scholarly journals Dicarboxylic acids, metals and isotopic compositions of C and N in atmospheric aerosols from inland China: implications for dust and coal burning emission and secondary aerosol formation

2010 ◽  
Vol 10 (13) ◽  
pp. 6087-6096 ◽  
Author(s):  
G. Wang ◽  
M. Xie ◽  
S. Hu ◽  
S. Gao ◽  
E. Tachibana ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Strong Dependence ◽  
Inversion Layer ◽  
Stable Carbon Isotope ◽  
Dicarboxylic Acids ◽  
Water Soluble ◽  
Total Carbon ◽  
Aerosol Formation ◽  
Coal Burning ◽  
Isotopic Compositions

Abstract. Dicarboxylic acids (C2–C10), metals, elemental carbon (EC), organic carbon (OC), and stable isotopic compositions of total carbon (TC) and total nitrogen (TN) were determined for PM10 samples collected at three urban and one suburban sites of Baoji, an inland city of China, during winter and spring 2008. Oxalic acid (C2) was the dominant diacid, followed by succinic (C4) and malonic (C3) acids. Total diacids in the urban and suburban areas were 1546±203 and 1728±495 ng m−3 during winter and 1236±335 and 1028±193 ng m−3 during spring. EC in the urban and the suburban atmospheres were 17±3.8 and 8.0±2.1 μg m−3 during winter and 20±5.9 and 7.1±2.7 μg m−3 during spring, while OC at the urban and suburban sites were 74±14 and 51±7.9 μg m−3 in winter and 51±20 and 23±6.1 μg m−3 in spring. Secondary organic carbon (SOC) accounted for 38±16% of OC in winter and 28±18% of OC in spring, suggesting an enhanced photochemical production of secondary organic aerosols in winter under an inversion layer development. Total metal elements in winter and spring were 34±10 and 61±27 μg m−3 in the urban air and 18±7 and 32±23 μg m−3 in the suburban air. A linear correlation (r2>0.8 in winter and r2>0.6 in spring) was found between primary organic carbon (POC) and Ca2+/Fe, together with a strong dependence of pH value of sample extracts on water-soluble inorganic carbon, suggesting fugitive dust as an important source of the airborne particles. Polycyclic aromatic hydrocarbons (PAHs), sulfate, and Pb in the samples well correlated each other (r2>0.6) in winter, indicating an importance of emissions from coal burning for house heating. Stable carbon isotope compositions of TC (δ13C) became higher with an increase in the concentration ratios of C2/OC due to aerosol aging. In contrast, nitrogen isotope compositions of TN (δ15N) became lower with an increases in the mass ratios of NH4+/PM10 and NO3−/PM10, which is possibly caused by an enhanced adsorption and/or condensation of gaseous NH3 and HNO3 onto particles.

scholarly journals Dicarboxylic acids, metals and isotopic compositions of C and N in atmospheric aerosols from inland China: implications for dust and coal burning emission and secondary aerosol formation

2010 ◽  
Vol 10 (3) ◽  
pp. 6895-6921 ◽  
Author(s):  
G. Wang ◽  
M. Xie ◽  
S. Hu ◽  
E. Tachibana ◽  
K. Kawamura
Keyword(s):  
Organic Carbon ◽  
Solid Phase ◽  
Strong Dependence ◽  
Inversion Layer ◽  
Dicarboxylic Acids ◽  
Water Soluble ◽  
Total Carbon ◽  
Aerosol Formation ◽  
Coal Burning ◽  
Isotopic Compositions

