scholarly journals Carbonaceous components, levoglucosan and inorganic ions in tropical aerosols from Tanzania, East Africa: implication for biomass burning contribution to organic aerosols

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±6.4 μg m−3 and 47±8.2 μg m−3 in wet season, and 39.1±9.8 μg m−3 and 61.4±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.

2013 ◽  
Vol 13 (20) ◽  
pp. 10325-10338 ◽  
Author(s):  
S. L. Mkoma ◽  
K. Kawamura ◽  
P. Q. Fu

Abstract. Atmospheric aerosol samples of PM2.5 and PM10 were collected at a rural site in Tanzania, East Africa, in 2011 during wet and dry seasons and were analysed for carbonaceous components, levoglucosan, mannosan and water-soluble inorganic ions. The contributions of biomass/biofuel burning to the organic carbon (OC) and particulate matter (PM) mass were estimated to be 46–52% and 87–13%, respectively. The mean mass concentrations of PM2.5 and PM10 were 28 ± 6 μg m−3 and 47 ± 8 μg m−3 in wet season, and 39 ± 10 μg m−3 and 61 ± 19 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, 86 to 89% of TC in PM2.5 and 87 to 90% of TC in PM10 was OC, of which 67–72% and 63% was found to be water-soluble organic carbon (WSOC) in PM2.5 and PM10, respectively. We found that concentrations of levoglucosan and mannosan (specific organic tracers of pyrolysis of cellulose) well correlated with non-sea-salt potassium (nss-K+) (r2 = 0.56–0.75), OC (r2 = 0.75–0.96) and WSOC (r2 = 0.52–0.78). The K+ / OC ratios varied from 0.06 to 0.36 in PM2.5 and from 0.03 to 0.36 in PM10 with slightly higher ratios in dry season. Mean percent ratios of levoglucosan and mannosan to OC were found to be 3–4% for PM2.5 and PM10 in both seasons. We found lower levoglucosan / K+ ratios and higher K+ / EC (elemental carbon) ratios in the biomass-burning aerosols from Tanzania than those reported from other regions. This feature is consistent with the high levels of potassium reported in the soils of Morogoro, Tanzania, suggesting an importance of direct emission of potassium by soil resuspension although K+ is present mostly in fine particles. It is also likely that biomass burning of vegetation of Tanzania emits high levels of potassium that may be enriched in plant tissues. The present study demonstrates that emissions from mixed biomass- and biofuel-burning activities largely influence the air quality in Tanzania.


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 ± 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 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 ± 0.3‰) in summer than in winter (−25.9 ± 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.


2015 ◽  
Vol 15 (3) ◽  
pp. 1299-1312 ◽  
Author(s):  
Y.-L. Zhang ◽  
R.-J. Huang ◽  
I. El Haddad ◽  
K.-F. Ho ◽  
J.-J. Cao ◽  
...  

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.


2009 ◽  
Vol 9 (5) ◽  
pp. 1521-1535 ◽  
Author(s):  
S. Szidat ◽  
M. Ruff ◽  
N. Perron ◽  
L. Wacker ◽  
H.-A. Synal ◽  
...  

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.


2004 ◽  
Vol 4 (4) ◽  
pp. 967-987 ◽  
Author(s):  
I. Trebs ◽  
F. X. Meixner ◽  
J. Slanina ◽  
R. Otjes ◽  
P. Jongejan ◽  
...  

Abstract. We measured the mixing ratios of ammonia (NH3), nitric acid (HNO3), nitrous acid (HONO), hydrochloric acid (HCl), sulfur dioxide (SO2 and the corresponding water-soluble inorganic aerosol species, ammonium (NH4+), nitrate (NO3-), nitrite (NO2-), chloride (Cl- and sulfate (SO42-), and their diel and seasonal variations at a pasture site in the Amazon Basin (Rondônia, Brazil). This study was conducted within the framework of LBA-SMOCC (Large Scale Biosphere Atmosphere Experiment in Amazonia - Smoke Aerosols, Clouds, Rainfall and Climate: Aerosols from Biomass Burning Perturb Global and Regional Climate). Sampling was performed from 12 September to 14 November 2002, extending from the dry season (extensive biomass burning activity), through the transition period to the wet season (background conditions). Measurements were made continuously using a wet-annular denuder (WAD) in combination with a Steam-Jet Aerosol Collector (SJAC) followed by suitable on-line analysis. A detailed description and verification of the inlet system for simultaneous sampling of soluble gases and aerosol compounds is presented. Overall measurement uncertainties of the ambient mixing ratios usually remained below 15%. The limit of detection (LOD) was determined for each single data point measured during the field experiment. Median LOD values (3σ-definition) were ≤0.015ppb for acidic trace gases and aerosol anions and ≤0.118ppb for NH3 and aerosol NH4+. Mixing ratios of acidic trace gases remained below 1ppb throughout the measurement period, while NH3 levels were an order of magnitude higher. Accordingly, mixing ratios of NH4+ exceeded those of other inorganic aerosol contributors by a factor of 4 to 10. During the wet season, mixing ratios decreased by nearly a factor of 3 for all compounds compared to those observed when intensive biomass burning took place. Additionally, N-containing gas and aerosol species featured pronounced diel variations. This is attributed to strong relative humidity and temperature variations between day and night as well as to changing photochemistry and stability conditions of the planetary boundary layer. HONO exhibited a characteristic diel cycle with high mixing ratios at nighttime and was not completely depleted by photolysis during daylight hours.


