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1.
Sci Total Environ ; 703: 134475, 2020 Feb 10.
Artigo em Inglês | MEDLINE | ID: mdl-31759721

RESUMO

Organic molecular composition of fine aerosols in the free troposphere is poorly understood. Here, PM2.5 (particles with aerodynamic diameters ≤ 2.5 µm) samples were collected at the summit of Mt. Emei (3080 m a.s.l.) in the Southwestern China on a daytime and nighttime basis during summer 2016 (June-July). The samples were analyzed by solvent-extraction followed by derivatization and gas chromatography/mass spectrometry (GC/MS). Four classes of organic compounds, i.e. n-alkanes, fatty acids, saccharides and lignin/resin acids were measured quantitatively. Fatty acids were found to be the most abundant species with an average concentration of 401 ±â€¯419 ng m-3 (range 25.7-1490 ng m-3) in the daytime, similar to the average concentration at night (399 ±â€¯447 ng m-3, 19.6-1970 ng m-3). However, the concentrations of biomass burning tracers (e.g., levoglucosan), primary biological aerosol tracers (e.g., mannitol and arabitol) and low molecular weight n-alkanes derived from fossil fuel combustion in daytime samples were obviously higher than those in nighttime samples. The results suggest that valley breezes transported a large number of aerosols and their precursors from the ground surface to the summit of Mt. Emei in the daytime. Estimated with tracer-based methods, the contributions of biogenic primary sources (plant debris, fungal spore, and biomass burning) to organic carbon was in the range of 3.28-83.5% (22.0 ±â€¯17.5%) in the daytime and 3.45-37.4% (10.9 ±â€¯8.97%) at night. As the largest contributor, biomass burning was an important anthropogenic/natural source of aerosol particles in the free troposphere over Mt. Emei. CAPSULE: Valley/mountain breeze is an important constraint to the temporal variations in organic aerosols over Mt. Emei.

2.
Chemosphere ; 241: 125133, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31683427

RESUMO

Black carbon (BC) plays a vital role in atmospheric environment and climate change. Temporal variations and transport pathways of BC in Xiamen, China with the impacts of synoptic circulation were investigated in 2014 with Aethalometer. Annual mean BC concentration was 4270 ng m-3. BC exhibited clear diurnal (seasonal) variations, with the maximum of 6182 (4755) ng m-3 at 6:00 (in spring) and minimum of 2847 (3774) ng m-3 at 13:00 (in summer). Conditional probability function analysis indicated that high BC concentrations were associated with northwesterly winds with low wind speed. Air masses originating from the East China Sea and passing along with East China Coast had the highest BC concentrations. Potential source contribution function and concentration weighted trajectory analysis suggested that major sources for BC included the surrounding region, southwestern Fujian and eastern Guangdong to the southwest, Hubei, Hunan and Jiangxi to the northwest, the East China Sea and the South China Sea. Of the nine synoptic circulation patterns, three cyclone-related patterns were associated with low BC concentrations and small biomass burning (BCbb) contributions. Of the six anticyclone-related patterns, the three cold-high circulations around winter were associated with moderate BC concentrations and large BCbb contributions. The two cold-high patterns in spring and autumn were associated with high BC concentrations and small BCbb contributions, while the warm-high pattern was associated with moderate BC concentration and small BCbb contribution. The findings provide insights into the transport mechanisms of BC with the impacts of synoptic pattern in China.

3.
Environ Sci Technol ; 53(13): 7380-7390, 2019 07 02.
Artigo em Inglês | MEDLINE | ID: mdl-31117537

RESUMO

Aerosol proteinaceous matter is comprised of a substantial fraction of bioaerosols. Its origins and interactions in the atmosphere remain poorly understood. We present observations of total proteins, combined, and free amino acids (CAAs and FAAs) in fine particulate matter (PM2.5) samples in urban Beijing before and during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. The decreases in proteins, CAAs and FAAs levels were observed after the implementation of restrictive emission controls. Significant changes were observed for the composition profiles in FAAs with the predominance of valine before the APEC and glycine during the APEC, respectively. These variations could be attributed to the influence of sources, atmospheric processes, and meteorological conditions. FAAs (especially valine and glycine) were suggested to be released by the degradation of high molecular weight proteins/polypeptides by atmospheric oxidants (i.e., ozone and free radicals) and nitrogen dioxide. Besides daytime reactions, nighttime chemistry was found to play an important role in the atmospheric formation of valine during the nights, suggesting the possible influence of NO3 radicals. Our findings provide new insights into the significant impacts of atmospheric oxidation capacity on the occurrence and transformation of aerosol proteinaceous matter which may affect its environmental, climate and health effects.