Abstract. Dicarboxylic acids (C2-C10), metals, elemental carbon (EC), organic carbon (OC), and stable isotopic compositions of total carbon (TC) and total nitrogen (TN) were determined for PM10 samples collected at three urban and one suburban sites of Baoji, an inland city of China, during winter and spring 2008. Oxalic acid (C2) was the dominant diacid, followed by succinic (C4) and malonic (C3) acids. Total diacids in the urban and suburban areas are 1546±203 and 1728±495 ng m−3 during winter and 1236±335 and 1028±193 ng m−3 during spring. EC in the urban and the suburban atmospheres are 17±3.8 and 8.0±2.1 μg m−3 during winter and 20±5.9 and 7.1±2.7 μg m−3 during spring whereas OC at the urban and suburban sites are 74±14 and 51±7.9 μg m−3 in winter and 51±20 and 23±6.1 μg m−3 in spring. Secondary organic carbon (SOC) accounted for 38±16% of OC in winter and 28±18% of OC in spring, suggesting an enhanced photochemical production of secondary organic aerosols in winter under an inversion layer development. Total metal elements in winter and spring are 34±10 and 61±27 μg m−3 in the urban air and 18±7 and 32±23 μg m−3 in the suburban air. A linear correlation (r2>0.8 in winter and r2>0.6 in spring) was found between primary organic carbon (POC) and Ca2+/Fe, together with a strong dependence of pH value on water-soluble inorganic carbon, suggesting fugitive dust as a major source of the airborne particles. Polycyclic aromatic hydrocarbons (PAHs), sulfate, and Pb in the samples well correlated each other (r2>0.6) in winter samples, suggesting an importance of emissions from coal burning for house heating. Stable carbon isotope compositions of TC (δ13C) became higher with an increase in the concentration ratios of C2/OC due to aerosol aging. In contrast, nitrogen isotope compositions of TN (δ15N) became lower with an increases in the mass ratios of NH4+/PM10 and NO3-/PM10 due to an enhanced adsorption and/or condensation of NH3 and HNO3 from gas phase onto solid phase.

scholarly journals Quantifying primary and secondary humic-like substances in urban aerosol based on emission source characterization and a source-oriented air quality model

2018 ◽  
Author(s):  
Xinghua Li ◽  
Junzan Han ◽  
Philip K. Hopke ◽  
Jingnan Hu ◽  
Qi Shu ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
Coal Combustion ◽  
Power Plants ◽  
Water Soluble ◽  
Aerosol Formation ◽  
Source Characterization ◽  
Air Quality Model ◽  
Coal Burning ◽  
Residential Coal

Abstract. Humic-like substances (HULIS) are a mixture of high molecular weight, water-soluble organic compounds that are widely distributed in atmospheric aerosol. Their sources are rarely studied quantitatively. Biomass burning is generally accepted as a major primary source of ambient humic-like substances (HULIS) with additional secondary material formed in the atmosphere. However, the present study provides direct evidence that residential coal burning is also a significant source of ambient HULIS, especially in the heating season in northern China based on source measurements, ambient sampling and analysis, and apportionment with source-oriented CMAQ modeling. Emissions tests show that residential coal combustion produces 5 to 24 % of the emitted organic carbon (OC) as HULIS carbon (HULISc). Estimation of primary emissions of HULIS in Beijing indicated that residential biofuel and coal burning contribute about 70 % and 25 % of annual primary HULIS, respectively. Vehicle exhaust, industry, and power plants contributions are negligible. Average concentration of ambient HULIS was 7.5 μg/m3 in atmospheric PM2.5 in urban Beijing and HULIS exhibited obvious seasonal variations with the highest concentrations in winter. HULISc account for 7.2 % of PM2.5 mass, 24.5 % of OC, and 59.5 % of water-soluble organic carbon, respectively. HULIS are found to correlate well with K+, Cl−, sulfate, and secondary organic aerosol suggesting its sources include biomass burning, coal combustion and secondary aerosol formation. Source apportionment based on CMAQ modeling shows residential biofuel and coal burning, secondary formation are important annual sources of ambient HULIS, contributing 57.5 %, 12.3 %, and 25.8 %, respectively.

scholarly journals Quantifying primary and secondary humic-like substances in urban aerosol based on emission source characterization and a source-oriented air quality model

2019 ◽  
Vol 19 (4) ◽  
pp. 2327-2341 ◽  
Author(s):  
Xinghua Li ◽  
Junzan Han ◽  
Philip K. Hopke ◽  
Jingnan Hu ◽  
Qi Shu ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
Coal Combustion ◽  
Water Soluble ◽  
Aerosol Formation ◽  
Source Characterization ◽  
Air Quality Model ◽  
Quality Model ◽  
Coal Burning ◽  
Residential Coal

