Case Study of Water-Soluble Metal Containing Organic Constituents of Biomass Burning Aerosol

2011 ◽  
Vol 45 (4) ◽  
pp. 1257-1263 ◽  
Author(s):  
Alexandra L. Chang-Graham ◽  
Luisa T. M. Profeta ◽  
Timothy J. Johnson ◽  
Robert J. Yokelson ◽  
Alexander Laskin ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Water Soluble ◽  
Organic Constituents ◽  
Biomass Burning Aerosol

scholarly journals Biomass burning contribution to Beijing aerosol

2013 ◽  
Vol 13 (3) ◽  
pp. 8387-8434 ◽  
Author(s):  
Y. Cheng ◽  
G. Engling ◽  
K. B. He ◽  
F. K. Duan ◽  
Y. L. Ma ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Elemental Carbon ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Winter Period ◽  
Summer Period ◽  
Pmf Model ◽  
Different Types ◽  
Biomass Burning Aerosol ◽  
Typical Summer

Abstract. Biomass burning, the largest global source of elemental carbon (EC) and primary organic carbon (OC), is strongly associated with many subjects of great scientific concern, such as secondary organic aerosol and brown carbon which exert important effects on the environment and on climate in particular. This study investigated the relationships between levoglucosan and other biomass burning tracers (i.e. water soluble potassium and mannosan) based on both ambient samples collected in Beijing and source samples. Compared with North America and Europe, Beijing was characterized by high ambient levoglucosan concentrations and low winter to summer ratios of levoglucosan, indicating significant impact of biomass burning activities throughout the year in Beijing. Comparison of levoglucosan and water soluble potassium (K+) levels suggested that it was acceptable to use K+ as a biomass burning tracer during summer in Beijing, while the contribution of fireworks to K+ could be significant during winter. Moreover, the levoglucosan to K+ ratio was found to be lower during the typical summer period (0.21±0.16) compared with the typical winter period (0.51±0.15). On the other hand, levoglucosan correlated strongly with mannosan (R2=0.97) throughout the winter and the levoglucosan to mannosan ratio averaged 9.49±1.63, whereas levoglucosan and mannosan exhibited relatively weak correlation (R2=0.73) during the typical summer period when the levoglucosan to mannosan ratio averaged 12.65±3.38. Results from PMF model analysis showed that about 50% of the OC and EC in Beijing were associated with biomass burning processes. In addition, a new source-identification method was developed based on the comparison of the levoglucosan to K+ ratio and the levoglucosan to mannosan ratio among different types of biomass. Using this method, the major source of biomass burning aerosol in Beijing was suggested to be the combustion of crop residuals, while the contribution from softwood burning was also non-negligible, especially in winter.

scholarly journals Chemical oxidative potential of secondary organic aerosol (SOA) generated from the photooxidation of biogenic and anthropogenic volatile organic compounds

2016 ◽  
Author(s):  
Wing Y. Tuet ◽  
Yunle Chen ◽  
Lu Xu ◽  
Shierly Fok ◽  
Dong Gao ◽  
...  
Keyword(s):  
Health Effects ◽  
Biomass Burning ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Hydrocarbon Emissions ◽  
Reaction Conditions ◽  
Oxidative Potential ◽  
Incomplete Combustion ◽  
Volatile Organic ◽  
Biomass Burning Aerosol

Abstract. Particulate matter (PM), of which a significant fraction is comprised of secondary organic aerosols (SOA), has received considerable attention due to their health implications. In this study, the water-soluble oxidative potential (OPWS) of SOA generated from the photooxidation of biogenic and anthropogenic hydrocarbon precursors (isoprene, α-pinene, β-caryophyllene, pentadecane, m-xylene, and naphthalene) under different reaction conditions (RO2 + HO2/RO2 + NO dominant, dry/humid) was characterized using dithiothreitol (DTT) consumption. The measured intrinsic OPWS-DTT ranged from 9–205 pmol min−1 µg−1 and were highly dependent on the specific hydrocarbon precursor, with naphthalene and isoprene SOA generating the highest and lowest OPWS-DTT, respectively. Humidity and RO2 fate affected OPWS-DTT in a hydrocarbon-specific manner, with naphthalene SOA exhibiting the most pronounced effects, likely due to the formation of nitroaromatics. Together, these results suggest that precursor identity may be more influential than reaction condition in determining SOA health effects, demonstrating the importance of sources, such as incomplete combustion, to aerosol toxicity. In the context of other PM sources, all SOA systems with the exception of naphthalene SOA were less DTT active than ambient sources related to incomplete combustion, including diesel and gasoline combustion as well as biomass burning. Finally, naphthalene SOA was as DTT active as biomass burning aerosol, which was found to be the most DTT active OA source in a previous ambient study. These results highlight a need to consider SOA contributions (particularly from anthropogenic hydrocarbons) to health effects in the context of hydrocarbon emissions, SOA yields, and other PM sources.