Assuntos
Poluentes Atmosféricos , Aerossóis , Ásia , Pequim , Monitoramento Ambiental , Material Particulado
4.
Environ Pollut ; 243(Pt B): 1579-1587, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30293040

RESUMO

Sugars and n-alkanes are important organic constituents of atmospheric fine particulate matter (PM2.5). For better understanding their sources and seasonal variations in urban atmosphere, sugar compounds (anhydrosugars, sugars and sugar alcohols) and homologue n-alkanes (C18-C37) were studied in PM2.5 samples collected from September 2013 to July 2014 in Beijing, China. In general, all measured compounds showed the lowest levels in summer. Higher concentrations of sugar compounds and n-alkanes were observed in winter, probably due to elevated combustion emissions (e.g., coal, biofuel and agricultural residue burning) and stable meteorological conditions during heating season. Levoglucosan was the major sugar species in all seasons particularly in autumn and winter, highlighting the significant contribution of biomass burning to fine organic aerosols throughout the whole year especially in cold seasons. Plant waxes contributed to n-alkanes the most in late spring (54.5%) and the least in winter (11.6%); while fossil fuel combustion had the largest contribution in winter (385 ng m-3). The weak odd-carbon predominance of n-alkanes in wintertime aerosols also suggests fossil fuel combustion as the important source of organic aerosols in the heating season. Soil resuspension, fossil fuel combustion and biomass burning, and secondary sources are the main sources of OC in PM2.5 at Beijing. The seasonal variation in source contributions indicates that meteorological condition is a key factor in controlling PM2.5 levels. Furthermore, dust storms in spring can strongly enhance the atmospheric level of fine organic matter in Beijing.


Assuntos
Poluentes Atmosféricos/análise , Alcanos/análise , Monitoramento Ambiental/métodos , Combustíveis Fósseis/análise , Material Particulado/análise , Material Particulado/química , Açúcares/análise , Aerossóis/análise , Atmosfera/química , Pequim , Biomassa , Carbono/análise , China , Estações do Ano , Solo/química
5.
Environ Pollut ; 243(Pt B): 919-928, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30245454

RESUMO

Organic tracers are useful for investigating the sources of carbonaceous aerosols but there are still no adequate studies in China. To obtain insights into the diurnal variations, properties, and the influence of regional emission controls on carbonaceous aerosols in Beijing, day-/nighttime PM2.5 samples were collected before (Oct. 15th - Nov. 2nd) and during (Nov. 3rd - Nov. 12th) the 2014 Asia-Pacific Economic Cooperation (APEC) summit. Eleven organic compound classes were analysed using gas chromatography/mass spectrometry (GC/MS). In addition, the stable carbon isotope ratios (δ13CTC) of total carbon (TC) were detected using an elemental analyser/isotope ratio mass spectrometry (EA/irMS). Most of the organic compounds were more abundant during the night than in the daytime, and their concentrations generally decreased during the APEC. These features were associated with the strict regional emission controls and meteorological conditions. The day/night variations of δ13CTC were smaller during the APEC than those before the APEC the summit, suggesting that regionally transported aerosols are potentially played an important role in the loading of organic aerosols in Beijing before the APEC summit. The source apportionment based on the organic tracers suggested that biomass burning, plastic and microbial emissions, and fossil fuel combustion were important sources of organic aerosols in Beijing. Furthermore, a similar contribution of biomass burning to OC before and during the APEC suggests biomass burning was a persistent contributor to PM2.5 in Beijing and its surroundings.


Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental , Material Particulado/análise , Aerossóis/análise , Poluição do Ar/estatística & dados numéricos , Ásia , Pequim , Biomassa , Carbono/análise , Isótopos de Carbono/análise , China , Cromatografia Gasosa-Espectrometria de Massas , Compostos Orgânicos/análise , Estações do Ano
6.
Sci Total Environ ; 633: 1156-1164, 2018 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-29758867