Abstract. Humic-like substances (HULIS) are a mixture of high-molecular-weight, water-soluble organic compounds that are widely distributed in atmospheric aerosol. Their sources are rarely studied quantitatively. Biomass burning is generally accepted as a major primary source of ambient humic-like substances (HULIS) with additional secondary material formed in the atmosphere. However, the present study provides direct evidence that residential coal burning is also a significant source of ambient HULIS, especially in the heating season in northern China based on source measurements, ambient sampling and analysis, and apportionment with source-oriented CMAQ modeling. Emission tests show that residential coal combustion produces 5 % to 24 % of the emitted organic carbon (OC) as HULIS carbon (HULISc). Estimation of primary emissions of HULIS in Beijing indicated that residential biofuel and coal burning contribute about 70 % and 25 % of annual primary HULIS, respectively. Vehicle exhaust, industry, and power plant contributions are negligible. The average concentration of ambient HULIS in PM2.5 was 7.5 µg m−3 in urban Beijing and HULIS exhibited obvious seasonal variations with the highest concentrations in winter. HULISc accounts for 7.2 % of PM2.5 mass, 24.5 % of OC, and 59.5 % of water-soluble organic carbon. HULIS are found to correlate well with K+, Cl−, sulfate, and secondary organic aerosol, suggesting its sources include biomass burning, coal combustion, and secondary aerosol formation. Source apportionment based on CMAQ modeling shows residential biofuel and coal burning and secondary formation are important sources of ambient HULIS, contributing 47.1 %, 15.1 %, and 38.9 %, respectively.

scholarly journals Diurnal variations of organic molecular tracers and stable carbon isotopic compositions in atmospheric aerosols over Mt. Tai in North China Plain: an influence of biomass burning

2012 ◽  
Vol 12 (4) ◽  
pp. 9079-9124
Author(s):  
P. Q. Fu ◽  
K. Kawamura ◽  
J. Chen ◽  
J. Li ◽  
Y. L. Sun ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Biomass Burning ◽  
North China Plain ◽  
North China ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Total Carbon ◽  
Stable Carbon ◽  
Isotopic Compositions ◽  
Carbon Isotopic

Abstract. Organic tracer compounds of tropospheric aerosols, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated for aerosol samples collected during early and late periods of Mount Tai eXperiment 2006 (MTX2006) field campaign in North China Plain. Total solvent extracts were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in North China Plain were very active, the total identified organics (2090 ± 1170 ng m−3) were double those in late June (926 ± 574 ng m−3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88–1210 ng m−3, 403 ng m−3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude and then transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the OC in the Mt. Tai aerosols was due to biomass burning in early June, followed by the contribution of isoprene SOC (mean 4.3%). In contrast, isoprene SOC was the main contributor (6.6%) to OC, and only 3.0% of the OC was due to biomass burning in late June. In early June, δ13C of TC (−26.6‰ to −23.2‰, mean −25.0‰) were lower than those (−23.9‰ to −21.9‰, mean −22.9‰) in late June. In addition, a strong anti-correlation was found between levoglucosan and δ13C values. This study demonstrates that crop-residue burning activities can significantly enhance the organic aerosol loading and alter the organic molecular compositions and stable carbon isotopic compositions of aerosol particles in the troposphere over North China Plain.

scholarly journals Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013

2015 ◽  
Vol 15 (3) ◽  
pp. 1299-1312 ◽  
Author(s):  
Y.-L. Zhang ◽  
R.-J. Huang ◽  
I. El Haddad ◽  
K.-F. Ho ◽  
J.-J. Cao ◽  
...  
Keyword(s):  
Particulate Matter ◽  
Organic Carbon ◽  
Biomass Burning ◽  
Water Soluble ◽  
Total Carbon ◽  
World Health ◽  
Biomass Combustion ◽  
Carbonaceous Aerosols ◽  
Haze Episode ◽  
Mass Concentrations

