Extreme Molecular Complexity Resulting in a Continuum of Carbonaceous Species in Biomass Burning Tar Balls from Wildfire Smoke

2021 ◽  
Author(s):  
Matthew A. Brege ◽  
Swarup China ◽  
Simeon Schum ◽  
Alla Zelenyuk ◽  
Lynn R. Mazzoleni
Keyword(s):  
Biomass Burning ◽  
Carbonaceous Species ◽  
Wildfire Smoke ◽  
Tar Balls ◽  
Molecular Complexity

scholarly journals Atmospheric tar balls: aged primary droplets from biomass burning?

2014 ◽  
Vol 14 (13) ◽  
pp. 6669-6675 ◽  
Author(s):  
A. Tóth ◽  
A. Hoffer ◽  
I. Nyirő-Kósa ◽  
M. Pósfai ◽  
A. Gelencsér
Keyword(s):  
Biomass Burning ◽  
Atmospheric Chemistry ◽  
Climate Forcing ◽  
Specific Subset ◽  
Transmission Electron ◽  
Direct Emission ◽  
Dry Distillation ◽  
Tar Balls ◽  
Special Morphology ◽  
Heat Transformation

Abstract. Atmospheric tar balls are particles of special morphology and composition that are fairly abundant in the plumes of biomass smoke. These particles form a specific subset of brown carbon (BrC) which has been shown to play a significant role in atmospheric shortwave absorption and, by extension, climate forcing. Here we suggest that tar balls are produced by the direct emission of liquid tar droplets followed by heat transformation upon biomass burning. For the first time in atmospheric chemistry we generated tar-ball particles from liquid tar obtained previously by dry distillation of wood in an all-glass apparatus in the laboratory with the total exclusion of flame processes. The particles were perfectly spherical with a mean optical diameter of 300 nm, refractory, externally mixed, and homogeneous in the contrast of the transmission electron microscopy (TEM) images. They lacked any graphene-like microstructure and exhibited a mean carbon-to-oxygen ratio of 10. All of the observed characteristics of laboratory-generated particles were very similar to those reported for atmospheric tar-ball particles in the literature, strongly supporting our hypothesis regarding the formation mechanism of atmospheric tar-ball particles.

scholarly journals Formation and evolution of Tar Balls from Northwestern US wildfires

2018 ◽  
Author(s):  
Arthur J. Sedlacek III ◽  
Peter R. Buseck ◽  
Kouji Adachi ◽  
Timothy B. Onasch ◽  
Stephen R. Springston ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Forest Fires ◽  
Wildland Fire ◽  
Carbonaceous Particle ◽  
Carbonaceous Particles ◽  
Tar Balls ◽  
Mass Fractions ◽  
Atmospheric Observations ◽  
Formation And Evolution

Abstract. Biomass burning is a major source of light-absorbing black and brown carbonaceous particles. Brown carbon is a poorly characterized mixture that includes tar balls (TBs), a type of carbonaceous particle apparently unique to biomass burning. Here we describe the first atmospheric observations of the formation and evolution of TBs from forest fires. Aerosol particles were collected on TEM grids during aircraft transects at various downwind distances from the Colockum Tarp wildland fire. TB mass fractions, derived from TEM and in-situ measurements, increased from

scholarly journals Airborne particles in the Brazilian city of São Paulo: One-year investigation for the chemical composition and source apportionment

2017 ◽  
Author(s):  
Guilherme Martins Pereira ◽  
Kimmo Teinilä ◽  
Danilo Custódio ◽  
Aldenor Gomes Santos ◽  
Huang Xian ◽  
...  
Keyword(s):  
Air Pollution ◽  
Particulate Matter ◽  
Source Apportionment ◽  
Health Risks ◽  
Biomass Burning ◽  
Sao Paulo ◽  
Airborne Particles ◽  
São Paulo ◽  
Carbonaceous Species ◽  
Local Sources

