Seasonal Variation and Source Apportionment of Inorganic and Organic Components in PM2.5: Influence of Organic Markers Application on PMF Source Apportionment

Abstract PM2.5 samples collected over a 1-year period in a Chinese megacity were analyzed for organic carbon (OC), elemental carbon (EC), water soluble ions, elements and organic markers such as polycyclic aromatic hydrocarbons (PAHs), hopanes, steranes, and n-alkanes. In order to study the applicability of organic markers in source apportionment, this study analyzes the relationship between organic and inorganic components, and four scenarios were implemented by incorporating different combinations of organic and inorganic tracers. A positive correlation of SO42− with 4 rings PAHs can prove that coal burning directly emits a portion of sulfate. A positive correlation of NO3− with 5-7 rings PAHs are found, implying collective impacts from the vehicle source. The concentrations of OC and EC positively correlate with the 5-7 rings PAHs and Cu and Zn, which proves that part of Cu and Zn comes from vehicle emissions. Five factors were identified by incorporating only conventional components, including secondary source (SS, 30%), urban fugitive dust (UFD, 14%), cement dust (CD, 4%), traffic source (TS, 19%) and coal combustion (CC, 14%). Six factors were identified by incorporating conventional components and PAHs, including SS (28%), UFD (15%), CD (4%), CC (13%), gasoline vehicles (GV, 12%) and diesel vehicles (DV, 10%). Eight factors were identified by incorporating conventional components, PAHs, hopanes, and n-alkanes, including SS (26%), UFD (17%), CD (3%), GV (14%), DV (8%), immature coal combustion (ICC, 5%), mature coal combustion (MCC, 10%) and biogenic source (BS, 1%).

Download Full-text

Combination of Different Approaches to Infer Local or Regional Contributions to PM2.5 Burdens in Graz, Austria

Applied Sciences ◽

10.3390/app10124222 ◽

2020 ◽

Vol 10 (12) ◽

pp. 4222

Author(s):

Bernadette Kirchsteiger ◽

Magdalena Kistler ◽

Thomas Steinkogler ◽

Christopher Herzig ◽

Andreas Limbeck ◽

...

Keyword(s):

Chemical Composition ◽

Source Apportionment ◽

Water Soluble ◽

The European Union ◽

Limit Value ◽

Soluble Ions ◽

Local Sources ◽

Polycyclic Aromatic ◽

Accumulation Of Pollutants ◽

Short Time

In early 2017 high particulate matter (PM) levels were observed across mid-Europe, including Austria. Here we characterize PM pollution in the city of Graz during January to March 2017, a period with substantial exceedances (34 days) of the European Union (EU) PM10 short time limit value. This study evaluates whether the observed exceedances can be attributed to the accumulation of pollutants emitted by local sources or to a larger scale pollution episode including transport. The analyses are based on the ratios of PM10 concentrations determined at an urban and background site, and the analyses of chemical composition of PM2.5 samples (i.e., water soluble ions, organic and elemental carbon, anhydro-sugars, humic-like substances, aluminum, and polycyclic aromatic hydrocarbons). Source apportionment was realized using a macro-tracer model. Overall, the combination of different approaches (PM10 ratios, chemical composition, and macro-tracer derived source apportionment) enabled a conclusive identification of time periods characterized by the accumulation of emissions from local sources or regional pollution episodes.

Download Full-text

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

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-8247-2017 ◽

2017 ◽

Vol 17 (13) ◽

pp. 8247-8268 ◽

Cited By ~ 31

Author(s):

Carlo Bozzetti ◽

Imad El Haddad ◽

Dalia Salameh ◽

Kaspar Rudolf Daellenbach ◽

Paola Fermo ◽

...

Keyword(s):

Source Apportionment ◽

Coke Production ◽

Water Soluble ◽

Biomass Combustion ◽

Seasonal Trends ◽

Soluble Ions ◽

Yearly Average ◽

Polycyclic Aromatic ◽

Field Deployment ◽

A Minor

Abstract. 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 a unique coal combustion and coke production marker. Online- and offline-AMS source apportionments revealed evolving levoglucosan : BBOA ratios, which were higher during late autumn and March. A similar seasonality was observed in the ratios of cellulose combustion markers to lignin combustion markers, highlighting the contribution from cellulose-rich biomass combustion, possibly related to agricultural activities.

Download Full-text

Measurement on PM and its chemical compositions for real-world emissions from non-road and on-road diesel vehicles

10.5194/acp-2016-1038 ◽

2016 ◽

Author(s):

Min Cui ◽

Yingjun Chen ◽

Cheng Li ◽

Junyu Zheng ◽

Chongguo Tian ◽

...