Abstract. During winter 2013, extremely high concentrations (i.e., 4–20 times higher than the World Health Organization guideline) of PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) mass concentrations (24 h samples) were found in four major cities in China including Xi'an, Beijing, Shanghai and Guangzhou. Statistical analysis of a combined data set from elemental carbon (EC), organic carbon (OC), 14C and biomass-burning marker measurements using Latin hypercube sampling allowed a quantitative source apportionment of carbonaceous aerosols. Based on 14C measurements of EC fractions (six samples each city), we found that fossil emissions from coal combustion and vehicle exhaust dominated EC with a mean contribution of 75 ± 8% across all sites. The remaining 25 ± 8% was exclusively attributed to biomass combustion, consistent with the measurements of biomass-burning markers such as anhydrosugars (levoglucosan and mannosan) and water-soluble potassium (K+). With a combination of the levoglucosan-to-mannosan and levoglucosan-to-K+ ratios, the major source of biomass burning in winter in China is suggested to be combustion of crop residues. The contribution of fossil sources to OC was highest in Beijing (58 ± 5%) and decreased from Shanghai (49 ± 2%) to Xi'an (38 ± 3%) and Guangzhou (35 ± 7%). Generally, a larger fraction of fossil OC was from secondary origins than primary sources for all sites. Non-fossil sources accounted on average for 55 ± 10 and 48 ± 9% of OC and total carbon (TC), respectively, which suggests that non-fossil emissions were very important contributors of urban carbonaceous aerosols in China. The primary biomass-burning emissions accounted for 40 ± 8, 48 ± 18, 53 ± 4 and 65 ± 26% of non-fossil OC for Xi'an, Beijing, Shanghai and Guangzhou, respectively. Other non-fossil sources excluding primary biomass burning were mainly attributed to formation of secondary organic carbon (SOC) from non-fossil precursors such as biomass-burning emissions. For each site, we also compared samples from moderately to heavily polluted days according to particulate matter mass. Despite a significant increase of the absolute mass concentrations of primary emissions from both fossil and non-fossil sources during the heavily polluted events, their relative contribution to TC was even decreased, whereas the portion of SOC was consistently increased at all sites. This observation indicates that SOC was an important fraction in the increment of carbonaceous aerosols during the haze episode in China.

scholarly journals Contribution of dissolved organic matter to submicron water-soluble organic aerosols in the marine boundary layer over the eastern equatorial Pacific

2016 ◽  
Author(s):  
Yuzo Miyazaki ◽  
Sean Coburn ◽  
Kaori Ono ◽  
David T. Ho ◽  
R. Bradley Pierce ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Organic Carbon ◽  
Marine Boundary Layer ◽  
Organic Aerosols ◽  
Equatorial Pacific ◽  
Water Soluble ◽  
Total Carbon ◽  
Stable Carbon ◽  
Study Region ◽  
Eastern Equatorial Pacific

Abstract. Stable carbon isotopic compositions of water-soluble organic carbon (WSOC) and organic molecular markers were measured to investigate the relative contributions of the sea-surface sources to the water-soluble fraction of submicron organic aerosols collected over the eastern equatorial Pacific during the Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOCs (TORERO)/KA-12-01 cruise. On average, the water-soluble organic fraction of the total carbon (TC) mass in submicron aerosols was ~ 30–35 % in the open oceans, whereas it was ~ 60 % in the coastal oceans. The average stable carbon isotope ratio of WSOC (δ13CWSOC) was −19.8 ± 2.0 ‰, which was systematically higher than that of TC (δ13CTC) (−21.8 ± 1.4 ‰). We found that in both coastal and open oceans, the δ13CWSOC was close to the typical values of δ13C for dissolved organic carbon (DOC), ranging from −22 ‰ to −20 ‰ in surface seawater of tropical Pacific oceans. This suggests an enrichment of marine biological products in WSOC aerosols in the study region regardless of the oceanic area. In particular, enhanced levels of WSOC and biogenic organic marker compounds together with high values of WSOC/TC (~ 60 %) and δ13CWSOC were observed over upwelling areas and phytoplankton blooms, which was attributed to planktonic tissues being more enriched in δ13C. The δ13C analysis estimated that on average, marine sources contribute ~ 90 ± 25 % of the aerosol carbon, indicating the predominance of marine-derived carbon in the submicron WSOC. This conclusion is supported by Lagrangian trajectory analysis, which suggests that the majority of the sampling points on the ship had been exposed to marine boundary layer air for more than 80 % of the time during the previous 7 days. The combined analysis of the δ13C and monosaccharides, such as glucose and fructose, indicated that DOC concentration was the major factor controlling the concentration levels of the submicron WSOC regardless of the oceanic areas over the study region.

scholarly journals High time-resolved measurement of stable carbon isotope composition in water-soluble organic aerosols: method optimization and a case study during winter haze in East China