Abstract. São Paulo in Brazil has relatively relaxed regulations for ambient air pollution standards and often experiences high air pollution levels due to emissions of airborne particles from local sources and long-range transport of biomass burning-impacted air masses. In order to evaluate the sources of particulate air pollution (PM) and related health risks, a year-round sampling was performed for PM2.5 (≤ 2.5 μm) and PM10 (≤ 10 μm) in 2014 through intensive (every day sampling in wintertime) and extensive campaigns (once a week for the whole year) with 24 h of sampling. This year was characterized to have lower average precipitation comparing to meteorological data, and high pollution episodes were observed all year round, with a significant increase of pollution level in the intensive campaign, which was performed during wintertime. Different chemical constituents, such as carbonaceous species, polycyclic aromatic hydrocarbons (PAHs) and derivatives, water-soluble ions and biomass burning tracers were identified in order to evaluate health risks and to apportion sources. The species such as PAHs, inorganic and organic ions and monosaccharides were determined by chromatographic techniques and carbonaceous species by thermal-optical analysis. The associated risks to particulate matter exposure based on PAH concentrations were also assessed, along with indexes such as the benzo[a]pyrene equivalent (BaPE) and lung cancer risk (LCR). High BaPE and LCR were observed in most of the samples, rising to critical values in the wintertime. Also, biomass burning tracers and PAHs were higher in this season, while secondarily formed ions presented low variation throughout the year. Meanwhile, vehicular tracer species were also higher in the intensive campaign suggesting the influence of lower dispersion conditions in that period. Source apportionment was done by Positive Matrix Factorization (PMF), which indicated five different factors: road dust, industrial emissions, vehicular exhaust, biomass burning and secondary processes. The results highlighted the contribution of vehicular emissions and the significant input from biomass combustion in wintertime, suggesting that most of the particulate matter is due to local sources, besides the influence of pre-harvest sugarcane burning.

scholarly journals Wildfire smoke in the Siberian Arctic in summer: source characterization and plume evolution from airborne measurements

2009 ◽  
Vol 9 (23) ◽  
pp. 9315-9327 ◽  
Author(s):  
J.-D. Paris ◽  
A. Stohl ◽  
P. Nédélec ◽  
M. Yu. Arshinov ◽  
M. V. Panchenko ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Forest Fires ◽  
Emission Factor ◽  
Fine Particles ◽  
Lagrangian Model ◽  
Mixing Ratio ◽  
Source Characterization ◽  
Airborne Measurements ◽  
Wildfire Smoke ◽  
Ultra Fine Particles

Abstract. We present airborne measurements of carbon dioxide (CO2), carbon monoxide (CO), ozone (O3), equivalent black carbon (EBC) and ultra fine particles over North-Eastern Siberia in July 2008 performed during the YAK-AEROSIB/POLARCAT experiment. During a "golden day" (11 July 2008) a number of biomass burning plumes were encountered with CO mixing ratio enhancements of up to 500 ppb relative to a background of 90 ppb. Number concentrations of aerosols in the size range 3.5–200 nm peaked at 4000 cm−3 and the EBC content reached 1.4 μg m−3. These high concentrations were caused by forest fires in the vicinity of the landing airport in Yakutsk where measurements in fresh smoke could be made during the descent. We estimate a combustion efficiency of 90 ± 3% based on CO and CO2 measurements and a CO emission factor of 65.5 ± 10.8 g CO per kilogram of dry matter burned. This suggests a potential increase in the average northern hemispheric CO mixing ratio of 3.0–7.2 ppb per million hectares of Siberian forest burned. For BC, we estimate an emission factor of 0.52 ± 0.07 g BC kg−1, comparable to values reported in the literature. The emission ratio of ultra-fine particles (3.5–200 nm) was 26 cm−3 (ppb CO)−1, consistent with other airborne studies. The transport of identified biomass burning plumes was investigated using the FLEXPART Lagrangian model. Based on sampling of wildfire plumes from the same source but with different atmospheric ages derived from FLEXPART, we estimate that the e-folding lifetimes of EBC and ultra fine particles (between 3.5 and 200 nm in size) against removal and growth processes are 5.1 and 5.5 days respectively, supporting lifetime estimates used in various modelling studies.

scholarly journals Atmospheric tar balls: aged primary droplets from biomass burning?