scholarly journals Chemical oxidative potential of secondary organic aerosol (SOA) generated from the photooxidation of biogenic and anthropogenic volatile organic compounds

2017 ◽  
Vol 17 (2) ◽  
pp. 839-853 ◽  
Author(s):  
Wing Y. Tuet ◽  
Yunle Chen ◽  
Lu Xu ◽  
Shierly Fok ◽  
Dong Gao ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Hydrocarbon Emissions ◽  
Reaction Conditions ◽  
Oxidative Potential ◽  
Incomplete Combustion ◽  
Volatile Organic ◽  
Specific Manner ◽  
Biomass Burning Aerosol

Abstract. Particulate matter (PM), of which a significant fraction is comprised of secondary organic aerosols (SOA), has received considerable attention due to its health implications. In this study, the water-soluble oxidative potential (OPWS) of SOA generated from the photooxidation of biogenic and anthropogenic hydrocarbon precursors (isoprene, α-pinene, β-caryophyllene, pentadecane, m-xylene, and naphthalene) under different reaction conditions (RO2+ HO2 vs. RO2+ NO dominant, dry vs. humid) was characterized using dithiothreitol (DTT) consumption. The measured intrinsic OPWS-DTT values ranged from 9 to 205 pmol min−1 µg−1 and were highly dependent on the specific hydrocarbon precursor, with naphthalene and isoprene SOA generating the highest and lowest OPWS-DTT values, respectively. Humidity and RO2 fate affected OPWS-DTT in a hydrocarbon-specific manner, with naphthalene SOA exhibiting the most pronounced effects, likely due to the formation of nitroaromatics. Together, these results suggest that precursor identity may be more influential than reaction condition in determining SOA oxidative potential, demonstrating the importance of sources, such as incomplete combustion, to aerosol toxicity. In the context of other PM sources, all SOA systems, with the exception of naphthalene SOA, were less DTT active than ambient sources related to incomplete combustion, including diesel and gasoline combustion as well as biomass burning. Finally, naphthalene SOA was as DTT active as biomass burning aerosol, which was found to be the most DTT-active OA source in a previous ambient study. These results highlight a need to consider SOA contributions (particularly from anthropogenic hydrocarbons) to health effects in the context of hydrocarbon emissions, SOA yields, and other PM sources.

scholarly journals Investigation of molar volume and surfactant characteristics of water-soluble organic compounds in biomass burning aerosol

2007 ◽  
Vol 7 (2) ◽  
pp. 3589-3627 ◽  
Author(s):  
A. Asa-Awuku ◽  
A. Nenes ◽  
A. P. Sullivan ◽  
C. J. Hennigan ◽  
R. J. Weber
Keyword(s):  
Surface Tension ◽  
Molar Volume ◽  
Biomass Burning ◽  
Solid Phase ◽  
Relative Proportion ◽  
Water Soluble ◽  
Original Sample ◽  
Biomass Burning Aerosol ◽  
Hydrophobic Fraction ◽  
Ccn Activity

