scholarly journals Size distributions of dicarboxylic acids, ketoacids, α-dicarbonyls, sugars, WSOC, OC, EC and inorganic ions in atmospheric particles over Northern Japan: implication for long-range transport of Siberian biomass burning and East Asian polluted aerosols

2010 ◽  
Vol 10 (3) ◽  
pp. 6713-6754 ◽  
Author(s):  
S. Agarwal ◽  
S. G. Aggarwal ◽  
K. Okuzawa ◽  
K. Kawamura

Abstract. To better understand the size-segregated chemical composition of aged organic aerosols in the western Pacific rim, day- and night-time aerosol samples were collected in Sapporo, Japan during summer 2005 using Andersen impactor sampler with 5 size bins: <1.1, 1.1–2.0, 2.0–3.3, 3.3–7.0, >7.0 μm. Samples were analyzed for the molecular compositions of dicarboxylic acids, ketoacids, α-dicarbonyls, and sugars, together with water-soluble organic carbon (WSOC), organic carbon (OC), elemental carbon (EC) and inorganic ions. Based on the analyses of backward trajectory and chemical tracers, we found that during campaign, the air masses were arrived from Siberia (biomass burning source region) on 8–9 August, China (anthropogenic source region) on 9–10 August and from the East China Sea/Sea of Japan (a mixed source receptor region) on 10–11 August. Most of the diacids, ketoacids, dicarbonyls, levoglucosan, WSOC, and inorganic ions, i.e., SO42−, NH42+ and K+ were enriched in fine particles (PM1.1) whereas Ca2+, Mg2+ and Cl− peaked in coarse sizes (>1.1 μm). Interestingly, OC, most sugar compounds and NO4

2010 ◽  
Vol 10 (13) ◽  
pp. 5839-5858 ◽  
Author(s):  
S. Agarwal ◽  
S. G. Aggarwal ◽  
K. Okuzawa ◽  
K. Kawamura

Abstract. To better understand the size-segregated chemical composition of aged organic aerosols in the western North Pacific rim, day- and night-time aerosol samples were collected in Sapporo, Japan during summer 2005 using an Andersen impactor sampler with 5 size bins: Dp<1.1, 1.1–2.0, 2.0–3.3, 3.3–7.0, >7.0 μm. Samples were analyzed for the molecular composition of dicarboxylic acids, ketoacids, α-dicarbonyls, and sugars, together with water-soluble organic carbon (WSOC), organic carbon (OC), elemental carbon (EC) and inorganic ions. Based on the analyses of backward trajectories and chemical tracers, we found that during the campaign, air masses arrived from Siberia (a biomass burning source region) on 8–9 August, from China (an anthropogenic source region) on 9–10 August, and from the East China Sea/Sea of Japan (a mixed source receptor region) on 10–11 August. Most of the diacids, ketoacids, dicarbonyls, levoglucosan, WSOC, and inorganic ions (i.e., SO42−, NH4+ and K+) were enriched in fine particles (PM1.1) whereas Ca2+, Mg2+ and Cl− peaked in coarse sizes (>1.1 μm). Interestingly, OC, most sugar compounds and NO3− showed bimodal distributions in fine and coarse modes. In PM1.1, diacids in biomass burning-influenced aerosols transported from Siberia (mean: 252 ng m−3) were more abundant than those in the aerosols originating from China (209 ng m−3) and ocean (142 ng m−3), whereas SO42− concentrations were highest in the aerosols from China (mean: 3970 ng m−3) followed by marine- (2950 ng m−3) and biomass burning-influenced (1980 ng m−3) aerosols. Higher loadings of WSOC (2430 ng m−3) and OC (4360 ng m−3) were found in the fine mode, where biomass-burning products such as levoglucosan are abundant. This paper presents a case study of long-range transported aerosols illustrating that biomass burning episodes in the Siberian region have a significant influence on the chemical composition of carbonaceous aerosols in the western North Pacific rim.