2013 ◽  
Vol 13 (12) ◽  
pp. 33089-33104 ◽  
Author(s):  
A. Tóth ◽  
A. Hoffer ◽  
I. Nyirő-Kósa ◽  
M. Pósfai ◽  
A. Gelencsér
Keyword(s):  
Biomass Burning ◽  
Climate Forcing ◽  
Size Distributions ◽  
Pyrolysis Products ◽  
Biomass Smoke ◽  
Specific Subset ◽  
Dry Distillation ◽  
Smoke Plumes ◽  
Tar Balls ◽  
Special Morphology

Abstract. Atmospheric tar balls are particles of special morphology and composition that are abundant in the plumes of biomass smoke. These particles form a specific subset of brown carbon (BrC) which has been shown to play a significant role in atmospheric shortwave absorption and thus climate forcing. Formerly tar balls were hypothesized to be formed in secondary processes in the atmosphere from lignin pyrolysis products. Based on their typical size distributions, morphology, chemical characteristics and other features we now suggest that tar balls are initially produced by the emission of primary tar droplets upon biomass burning. To verify our hypothesis tar balls were produced under laboratory conditions with the total exclusion of flame processes. An all-glass apparatus was designed and tar ball particles were generated from liquid tar obtained previously by dry distillation of wood. The size range, morphology and the chemical composition of the laboratory-generated tar ball particles were similar to those observed in biomass smoke plumes or elsewhere in the atmosphere. Based on our results and the chemical and physical characteristics of tar we suggest that tar balls can be formed by the chemical transformation of emitted primary tar droplets.

scholarly journals Wildfire smoke in the Siberian Arctic in summer: source characterization and plume evolution from airborne measurements

2009 ◽  
Vol 9 (5) ◽  
pp. 18201-18233 ◽  
Author(s):  
J.-D. Paris ◽  
A. Stohl ◽  
P. Nédélec ◽  
M. Yu. Arshinov ◽  
M. V. Panchenko ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Forest Fires ◽  
Emission Factor ◽  
Fine Particles ◽  
Lagrangian Model ◽  
Source Characterization ◽  
Airborne Measurements ◽  
Wildfire Smoke ◽  
Co Concentration ◽  
Ultra Fine Particles

Abstract. We present airborne measurements of carbon dioxide (CO2), carbon monoxide (CO), ozone (O3), equivalent black carbon (EBC) and ultra fine particles over North-Eastern Siberia in July 2008 performed during the YAK-AEROSIB/POLARCAT experiment. During a "golden day" (11 July 2008) a number of biomass burning plumes were encountered with CO concentration enhancements of up to 500 ppb relative to a background of 90 ppb. Number concentrations of aerosols in the size range 3.5–200 nm peaked at 4000 cm−3 and the EBC content reached 1.4 μg m−3. These high concentrations were caused by forest fires in the vicinity of the landing airport in Yakutsk where during the descent measurements in fresh smoke could be made. We estimate a combustion efficiency of 90±3% based on CO and CO2 measurements. The emission factor of CO emitted was 59.6±15.2 g CO per kilogram of dry matter burned, suggesting an increase in the average northern hemispheric CO concentration of 3.0–7.2 ppb per million hectares of Siberian forest burned. For BC, we estimate an emission factor of 0.52±0.07 g BC kg−1, comparable to values reported in the literature. The emission ratio of ultra-fine particles (3.5–200 nm) was 26 cm−3 (ppb CO)−1, consistent with other airborne studies. The transport of identified biomass burning plumes was investigated using the FLEXPART Lagrangian model. Based on sampling of wildfire plumes from the same source but with different atmospheric ages derived from FLEXPART, we estimate that the e-folding lifetimes of EBC and ultra fine particles (between 3.5 and 200 nm in size) against removal and growth processes are 5.1 and 5.5 days, respectively, supporting lifetimes estimates used in various modelling studies.

scholarly journals Exploring wintertime regional haze in northeast China: role of coal and biomass burning