2021 ◽  
Vol 21 (15) ◽  
pp. 11815-11828
Author(s):  
Nana Suto ◽  
Hiroto Kawashima

Abstract. The sources and seasonal trends of water-soluble organic carbon (WSOC) in carbonaceous aerosols are of significant interest. From July 2017 to July 2019, we collected samples of PM2.5 (particulate matter, aerodynamic diameter<2.5 µm) from one suburban and one rural site in Japan. The average δ13CWSOC was -25.2±1.1 ‰ and -24.6±2.4 ‰ at the suburban site and rural site, respectively. At the suburban site, the δ13CWSOC was consistent with the δ13C of burned C3 plants, and a high correlation was found between WSOC concentrations and non-sea-salt potassium concentrations; these results suggest that the main source of WSOC at this site was biomass burning of rice straw. At the rural site, the average δ13CWSOC was significantly heavier from autumn to spring (-23.9±2.1 ‰) than in summer (-27.4±0.7 ‰) (p<0.01). The δ13CWSOC from autumn to spring was consistent with that of biomass burning of rice straw, whereas that in summer was considered to reflect mainly the formation of secondary organic aerosols from biogenic volatile organic compounds (VOCs). The heaviest δ13CWSOC (-21.3±1.9 ‰) was observed from February to April 2019, which may be explained by long-range transport of C4 plant burning such as corn from overseas. Thus, the present study indicates that δ13CWSOC is potentially useful for elucidating the sources and atmospheric processes that contribute to seasonal variations of WSOC concentration.


2016 ◽  
Author(s):  
Ulrike Dusek ◽  
Regina Hitzenberger ◽  
Anne Kasper-Giebl ◽  
Magdalena Kistler ◽  
Harro A. J. Meijer ◽  
...  

Abstract. We measured the radioactive carbon isotope 14C (radiocarbon) in various fractions of the carbonaceous aerosol sampled between February 2011 and March 2012 at the Cesar observatory in the Netherlands. Based on the radiocarbon content in total carbon (TC), organic carbon (OC), water insoluble organic carbon (WIOC), and elemental carbon (EC), we estimated the contribution of major sources to the carbonaceous aerosol. The main source categories were fossil fuel combustion, biomass burning and other contemporary carbon, which is mainly biogenic secondary organic aerosol material (SOA). A clear seasonal variation is seen in EC from biomass burning (ECBB), with lowest values in summer and highest values in winter, but ECBB is a minor fraction of EC in all seasons. WIOC from contemporary sources is highly correlated with ECBB, indicating that biomass burning is the dominant source of contemporary WIOC. This suggests that most biogenic SOA is water-soluble and that water insoluble carbon stems mainly from primary sources. Seasonal variations in other carbon fractions are less clear and hardly distinguishable from variations related to air mass history. Air masses originating from the ocean sector presumably contain little carbonaceous aerosol from outside the Netherlands, and during these conditions measured carbon concentrations reflect regional sources. In these situations absolute TC concentrations are usually rather low, around 1.5 μg m−3 and ECBB is always very low (~ 0.05 μg m−3), even in winter, indicating that biomass burning is not a strong source of carbonaceous aerosol in the Netherlands. In continental air masses, which usually arrive from the East or South and have spent several days over land, TC concentrations are on average by a factor of 3 higher. ECBB increases more strongly than TC to 0.2 μg m−3. Fossil EC and fossil WIOC, which are indicative of primary emissions, show a more moderate increase by a factor of 2.5 on average. An interesting case is fossil water soluble organic carbon (WSOC, calculated as OC-WIOC), which can be regarded as a proxy for SOA from fossil precursors. Fossil WSOC has low concentrations when regional sources are sampled and increases by more than a factor of 5 in continental air masses. A longer residence time of air masses over land seems to result in increased SOA concentrations from fossil origin.


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