Abstract. In this study, we characterize the CCN activity of the water-soluble organics in biomass burning aerosol. The aerosol after collection upon filters is dissolved in water using sonication. Hydrophobic and hydrophilic components are fractionated from a portion of the original sample using solid phase extraction, and subsequently desalted. The surface tension and CCN activity of these different samples are measured with a KSV CAM 200 goniometer and a DMT Streamwise Thermal Gradient CCN Counter, respectively. The measurements show that the strongest surfactants are isolated in the hydrophobic fraction, while the hydrophilics exhibit negligible surface tension depression. The presence of salts (primarily (NH4)2SO4) in the hydrophobic fraction substantially enhances surface tension depression; their synergistic effects considerably enhance CCN activity, exceeding that of pure (NH4)2SO4. For our analysis, average thermodynamic properties (i.e., molar volume) are determined for samples using our newly developed Köhler Theory Analysis (KTA) method. We have found that, the molar mass of the hydrophilic and hydrophobic aerosol components is estimated to be 87±26 g mol−1 and 780±231 g mol−1, respectively. KTA also suggests that the relative proportion (in moles) of hydrophobic to hydrophilic compounds in the original sample to be 1:3. For the first time, KTA is applied to an aerosol with this level of complexity and displays its potential for providing physically-based constraints for GCM parameterizations of the aerosol indirect effect.

scholarly journals Biomass burning contribution to Beijing aerosol

2013 ◽  
Vol 13 (15) ◽  
pp. 7765-7781 ◽  
Author(s):  
Y. Cheng ◽  
G. Engling ◽  
K.-B. He ◽  
F.-K. Duan ◽  
Y.-L. Ma ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Winter Period ◽  
Summer Period ◽  
Positive Matrix ◽  
Pmf Model ◽  
Different Types ◽  
Biomass Burning Aerosol ◽  
Typical Summer

Abstract. Biomass burning, the largest global source of elemental carbon (EC) and primary organic carbon (OC), is strongly associated with many subjects of great scientific concern, such as secondary organic aerosol and brown carbon which exert important effects on the environment and on climate in particular. This study investigated the relationships between levoglucosan and other biomass burning tracers (i.e., water soluble potassium and mannosan) based on both ambient samples collected in Beijing and source samples. Compared with North America and Europe, Beijing was characterized by high ambient levoglucosan concentrations and low winter to summer ratios of levoglucosan, indicating significant impact of biomass burning activities throughout the year in Beijing. Comparison of levoglucosan and water soluble potassium (K+) levels suggested that it was acceptable to use K+ as a biomass burning tracer during summer in Beijing, while the contribution of fireworks to K+ could be significant during winter. Moreover, the levoglucosan to K+ ratio was found to be lower during the typical summer period (0.21 ± 0.16) compared with the typical winter period (0.51 ± 0.15). Levoglucosan correlated strongly with mannosan (R2 = 0.97) throughout the winter and the levoglucosan to mannosan ratio averaged 9.49 ± 1.63, whereas levoglucosan and mannosan exhibited relatively weak correlation (R2 = 0.73) during the typical summer period when the levoglucosan to mannosan ratio averaged 12.65 ± 3.38. Results from positive matrix factorization (PMF) model analysis showed that about 50% of the OC and EC in Beijing were associated with biomass burning processes. In addition, a new source identification method was developed based on the comparison of the levoglucosan to K+ ratio and the levoglucosan to mannosan ratio among different types of biomass. Using this method, the major source of biomass burning aerosol in Beijing was suggested to be the combustion of crop residuals, while the contribution from softwood burning was also non-negligible, especially in winter.

scholarly journals Chemical aging of single and multicomponent biomass burning aerosol surrogate-particles by OH: implications for cloud condensation nucleus activity

2015 ◽  
Vol 15 (5) ◽  
pp. 6771-6819
Author(s):  
J. H. Slade ◽  
R. Thalman ◽  
J. Wang ◽  
D. A. Knopf
Keyword(s):  
Biomass Burning ◽  
Wet Deposition ◽  
Water Solubility ◽  
Inorganic Compounds ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Oh Radicals ◽  
Chemical Aging ◽  
Biomass Burning Aerosol ◽  
Ccn Activity

Abstract. Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low soluble single-component OA by OH and O3 can increase their water-solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water-solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate-particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH/O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~0.1, indicating that chemically-aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally-mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient amount of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide-range of solubilities.

scholarly journals Chemical aging of single and multicomponent biomass burning aerosol surrogate particles by OH: implications for cloud condensation nucleus activity

2015 ◽  
Vol 15 (17) ◽  
pp. 10183-10201 ◽  
Author(s):  
J. H. Slade ◽  
R. Thalman ◽  
J. Wang ◽  
D. A. Knopf
Keyword(s):  
Biomass Burning ◽  
Wet Deposition ◽  
Water Solubility ◽  
Inorganic Compounds ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Oh Radicals ◽  
Chemical Aging ◽  
Biomass Burning Aerosol ◽  
Ccn Activity