Keyword(s):

Real World ◽

Water Soluble ◽

Chemical Compositions ◽

Fuel Quality ◽

Operating Modes ◽

Diesel Vehicles ◽

Emission Standards ◽

Soluble Ions ◽

Wide Range ◽

Polycyclic Aromatic

Abstract. With increasing population of both non-road and on-road diesel vehicles, the adverse effects of PM and its compositions (such as elemental carbon (EC), polycyclic aromatic hydrocarbons (PAHs)) on air quality and human health get more and more attention. However, characteristics of PM and its compositions emitted from diesel vehicles, particularly measured under real-world condition, are scarce. In this study, six excavators and five trucks, involving wide-range emission standards and working in different operating modes, were tested to characterize constituents of PM (including organic carbon (OC), EC, water soluble ions (WSIs), elements, and organic species such as PAHs, n-alkanes, hopanes and steranes). The average emission factors of PM (EFPM) for excavators and trucks were 829 ± 806 and 498 ± 234 mg kg−1 fuel, respectively, which are comparable with other studies. However, EFPM was significantly affected by fuel quality, operating modes and emission standards. High correlation (R2 = 0.79, p

Download Full-text

Aerosols chemical composition, light extinction, and source apportionment near a desert margin city, Yulin, China

PeerJ ◽

10.7717/peerj.8447 ◽

2020 ◽

Vol 8 ◽

pp. e8447 ◽

Cited By ~ 2

Author(s):

Yali Lei ◽

Zhenxing Shen ◽

Zhuoyue Tang ◽

Qian Zhang ◽

Jian Sun ◽

...

Keyword(s):

Source Apportionment ◽

Coal Combustion ◽

Vehicle Emissions ◽

Principal Component ◽

Water Soluble ◽

Light Extinction ◽

Potential Contribution ◽

Light Extinction Coefficient ◽

Soluble Ions ◽

Chemical Profiles

Daily PM10and PM2.5 sampling was conducted during four seasons from December 2013 to October 2014 at three monitoring sites over Yulin, a desert margin city. PM10 and PM2.5 levels, water soluble ions, organic carbon (OC), and elemental carbon (EC) were also analyzed to characterize their chemical profiles. bext (light extinction coefficient) was calculated, which showed the highest in winter with an average of 232.95 ± 154.88 Mm−1, followed by autumn, summer, spring. Light extinction source apportionment results investigated (NH4)2SO4 and NH4NO3 played key roles in the light extinction under high RH conditions during summer and winter. Sulfate, nitrate and Ca2 + dominated in PM10/PM2.5 ions. Ion balance results illustrated that PM samples were alkaline, and PM10 samples were more alkaline than PM2.5. High SO42−/K+ and Cl−/K+ ratio indicated the important contribution of coal combustion, which was consistent with the OC/EC regression equation intercepts results. Principal component analysis (PCA) analyses results showed that the fugitive dust was the most major source of PM, followed by coal combustion & gasoline vehicle emissions, secondary formation and diesel vehicle emissions. Potential contribution source function (PSCF) results suggested that local emissions, as well as certain regional transport from northwesterly and southerly areas contributed to PM2.5 loadings during the whole year. Local government should take some measures to reduce the PM levels.

Download Full-text

Measurement of PM2.5 and Water-Soluble Ions at Central Tokyo, Japan and Source Apportionment

The Global Environmental Engineers ◽

10.15377/2410-3624.2015.02.02.4 ◽

2016 ◽

Vol 2 (2) ◽

pp. 71-78

Author(s):

Yoshika Sekine ◽

◽

Nami Takahashi ◽

Yuri Ohkoshi ◽

Akihiro Takemasa ◽

...

Keyword(s):

Source Apportionment ◽

Water Soluble ◽

Soluble Ions ◽

Water Soluble Ions

Download Full-text

Characteristics of concentrations and chemical compositions for PM<sub>2.5</sub> in the region of Beijing, Tianjin, and Hebei, China

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-863-2013 ◽

2013 ◽

Vol 13 (1) ◽

pp. 863-901 ◽

Cited By ~ 9

Author(s):

P. S. Zhao ◽

F. Dong ◽

D. He ◽

X. J. Zhao ◽

W. Z. Zhang ◽

...