2018 ◽  
Author(s):  
Wenqi Zhang ◽  
Yan-Lin Zhang ◽  
Fang Cao ◽  
Yankun Xiang ◽  
Yuanyuan Zhang ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Carbon Isotope ◽  
Isotope Composition ◽  
Stable Carbon Isotope ◽  
Organic Aerosols ◽  
Carbon Isotope Composition ◽  
Water Soluble ◽  
High Time ◽  
Stable Carbon ◽  
Air Mass

Abstract. Water soluble organic carbon (WSOC) is a significant fraction of organic carbon (OC) in atmospheric aerosols. WSOC is of great interest due to its significant effects on atmospheric chemistry, the Earth’s climate and human health. Stable carbon isotope (δ13C) can be used to track the potential sources and investigate atmospheric processes of organic aerosols. In this study, a method of simultaneously measuring the mass concentration and δ13C values of WSOC from aerosol samples is established by coupling the Gas Bench II preparation device with isotopic ratio mass spectrometry. The precision and accuracy of isotope determination is better than 0.17 ‰ and 0.5 ‰, respectively, for samples containing carbon larger than 5 μg. This method is then applied for the high time-resolution aerosol samples during a severe wintertime haze period in Nanjing, East China. WSOC varies between 3–32 μg m−3, whereas δ13C-WSOC ranges from −26.24 ‰ to −23.35 ‰. Three different episodes (e.g., namely the Episode 1, the Episode 2, the Episode 3) are identified in the sampling period, showing a different tendency of δ13C-WSOC with the accumulation process of WSOC aerosols. The increases in both the WSOC mass concentrations and the δ13C-WSOC values in the Episode 1 indicate that WSOC is subject to a substantial photochemical aging during the air mass transport. In the Episode 2, the decline of the δ13C-WSOC is accompanied by the increase in the WSOC mass concentrations, which is associated with regional-transported biomass burning emissions. In the Episode 3, heavier isotope (13C) is exclusively enriched in total carbon (TC) compares to WSOC aerosols. This suggests that water-insoluble carbon may contain 13C-enriched components such as dust carbonate which is supported by the enhanced Ca2+ concentrations and air mass trajectories analysis. The present study provides a novel method to determine stable carbon isotope composition of WSOC and it offers a great potential to better understand the source emission, the atmospheric aging and the secondary production of water soluble organic aerosols.

scholarly journals Fossil and non-fossil sources of organic carbon (OC) and elemental carbon (EC) in Göteborg, Sweden

2009 ◽  
Vol 9 (5) ◽  
pp. 1521-1535 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
N. Perron ◽  
L. Wacker ◽  
H.-A. Synal ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Elemental Carbon ◽  
Latin Hypercube Sampling ◽  
Water Soluble ◽  
Total Carbon ◽  
Rural Site ◽  
Urban Site ◽  
Winter Period ◽  
Back Trajectories ◽  
Wood Burning

Abstract. Particulate matter was collected at an urban site in Göteborg (Sweden) in February/March 2005 and in June/July 2006. Additional samples were collected at a rural site for the winter period. Total carbon (TC) concentrations were 2.1–3.6 μg m−3, 1.8–1.9 μg m−3, and 2.2–3.0 μg m−3 for urban/winter, rural/winter, and urban/summer conditions, respectively. Elemental carbon (EC), organic carbon (OC), water-insoluble OC (WINSOC), and water-soluble OC (WSOC) were analyzed for 14C in order to distinguish fossil from non-fossil emissions. As wood burning is the single major source of non-fossil EC, its contribution can be quantified directly. For non-fossil OC, the wood-burning fraction was determined independently by levoglucosan and 14C analysis and combined using Latin-hypercube sampling (LHS). For the winter period, the relative contribution of EC from wood burning to the total EC was >3 times higher at the rural site compared to the urban site, whereas the absolute concentrations of EC from wood burning were elevated only moderately at the rural compared to the urban site. Thus, the urban site is substantially more influenced by fossil EC emissions. For summer, biogenic emissions dominated OC concentrations most likely due to secondary organic aerosol (SOA) formation. During both seasons, a more pronounced fossil signal was observed for Göteborg than has previously been reported for Zurich, Switzerland. Analysis of air mass origin using back trajectories suggests that the fossil impact was larger when local sources dominated, whereas long-range transport caused an enhanced non-fossil signal. In comparison to other European locations, concentrations of levoglucosan and other monosaccharide anhydrides were low for the urban and the rural site in the area of Göteborg during winter.

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