Abstract. Multiphase OH and O3 oxidation reactions with atmospheric organic aerosol (OA) can influence particle physicochemical properties including composition, morphology, and lifetime. Chemical aging of initially insoluble or low-soluble single-component OA by OH and O3 can increase their water solubility and hygroscopicity, making them more active as cloud condensation nuclei (CCN) and susceptible to wet deposition. However, an outstanding problem is whether the effects of chemical aging on their CCN activity are preserved when mixed with other organic or inorganic compounds exhibiting greater water solubility. In this work, the CCN activity of laboratory-generated biomass burning aerosol (BBA) surrogate particles exposed to OH and O3 is evaluated by determining the hygroscopicity parameter, κ, as a function of particle type, mixing state, and OH and O3 exposure applying a CCN counter (CCNc) coupled to an aerosol flow reactor (AFR). Levoglucosan (LEV), 4-methyl-5-nitrocatechol (MNC), and potassium sulfate (KS) serve as representative BBA compounds that exhibit different hygroscopicity, water solubility, chemical functionalities, and reactivity with OH radicals, and thus exemplify the complexity of mixed inorganic/organic aerosol in the atmosphere. The CCN activities of all of the particles were unaffected by O3 exposure. Following exposure to OH, κ of MNC was enhanced by an order of magnitude, from 0.009 to ~ 0.1, indicating that chemically aged MNC particles are better CCN and more prone to wet deposition than pure MNC particles. No significant enhancement in κ was observed for pure LEV particles following OH exposure. κ of the internally mixed particles was not affected by OH oxidation. Furthermore, the CCN activity of OH-exposed MNC-coated KS particles is similar to the OH unexposed atomized 1 : 1 by mass MNC : KS binary-component particles. Our results strongly suggest that when OA is dominated by water-soluble organic carbon (WSOC) or inorganic ions, chemical aging has no significant impact on OA hygroscopicity. The organic compounds exhibiting low solubility behave as if they are infinitely soluble when mixed with a sufficient number of water-soluble compounds. At and beyond this point, the particles' CCN activity is governed entirely by the water-soluble fraction and is not influenced by the oxidized organic fraction. Our results have important implications for heterogeneous oxidation and its impact on cloud formation given that atmospheric aerosol is a complex mixture of organic and inorganic compounds exhibiting a wide range of solubilities.

scholarly journals Long-range aerosol transport and impacts on size-resolved aerosol composition in Metro Manila, Philippines

2020 ◽  
Vol 20 (4) ◽  
pp. 2387-2405 ◽  
Author(s):  
Rachel A. Braun ◽  
Mojtaba Azadi Aghdam ◽  
Paola Angela Bañaga ◽  
Grace Betito ◽  
Maria Obiminda Cambaliza ◽  
...  
Keyword(s):  
Long Range ◽  
Biomass Burning ◽  
Dicarboxylic Acids ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Long Range Transport ◽  
Aerosol Transport ◽  
Range Transport ◽  
Metro Manila ◽  
Biomass Burning Aerosol

Abstract. This study analyzes long-range transport of aerosol and aerosol chemical characteristics based on instances of high- and low-aerosol-loading events determined via ground-based size-resolved aerosol measurements collected at the Manila Observatory in Metro Manila, Philippines, from July to October 2018. Multiple data sources, including models, remote sensing, and in situ measurements, are used to analyze the impacts of long-range aerosol transport on Metro Manila and the conditions at the local and synoptic scales facilitating this transport. Through the use of case studies, evidence of long-range transport of biomass burning aerosol and continental emissions is identified in Metro Manila. Long-range transport of biomass burning aerosol from the Maritime Continent, bolstered by southwesterly flow and permitted by low rainfall, was identified through model results and the presence of biomass burning tracers (e.g., K, Rb) in the ground-based measurements. The impacts of emissions transported from continental East Asia on the aerosol characteristics in Metro Manila are also identified; for one of the events analyzed, this transport was facilitated by the nearby passage of a typhoon. Changes in the aerosol size distributions, water-soluble chemical composition, and contributions of various organic aerosol species to the total water-soluble organic aerosol were examined for the different cases. The events impacted by biomass burning transport had the overall highest concentration of water-soluble organic acids, while the events impacted by long-range transport from continental East Asia showed high percent contributions from shorter-chain dicarboxylic acids (i.e., oxalate) that are often representative of photochemical and aqueous processing in the atmosphere. The low-aerosol-loading event was subject to a larger precipitation accumulation than the high-aerosol events, indicative of wet scavenging as an aerosol sink in the study region. This low-aerosol event was characterized by a larger relative contribution from supermicrometer aerosols and had a higher percent contribution from longer-chain dicarboxylic acids (i.e., maleate) to the water-soluble organic aerosol fraction, indicating the importance of both primary aerosol emissions and local emissions.