2012 ◽  
Vol 12 (11) ◽  
pp. 28661-28703 ◽  
Author(s):  
S. L. Mkoma ◽  
K. Kawamura ◽  
P. Fu

Abstract. Atmospheric aerosol samples of PM2.5 and PM10 were collected at a rural site in Tanzania in 2011 during wet and dry seasons and they were analysed for carbonaceous components, levoglucosan and water-soluble inorganic ions. The mean mass concentrations of PM2.5 and PM10 were 28.2&amp;pm;6.4 μg m−3 and 47&amp;pm;8.2 μg m−3 in wet season, and 39.1&amp;pm;9.8 μg m−3 and 61.4&amp;pm;19.2 μg m−3 in dry season, respectively. Total carbon (TC) accounted for 16–19% of the PM2.5 mass and 13–15% of the PM10 mass. On average, 85.9 to 88.7% of TC in PM2.5 and 87.2 to 90.1% in PM10 was organic carbon (OC), of which 67–72% and 63% was found to be water-soluble organic carbon (WSOC) in PM2.5 and PM10, respectively. Water-soluble potassium (K+) and sulphate (SO42−) in PM2.5 and, sodium (Na+) and SO42− in PM10 were the dominant ionic species. We found, that concentrations of biomass burning tracers (levoglucosan and mannosan) well correlated with non-sea-salt-K+, WSOC and OC in the aerosols from Tanzania, East Africa. Mean contributions of levoglucosan to OC ranged between 3.9–4.2% for PM2.5 and 3.5–3.8% for PM10. This study demonstrates that emissions from biomass- and biofuel-burning activities followed by atmospheric photochemical processes mainly control the air quality in Tanzania.


2021 ◽  
Author(s):  
Connor Stahl ◽  
Ewan Crosbie ◽  
Paola Angela Bañaga ◽  
Grace Betito ◽  
Rachel A. Braun ◽  
...  

Abstract. This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA’s Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC levels and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an Axial Cyclone Cloud water Collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonate (MSA), and dimethylamine (DMA). TOC values range between 0.018–13.660 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on carbon mass basis) an average of 30.0 % to TOC in the study region, and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows: acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, thus highlighting the complex nature of organics in the study region; samples collected in biomass burning plumes have up to 95.6 % of unaccounted TOC mass based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (~75 %) and are about four times in greater abundance than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl−) tracers exhibit strong correlations with speciated organics, thus supporting how coarse aerosol surfaces interact with these water-soluble organics.


2021 ◽  
Vol 21 (9) ◽  
pp. 7321-7341
Author(s):  
Jingsha Xu ◽  
Di Liu ◽  
Xuefang Wu ◽  
Tuan V. Vu ◽  
Yanli Zhang ◽  
...  

Abstract. Fine particles were sampled from 9 November to 11 December 2016 and 22 May to 24 June 2017 as part of the Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-China) field campaigns in urban Beijing, China. Inorganic ions, trace elements, organic carbon (OC), elemental carbon (EC), and organic compounds, including biomarkers, hopanes, polycyclic aromatic hydrocarbons (PAHs), n-alkanes, and fatty acids, were determined for source apportionment in this study. Carbonaceous components contributed on average 47.2 % and 35.2 % of total reconstructed PM2.5 during the winter and summer campaigns, respectively. Secondary inorganic ions (sulfate, nitrate, ammonium; SNA) accounted for 35.0 % and 45.2 % of total PM2.5 in winter and summer. Other components including inorganic ions (K+, Na+, Cl−), geological minerals, and trace metals only contributed 13.2 % and 12.4 % of PM2.5 during the winter and summer campaigns. Fine OC was explained by seven primary sources (industrial and residential coal burning, biomass burning, gasoline and diesel vehicles, cooking, and vegetative detritus) based on a chemical mass balance (CMB) receptor model. It explained an average of 75.7 % and 56.1 % of fine OC in winter and summer, respectively. Other (unexplained) OC was compared with the secondary OC (SOC) estimated by the EC-tracer method, with correlation coefficients (R2) of 0.58 and 0.73 and slopes of 1.16 and 0.80 in winter and summer, respectively. This suggests that the unexplained OC by the CMB model was mostly associated with SOC. PM2.5 apportioned by the CMB model showed that the SNA and secondary organic matter were the two highest contributors to PM2.5. After these, coal combustion and biomass burning were also significant sources of PM2.5 in winter. The CMB results were also compared with results from the positive matrix factorization (PMF) analysis of co-located aerosol mass spectrometer (AMS) data. The CMB model was found to resolve more primary organic aerosol (OA) sources than AMS-PMF, but the latter could apportion secondary OA sources. The AMS-PMF results for major components, such as coal combustion OC and oxidized OC, correlated well with the results from the CMB model. However, discrepancies and poor agreements were found for other OC sources, such as biomass burning and cooking, some of which were not identified in AMS-PMF factors.


2021 ◽  
Vol 21 (18) ◽  
pp. 14109-14129
Author(s):  
Connor Stahl ◽  
Ewan Crosbie ◽  
Paola Angela Bañaga ◽  
Grace Betito ◽  
Rachel A. Braun ◽  
...  