Keyword(s):

Coal Combustion ◽

Urban Areas ◽

Motor Vehicle ◽

Water Soluble ◽

Photochemical Oxidation ◽

Chemical Compositions ◽

Soluble Ions ◽

Secondary Ions ◽

Water Soluble Ions ◽

Autumn And Winter

Abstract. In order to study the temporal and spatial variations of PM2.5 and its chemical compositions in the region of Beijing, Tianjin, and Hebei (BTH), PM2.5 samples were collected at four urban sites in Beijing (BJ), Tianjin (TJ), Shijiazhuang (SJZ), and Chengde (CD) and one site at Shangdianzi (SDZ) regional background station over four seasons from 2009 to 2010. The samples were weighted for mass concentrations and analyzed in laboratory for chemical profiles of 19 elements (Al, As, Ba, Ca, Cd, Co, Cr, Cu, Fe, K, Mg, Mn, Ni, P, Pb, Sr, Ti, V, and Zn), eight water-soluble ions (Na+, NH4+, K+, Mg2+, Ca2+, Cl−, NO3−, and SO42−), and carbon fractions (OC and EC). The concentrations of PM2.5 and its major chemical species were season-dependent and showed spatially similar characteristics in the plain area of BTH. The average annual concentrations of PM2.5 were 71.8–191.2 μg m−3 at five sites, with more than 90 % sampling days exceeded 50 μg m−3 at BJ, TJ, and SJZ. PM2.5 pollution was most serious at SJZ, and the annual concentrations of PM2.5, secondary ions, OC, EC, and most of crustal elements were all highest. Due to stronger photochemical oxidation, the sum of concentrations of secondary ions (NH4+, NO3−, and SO42−) was highest in the summer at SDZ, BJ, TJ, and CD. Analysis of electric charges of water-soluble ions indicated the existence of nitric acid or hydrochloric acid in PM2.5. For all five sites, the concentrations of OC, EC and also secondary organic carbon (SOC) in the spring and summer were lower than those in the autumn and winter. Stable atmosphere and low temperatures appearing more frequently during autumn and winter facilitated the formation of SOC. The sums of crustal elements (Al, Ca, Fe, Mg, Ti, Ba, and Sr) were higher in the spring and autumn owing to more days with blowing or floating dust. The concentrations of heavy metals were at higher levels in the BTH area by comparison with other studies. In Shijiazhuang and Chengde, the PM2.5 pollution was dominated by coal combustion. Motor vehicle exhausts and coal combustion emissions both played important role in Tianjin PM2.5$ pollution. However, motor vehicle exhausts had played more important role in Beijing owing to the reduction of coal consumption and sharply increase of cars in recent years. At SDZ, regional transportation of air pollutants from southern urban areas was significant.

Download Full-text

Emission and simulation of primary fine and submicron particles and water-soluble ions from domestic coal combustion in China

Atmospheric Environment ◽

10.1016/j.atmosenv.2020.117308 ◽

2020 ◽

Vol 224 ◽

pp. 117308 ◽

Cited By ~ 3

Author(s):

Qin Yan ◽

Shaofei Kong ◽

Yingying Yan ◽

Haibiao Liu ◽

Wei Wang ◽

...

Keyword(s):

Coal Combustion ◽

Water Soluble ◽

Submicron Particles ◽

Soluble Ions ◽

Water Soluble Ions

Download Full-text

Evaluation of organic markers for chemical mass balance source apportionment at the Fresno Supersite

Atmospheric Chemistry and Physics ◽

10.5194/acp-7-1741-2007 ◽

2007 ◽

Vol 7 (7) ◽

pp. 1741-1754 ◽

Cited By ~ 105

Author(s):

J. C. Chow ◽

J. G. Watson ◽

D. H. Lowenthal ◽

L. W. A. Chen ◽

B. Zielinska ◽

...

Keyword(s):

Mass Balance ◽

Source Apportionment ◽

Vehicle Emissions ◽

Motor Vehicle ◽

Simulated Data ◽

Water Soluble ◽

Chemical Mass Balance ◽

Wood Combustion ◽

Organic Markers ◽

Diesel Vehicle

Abstract. Sources of PM2.5 at the Fresno Supersite during high PM2.5 episodes occurring from 15 December 2000–3 February 2001 were estimated with the Chemical Mass Balance (CMB) receptor model. The ability of source profiles with organic markers to distinguish motor vehicle, residential wood combustion (RWC), and cooking emissions was evaluated with simulated data. Organics improved the distinction between gasoline and diesel vehicle emissions and allowed a more precise estimate of the cooking source contribution. Sensitivity tests using average ambient concentrations showed that the gasoline vehicle contribution was not resolved without organics. Organics were not required to estimate hardwood contributions. The most important RWC marker was the water-soluble potassium ion. The estimated cooking contribution did not depend on cholesterol because its concentrations were below the detection limit in most samples. Winter time source contributions were estimated by applying the CMB model to individual and average sample concentrations. RWC was the largest source, contributing 29–31% of measured PM2.5. Hardwood and softwood combustion accounted for 16–17% and 12–15%, respectively. Secondary ammonium nitrate and motor vehicle emissions accounted for 31–33% and 9–15%, respectively. The gasoline vehicle contribution (3–10%) was comparable to the diesel vehicle contribution (5–6%). The cooking contribution was 5–19% of PM2.5. Fresno source apportionment results were consistent with those estimated in previous studies.