scholarly journals Open cells exhibit weaker entrainment of free-tropospheric biomass burning aerosol into the south-east Atlantic boundary layer

2020 ◽  
Vol 20 (7) ◽  
pp. 4059-4084 ◽  
Author(s):  
Steven J. Abel ◽  
Paul A. Barrett ◽  
Paquita Zuidema ◽  
Jianhao Zhang ◽  
Matt Christensen ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Carbon Monoxide ◽  
Biomass Burning ◽  
Cloud Base ◽  
Trade Wind ◽  
The South ◽  
East Atlantic ◽  
Accumulation Mode ◽  
Biomass Burning Aerosol

Abstract. This work presents synergistic satellite, airborne and surface-based observations of a pocket of open cells (POC) in the remote south-east Atlantic. The observations were obtained over and upwind of Ascension Island during the CLouds and Aerosol Radiative Impacts and Forcing (CLARIFY) and the Layered Smoke Interacting with Clouds (LASIC) field experiments. A novel aspect of this case study is that an extensive free-tropospheric biomass burning aerosol plume that had been transported from the African continent was observed to be in contact with the boundary layer inversion over the POC and the surrounding closed cellular cloud regime. The in situ measurements show marked contrasts in the boundary layer thermodynamic structure, cloud properties, precipitation and aerosol conditions between the open cells and surrounding overcast cloud field. The data demonstrate that the overlying biomass burning aerosol was mixing down into the boundary layer in the stratocumulus cloud downwind of the POC, with elevated carbon monoxide, black carbon mass loadings and accumulation-mode aerosol concentrations measured beneath the trade-wind inversion. The stratocumulus cloud in this region was moderately polluted and exhibited very little precipitation falling below cloud base. A rapid transition to actively precipitating cumulus clouds and detrained stratiform remnants in the form of thin quiescent veil clouds was observed across the boundary into and deep within the POC. The subcloud layer in the POC was much cleaner than that in the stratocumulus region. The clouds in the POC formed within an ultra-clean layer (accumulation-mode aerosol concentrations of approximately a few cm−3) in the upper region of the boundary layer, which was likely to have been formed via efficient collision–coalescence and sedimentation processes. Enhanced Aitken-mode aerosol concentrations were also observed intermittently in this ultra-clean layer, suggesting that new particle formation was taking place. Across the boundary layer inversion and immediately above the ultra-clean layer, accumulation-mode aerosol concentrations were ∼ 1000 cm−3. Importantly, the air mass in the POC showed no evidence of elevated carbon monoxide over and above typical background conditions at this location and time of year. As carbon monoxide is a good tracer for biomass burning aerosol that is not readily removed by cloud processing and precipitation, it demonstrates that the open cellular convection in the POC is not able to entrain large quantities of the free-tropospheric aerosol that was sitting directly on top of the boundary layer inversion. This suggests that the structure of the mesoscale cellular convection may play an important role in regulating the transport of aerosol from the free troposphere down into the marine boundary layer. We then develop a climatology of open cellular cloud conditions in the south-east Atlantic from 19 years of September Moderate Resolution Imaging Spectroradiometer (MODIS) Terra imagery. This shows that the maxima in open cell frequency (> 0.25) occurs far offshore and in a region where subsiding biomass burning aerosol plumes may often come into contact with the underlying boundary layer cloud. If the results from the observational case study applied more broadly, then the apparent low susceptibility of open cells to free-tropospheric intrusions of additional cloud condensation nuclei could have some important consequences for aerosol–cloud interactions in the region.

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