Abstract. This work focuses on total organic carbon (TOC) and contributing species in cloud water over Southeast Asia using a rare airborne dataset collected during NASA's Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP2Ex), in which a wide variety of maritime clouds were studied, including cumulus congestus, altocumulus, altostratus, and cumulus. Knowledge of TOC masses and their contributing species is needed for improved modeling of cloud processing of organics and to understand how aerosols and gases impact and are impacted by clouds. This work relies on 159 samples collected with an axial cyclone cloud-water collector at altitudes of 0.2–6.8 km that had sufficient volume for both TOC and speciated organic composition analysis. Species included monocarboxylic acids (glycolate, acetate, formate, and pyruvate), dicarboxylic acids (glutarate, adipate, succinate, maleate, and oxalate), methanesulfonic acid (MSA), and dimethylamine (DMA). TOC values range between 0.018 and 13.66 ppm C with a mean of 0.902 ppm C. The highest TOC values are observed below 2 km with a general reduction aloft. An exception is samples impacted by biomass burning for which TOC remains enhanced at altitudes as high as 6.5 km (7.048 ppm C). Estimated total organic matter derived from TOC contributes a mean of 30.7 % to total measured mass (inorganics + organics). Speciated organics contribute (on a carbon mass basis) an average of 30.0 % to TOC in the study region and account for an average of 10.3 % to total measured mass. The order of the average contribution of species to TOC, in decreasing contribution of carbon mass, is as follows (±1 standard deviation): acetate (14.7 ± 20.5 %), formate (5.4 ± 9.3 %), oxalate (2.8 ± 4.3 %), DMA (1.7 ± 6.3 %), succinate (1.6 ± 2.4 %), pyruvate (1.3 ± 4.5 %), glycolate (1.3 ± 3.7 %), adipate (1.0 ± 3.6 %), MSA (0.1 ± 0.1 %), glutarate (0.1 ± 0.2 %), and maleate (< 0.1 ± 0.1 %). Approximately 70 % of TOC remains unaccounted for, highlighting the complex nature of organics in the study region; in samples collected in biomass burning plumes, up to 95.6 % of TOC mass is unaccounted for based on the species detected. Consistent with other regions, monocarboxylic acids dominate the speciated organic mass (∼ 75 %) and are about 4 times more abundant than dicarboxylic acids. Samples are categorized into four cases based on back-trajectory history, revealing source-independent similarity between the bulk contributions of monocarboxylic and dicarboxylic acids to TOC (16.03 %–23.66 % and 3.70 %–8.75 %, respectively). Furthermore, acetate, formate, succinate, glutarate, pyruvate, oxalate, and MSA are especially enhanced during biomass burning periods, which is attributed to peat emissions transported from Sumatra and Borneo. Lastly, dust (Ca2+) and sea salt (Na+/Cl-) tracers exhibit strong correlations with speciated organics, supporting how coarse aerosol surfaces interact with these water-soluble organics.


2013 ◽  
Vol 13 (9) ◽  
pp. 4667-4680 ◽  
Author(s):  
S. G. Aggarwal ◽  
K. Kawamura ◽  
G. S. Umarji ◽  
E. Tachibana ◽  
R. S. Patil ◽  
...  

Abstract. To better understand the sources of PM10 samples in Mumbai, India, aerosol chemical composition, i.e., total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4‰, also suggests that biofuel/biomass burning is a predominate source in both the summer and winter seasons. Aerosol mass concentrations of major species increased 3–4 times in winter compared to summer, indicating enhanced emission from these sources in the winter season. Photochemical production tracers, C2 diacid and nssSO42−, do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for daytime (0.37 &amp;pm; 0.06 (0.28 &amp;pm; 0.04)) and nighttime (0.38 &amp;pm; 0.07 (0.28 &amp;pm; 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant and the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from −27.0 to −25.4‰, with slightly lower average (−26.5 &amp;pm; 0.3‰) in summer than in winter (−25.9 &amp;pm; 0.3‰). Positive correlation between WSOC/TC ratios and δ13C values suggested that the relative increment in 13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests that in winter, the tropical aerosols are more aged due to longer residence time in the atmosphere than in summer aerosols. However, these conclusions are based on the analysis of a limited number of samples (n=25) and more information on this topic may be needed from other similar coastal sites in future.