Download Full-text

The relative importance of tailpipe and non-tailpipe emissions on the oxidative potential of ambient particles in Los Angeles, CA

Faraday Discussions ◽

10.1039/c5fd00166h ◽

2016 ◽

Vol 189 ◽

pp. 361-380 ◽

Cited By ~ 25

Author(s):

Farimah Shirmohammadi ◽

Sina Hasheminassab ◽

Dongbin Wang ◽

James J. Schauer ◽

Martin M. Shafer ◽

...

Keyword(s):

Los Angeles ◽

Chemical Constituents ◽

Univariate Analysis ◽

Water Soluble ◽

Crustal Material ◽

Relative Importance ◽

Oxidative Potential ◽

Carbonaceous Species ◽

Soluble Ions ◽

Polycyclic Aromatic

This study examines the associations between the oxidative potential of ambient PM2.5and PM0.18, measured by means of the dithiothreitol (DTT) assay, and their chemical constituents and modeled sources. Particulate matter (PM) samples were collected from 2012–2013 in Central Los Angeles (LA) and 2013–2014 in Anaheim, California, USA. Detailed chemical analyses of the PM samples, including carbonaceous species, inorganic elements and water-soluble ions, were conducted. Univariate analysis indicated a high correlation (R> 0.60) between the DTT activity and the concentrations of carbonaceous species at both sites. The strongest correlations were observed between DTT and organic tracers of primary vehicle tailpipe emissions including polycyclic aromatic hydrocarbons (PAHs) and hopanes as well as EC, with higher correlations for PM0.18versusPM2.5components. Moreover, metals and trace elements (e.g., Ba, Cu, Fe, Mn, Pb and Sb) in both size ranges were also associated with DTT activity. Multiple linear regression (MLR) analysis was performed on DTT activity and PM sources identified by a Molecular Marker-Chemical Mass Balance (MM-CMB) model (i.e.major carbonaceous sources: vehicle tailpipe emissions, wood smoke, primary biogenic and secondary organic carbon) together with other typical sources of ambient PM (i.e.crustal material, vehicular abrasion, secondary ions and sea salt). Overall, our findings illustrate the relative importance of different traffic sources on the oxidative potential of ambient PM. Despite major reductions of tailpipe emissions, the lack of similar reductions (and possibly an increase) in non-tailpipe emissions makes them an important source of traffic-related PM in Los Angeles and their increasing role in the overall PM toxicity raises concerns for public health.

Download Full-text

Large contribution of fossil-fuel derived secondary organic carbon to water-soluble organic aerosols in winter haze of China

10.5194/acp-2017-1130 ◽

2017 ◽

Author(s):

Yan-Lin Zhang ◽

Imad El-Haddad ◽

Ru-Jin Huang ◽

Kin-Fai Ho ◽

Jun-Ji Cao ◽

...

Keyword(s):

Organic Carbon ◽

Source Apportionment ◽

Atmospheric Chemistry ◽

Coal Combustion ◽

Large Fraction ◽

Organic Aerosols ◽

Water Soluble ◽

Primary Sources ◽

Large Contribution ◽

Secondary Organic Carbon

Abstract. Water-soluble organic carbon (WSOC) is a large fraction of organic aerosols (OA) globally and has significant impacts on climate and human health. The sources of WSOC remain very uncertain in polluted regions. Here we present a quantitative source apportionment of WSOC isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time-of-flight aerosol mass spectrometer measurements. Fossil emissions on average accounted for 32–47 % of WSOC. Secondary organic carbon (SOC) dominated both the non-fossil and fossil derived WSOC, highlighting the importance of secondary formation to WSOC in severe winter haze episodes. Contributions from fossil emissions to SOC were 61 ± 4 % and 50 ± 9 % in Shanghai and Beijing, respectively, significantly larger than those in Guangzhou (36 ± 9 %) and Xi'an (26 ± 9 %). The most important primary sources were biomass burning emissions, contributing 17–26 % of WSOC. The remaining primary sources such as coal combustion, cooking and traffic were generally very small but not negligible contributors, as coal combustion contribution could exceed 10 %. Taken together with earlier 14C source apportionment studies in urban, rural, semi-urban, and background regions in Asia, Europe and USA, we demonstrated a dominant contribution of non-fossil emissions (i.e., 75 ± 11 %) to WSOC aerosols in the North Hemisphere; however, the fossil fraction is substantially larger in aerosols from East Asia and the East Asian pollution outflow especially during winter due to increasing coal combustion. Inclusion of our findings can improve a modelling of effects of WSOC aerosols on climate, atmospheric chemistry and public health.

Download Full-text