2020 ◽  
Vol 20 (9) ◽  
pp. 5355-5372 ◽  
Author(s):  
Jian Zhang ◽  
Lei Liu ◽  
Liang Xu ◽  
Qiuhan Lin ◽  
Hujia Zhao ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Northeast China ◽  
Aerosol Particles ◽  
Urban Site ◽  
Particle Analysis ◽  
Aerosol Formation ◽  
Tar Balls ◽  
Mountain Site ◽  
Regional Haze ◽  
Haze Formation

Abstract. As one of the intense anthropogenic emission regions across the relatively high-latitude (>40∘ N) areas on Earth, northeast China faces the serious problem of regional haze during the heating period of the year. Aerosols in polluted haze in northeast China are poorly understood compared with the haze in other regions of China such as the North China Plain. Here, we integrated bulk chemical measurements with single-particle analysis from transmission electron microscopy (TEM), nanoscale secondary ion mass spectrometry (NanoSIMS), and atomic force microscopy (AFM) to obtain morphology, size, composition, aging process, and sources of aerosol particles collected during two contrasting regional haze events (Haze-I and Haze-II) at an urban site and a mountain site in northeast China and further investigated the causes of regional haze formation. Haze-I evolved from moderate (average PM2.5: 76–108 µg m−3) to heavy pollution (151–154 µg m−3), with the dominant PM2.5 component changing from organic matter (OM) (39–45 µg m−3) to secondary inorganic ions (94–101 µg m−3). Similarly, TEM observations showed that S-rich particles internally mixed with OM (named S-OM) increased from 29 % to 60 % by number at an urban site and 64 % to 74 % at a mountain site from the moderate Haze-I to heavy Haze-I events, and 75 %–96 % of Haze-I particles included primary OM. We found that change of wind direction caused Haze-I to rapidly turn into Haze-II (185–223 µg m−3) with predominantly OM (98–133 µg m−3) and unexpectedly high K+ (3.8 µg m−3). TEM also showed that K-rich particles internally mixed with OM (named K-OM) increased from 4 %–5 % by number to 50 %–52 %. The results indicate that there were different sources of aerosol particles causing the Haze-I and Haze-II formation: Haze-I was mainly induced by accumulation of primary OM emitted from residential coal burning and further deteriorated by secondary aerosol formation via heterogeneous reactions; Haze-II was caused by long-range transport of agricultural biomass burning emissions. Moreover, abundant primary OM particles emitted from coal and biomass burning were considered to be one typical brown carbon, i.e., tar balls. Our study highlights that large numbers of light-absorbing tar balls significantly contribute to winter haze formation in northeast China and they should be further considered in climate models.

scholarly journals Chemical apportionment of southern African aerosol mass and optical depth

2009 ◽  
Vol 9 (3) ◽  
pp. 13439-13474
Author(s):  
B. I. Magi
Keyword(s):  
Optical Properties ◽  
Biomass Burning ◽  
Cross Sections ◽  
Southern Africa ◽  
Climate Models ◽  
Critical Role ◽  
Carbonaceous Aerosol ◽  
Aerosol Optical Properties ◽  
Carbonaceous Species ◽  
Aerosol Mass

Abstract. We investigate the aerosol mass apportionment and derive aerosol optical properties that characterize the aerosol over extratropical and tropical southern Africa during the biomass burning season. We find that 54% and 83% of the extratropical and tropical aerosol mass, respectively, is composed of carbonaceous species, consistent with the fact that the major source of particulate matter in southern Africa is biomass burning. This mass apportionment implies that carbonaceous species in the form of organic carbon (OC) and black carbon (BC) play a critical role in the aerosol optical properties. By combining the in situ measurements of aerosol mass concentrations with concurrent measurements of aerosol optical properties at a wavelength of 550 nm, we find that 80–90% of the aerosol scattering is due to carbonaceous aerosol, where our derived mass scattering cross sections (MSC) for OC and BC are 3.9±0.6 m2/g and 1.6±0.2 m2/g, respectively. Our derived values of mass absorption cross sections (MAC) for OC and BC are 0.7±0.6 m2/g and 8.2±1.1 m2/g, respectively. The values of MAC imply that 26–27% of the aerosol absorption in southern Africa is due to OC, with the remainder due to BC. Our results provide important constraints for aerosol properties in a region dominated by biomass burning and should be integrated into climate models to improve aerosol simulations.

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