2012 ◽  
Vol 12 (8) ◽  
pp. 20593-20630 ◽  
Author(s):  
S. G. Aggarwal ◽  
K. Kawamura ◽  
G. S. Umarji ◽  
E. Tachibana ◽  
R. S. Patil ◽  
...  

Abstract. To better understand the sources of PM10 samples from Mumbai, India, aerosol chemical compositions, i.e. total carbon (TC), organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and inorganic ions were studied together with specific markers such as methanesulfonate (MSA), oxalic acid (C2), azelaic acid (C9), and levoglucosan. The results revealed that biofuel/biomass burning and fossil fuel combustion are the major sources of the Mumbai aerosols. Nitrogen-isotopic (δ15N) composition of aerosol total nitrogen, which ranged from 18.1 to 25.4‰, also suggest that biofuel/biomass burning is the dominant source in both summer and winter seasons. Aerosol mass concentrations of major species increased 3–4 times in winter compared to summer, indicating an enhanced emission from these sources in winter season. Photochemical production tracers, C2 diacid and nssSO42− do not show diurnal changes. Concentrations of C2 diacid and WSOC show a strong correlation (r2 = 0.95). In addition, WSOC to OC (or TC) ratios remain almost constant for day- (0.37 ± 0.06 (0.28 ± 0.04)) and nighttime (0.38 ± 0.07 (0.28 ± 0.06)), suggesting that mixing of fresh secondary organic aerosols is not significant rather the Mumbai aerosols are photochemically well processed. Concentrations of MSA and C9 diacid present a positive correlation (r2 = 0.75), indicating a marine influence on Mumbai aerosols in addition to local/regional influence. Backward air mass trajectory analyses further suggested that the Mumbai aerosols are largely influenced by long-range continental and regional transport. Stable C-isotopic ratios (δ13C) of TC ranged from −27.0 to −25.4‰ with slightly lower average (−26.5 ± 0.3‰) in summer than in winter (−25.9 ± 0.3‰). Positive correlation between WSOC/TC ratios and δ13C values suggested that the increment in δ13C of wintertime TC may be caused by prolonged photochemical processing of organic aerosols in this season. This study suggests that in winter, the tropical aerosols are more aged due to longer residence time in the atmosphere than in the summer aerosols.


2018 ◽  
Author(s):  
Xinghua Li ◽  
Junzan Han ◽  
Philip K. Hopke ◽  
Jingnan Hu ◽  
Qi Shu ◽  
...  

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.


Author(s):  
Xing Li ◽  
Shanshan Li ◽  
Qiulin Xiong ◽  
Xingchuan Yang ◽  
Mengxi Qi ◽  
...  

Beijing, which is the capital of China, suffers from severe Fine Particles (PM2.5) pollution during the heating season. In order to take measures to control the PM2.5 pollution and improve the atmospheric environmental quality, daily PM2.5 samples were collected at an urban site from 15 November to 31 December 2016, characteristics of PM2.5 chemical compositions and their effect on atmospheric visibility were analyzed. It was found that the daily average mass concentrations of PM2.5 ranged from 7.64 to 383.00 μg m−3, with an average concentration of 114.17 μg m−3. On average, the Organic Carbon (OC) and Elemental Carbon (EC) contributed 21.39% and 5.21% to PM2.5, respectively. Secondary inorganic ions (SNA: SO42− + NO3− + NH4+) dominated the Water-Soluble Inorganic Ions (WSIIs) and they accounted for 47.09% of PM2.5. The mass concentrations of NH4+, NO3− and SO42− during the highly polluted period were 8.08, 8.88 and 6.85 times greater, respectively, than during the clean period, which contributed most to the serious PM2.5 pollution through the secondary transformation of NO2, SO2 and NH3. During the highly polluted period, NH4NO3 contributed most to the reconstruction extinction coefficient (b′ext), accounting for 35.7%, followed by (NH4)2SO4 (34.44%) and Organic Matter (OM: 15.24%). The acidity of PM2.5 in Beijing was weakly acid. Acidity of PM2.5 and relatively high humidity could aggravate PM2.5 pollution and visibility impairment by promoting the generation of secondary aerosol. Local motor vehicles contributed the most to NO3−, OC, and visibility impairment in urban Beijing. Other sources of pollution in the area surrounding urban Beijing, including coal burning, agricultural sources, and industrial sources in the Hebei, Shandong, and Henan provinces, released large amounts of SO2, NH3, and NO2. These, which were transformed into SO42−, NH4+, and NO3− during the transmission process, respectively, and had a great impact on atmospheric visibility impairment.


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