RESUMO

Pervasive particulate pollution has been observed over large areas of the North China Plain. The high level of sulfate, a major component in fine particles, is pronounced during heavy pollution periods. Being different from source apportionments by atmospheric chemistry-transport model and receptor modeling methods, here we utilize sulfur isotopes to discern the potential emission sources. Sixty-five daily PM2.5 samples were collected at an urban site in Beijing between September 2013 and July 2014. Inorganic ions, organic/elemental carbon and stable sulfur isotopes of sulfate were analyzed. The "fingerprint" characteristics of stable sulfur isotopic composition, together with trajectory clustering modeled by HYSPLIT-4 (HYbrid Single-Particle Lagrangian Integrated Trajectory) and FLEXPART ("FLEXible PARTicle dispersion model"), was employed to identify potential aerosol sources in Beijing. Results exhibited a distinctive seasonality with sulfate, nitrate, ammonium, organic matter, and element carbon being the dominant species of PM2.5. Elevated concentrations of chloride with high organic matter were found in autumn and winter as a result of enhanced fossil fuel (mainly coal) combustion. The δ34S values of the Beijing aerosols ranged from 2.8‰ to 9.9‰ with an average of 6.0 ±â€¯1.8‰, further indicating that the major sulfur source was direct coal burning emission. Owing to the changing patterns between oxidation pathways of S(IV) in different seasons, δ34S values varied with a winter maximum (8.2 ±â€¯1.1‰) and a summer minimum (4.9 ±â€¯1.9‰). The results of trajectory clustering and FLEXPART demonstrated that higher concentrations of sulfate with lower sulfur isotope ratios (4.6 ±â€¯0.8‰) were associated with air masses from the south or east, whereas lower sulfate concentrations with heavier sulfur isotope ratios (6.7 ±â€¯1.6‰) were observed when the air masses were mainly from the north or northwest. These results suggested that the fine aerosol pollution in Beijing, especially sulfate pollution, was mainly due to coal combustion sources from regional and local regions.

7.
Environ Sci Technol ; 51(14): 7842-7852, 2017 Jul 18.
Artigo em Inglês | MEDLINE | ID: mdl-28648047

RESUMO

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 (14C) 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. 14C 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 14C 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.


Assuntos
Aerossóis , Poluentes Atmosféricos , Monitoramento Ambiental , Ásia , Pequim , Carbono , China , Europa (Continente) , Material Particulado
8.
Sci Rep ; 6: 27481, 2016 06 08.
Artigo em Inglês | MEDLINE | ID: mdl-27270951

RESUMO

Molecular distributions and stable carbon isotopic compositions (δ(13)C) of n-alkanes, fatty acids and n-alcohols were investigated in urban aerosols from Beijing, northern China to better understand the sources and long-range atmospheric transport of terrestrial organic matter during polluted and clear days in winter. n-Alkanes (C19-C36), fatty acids (C8-C32) and n-alcohols (C16-C32) detected in Beijing aerosols are characterized by the predominance of C23, C16 and C28, respectively. Carbon preference index (CPI) values of n-alkanes, the ratios of the sum of odd-numbered n-alkanes to the sum of even-numbered n-alkanes, are close to 1, indicating a heavy influence of fossil fuel combustion. Relatively higher ratios of C(18:0+16:0)/C(18:n+16:1) (fatty acids) on clear days than polluted days indicate that long-distance transport and/or photochemical aging are more significant during clear days. δ(13)C values of n-alkanes and low molecular weight fatty acids (C16:0, C18:0) ranged from -34.1 to -24.7% and -26.9 to -24.6%, respectively, which are generally heavier on polluted days than those on clear days. Such a wide range suggests that atmospheric lipids in Beijing aerosols originate from multiple sources and encounter complicated atmospheric processes during long-range transport in North China.

9.
Sci Rep ; 5: 9845, 2015 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-25920042

RESUMO

Organic aerosols are ubiquitous in the earth's atmosphere. They have been extensively studied in urban, rural and marine environments. However, little is known about the fluorescence properties of water-soluble organic carbon (WSOC) or their transport to and distribution in the polar regions. Here, we present evidence that fluorescent WSOC is a substantial component of High Arctic aerosols. The ratios of fluorescence intensity of protein-like peak to humic-like peak generally increased from dark winter to early summer, indicating an enhanced contribution of protein-like organics from the ocean to Arctic aerosols after the polar sunrise. Such a seasonal pattern is in agreement with an increase of stable carbon isotope ratios of total carbon (δCTC) from -26.8‰ to -22.5‰. Our results suggest that Arctic aerosols are derived from a combination of the long-range transport of terrestrial organics and local sea-to-air emission of marine organics, with an estimated contribution from the latter of 8.7-77% (mean 45%).

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