically, sea salt (SS), water-insoluble organic matter (WIOM), water-soluble organic matter (WSOM), nitrate, ammonium, oxalate, amines, methanesulfonic acid (MSA) and water-soluble organic nitrogen (WSON) - were examined in great detail. Sea salt fluxes were estimated by the boundary layer box model and ranged from 0.3 to 3.5 ng m-2 s-1 over the wind speed range of 5-12 m s-1 and compared well with the derived fluxes from existing sea salt source parameterisations. The observed seasonal pattern of sea salt gradients was mainly driven by wind stress in addition to the yet unquantified effect of marine OM modifying fractional contributions of SS and OM in sea spray. WIOM gradients were a complex combination of rising and waning biological activity, especially in the flux footprint area, and wind-driven primary sea spray production supporting the coupling of recently developed sea spray and marine OM parameterisations.

  10. Particle size distribution of indoor aerosol sources

    SciTech Connect

    Shah, K.B.

    1990-10-24

    As concern about Indoor Air Quality (IAQ) has grown in recent years, it has become necessary to determine the nature of particles produced by different indoor aerosol sources and the typical concentration that these sources tend to produce. These data are important in predicting the dose of particles to people exposed to these sources and it will also enable us to take effective mitigation procedures. Further, it will also help in designing appropriate air cleaners. A new state of the art technique, DMPS (Differential Mobility Particle Sizer) System is used to determine the particle size distributions of a number of sources. This system employs the electrical mobility characteristics of these particles and is very effective in the 0.01--1.0 {mu}m size range. A modified system that can measure particle sizes in the lower size range down to 3 nm was also used. Experimental results for various aerosol sources is presented in the ensuing chapters. 37 refs., 20 figs., 2 tabs.

  11. Source apportionment of visibility impairment using a three-dimensional source-oriented air quality model.

    PubMed

    Ying, Qi; Mysliwiec, Mitchell; Kleeman, Michael J

    2004-02-15

    A three-dimensional source-oriented Eulerian air quality model is developed that can predict source contributions to the visibility reduction. Particulate matter and precursor gases from 14 different sources (crustal material, paved road dust, diesel engines, meat cooking, noncatalyst-equipped gasoline engines, catalyst-equipped gasoline engines, high-sulfur fuel, sea salt, refrigerant losses, residential production, animals, soil and fertilizer application, other anthropogenic sources, and background sources) are tracked though a mathematical simulation of emission, chemical reaction, gas-to-particle conversion, transport, and deposition. A visibility model based on Mie theory is modified to use the calculated source contributions to airborne particulate matter size and composition as well as gas-phase pollutant concentrations to quantify total source contributions to visibility impairment. The combined air quality-visibility model is applied to predict source contributions to visibility reduction in southern California for a typical air pollution episode (September 23-25, 1996). The model successfully predicts a severe visibility reduction in the eastern portion of the South Coast Air Basin where the average daytime vi