Morphology of Organic Carbon Coatings on Biomass-Burning Particles and Their Role in Reactive Gas Uptake

Abstract. Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5–2.0 μm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 μm (PM1) was measured by a high resolution aerosol mass spectrometer (HR-AMS). The field site was also influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire influenced periods, 0.5–2.0 μm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O/C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon/organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models under-predicting organic carbon (OC) in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest United States, particularly considering increasing intensity and frequency of Canadian wildfires.

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Ubiquitous influence of wildfire emissions and secondary organic aerosol on summertime atmospheric aerosol in the forested Great Lakes region

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-3701-2018 ◽

2018 ◽

Vol 18 (5) ◽

pp. 3701-3715 ◽

Cited By ~ 15

Author(s):

Matthew J. Gunsch ◽

Nathaniel W. May ◽

Miao Wen ◽

Courtney L. H. Bottenus ◽

Daniel J. Gardner ◽

...

Keyword(s):

Organic Carbon ◽

Great Lakes ◽

Long Range ◽

Mass Spectrometer ◽

Biomass Burning ◽

Secondary Organic Aerosol ◽

Organic Aerosol ◽

Great Lakes Region ◽

Aerosol Mass ◽

Biomass Burning Particles

Abstract. Long-range aerosol transport affects locations hundreds of kilometers from the point of emission, leading to distant particle sources influencing rural environments that have few major local sources. Source apportionment was conducted using real-time aerosol chemistry measurements made in July 2014 at the forested University of Michigan Biological Station near Pellston, Michigan, a site representative of the remote forested Great Lakes region. Size-resolved chemical composition of individual 0.5–2.0 µm particles was measured using an aerosol time-of-flight mass spectrometer (ATOFMS), and non-refractory aerosol mass less than 1 µm (PM1) was measured with a high-resolution aerosol mass spectrometer (HR-AMS). The field site was influenced by air masses transporting Canadian wildfire emissions and urban pollution from Milwaukee and Chicago. During wildfire-influenced periods, 0.5–2.0 µm particles were primarily aged biomass burning particles (88 % by number). These particles were heavily coated with secondary organic aerosol (SOA) formed during transport, with organics (average O∕C ratio of 0.8) contributing 89 % of the PM1 mass. During urban-influenced periods, organic carbon, elemental carbon–organic carbon, and aged biomass burning particles were identified, with inorganic secondary species (ammonium, sulfate, and nitrate) contributing 41 % of the PM1 mass, indicative of atmospheric processing. With current models underpredicting organic carbon in this region and biomass burning being the largest combustion contributor to SOA by mass, these results highlight the importance for regional chemical transport models to accurately predict the impact of long-range transported particles on air quality in the upper Midwest, United States, particularly considering increasing intensity and frequency of Canadian wildfires.

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Quantifying primary and secondary humic-like substances in urban aerosol based on emission source characterization and a source-oriented air quality model

10.5194/acp-2018-779 ◽

2018 ◽

Author(s):

Xinghua Li ◽

Junzan Han ◽

Philip K. Hopke ◽

Jingnan Hu ◽

Qi Shu ◽

...

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

Coal Combustion ◽

Power Plants ◽

Water Soluble ◽

Aerosol Formation ◽

Source Characterization ◽

Air Quality Model ◽

Coal Burning ◽

Residential Coal

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.

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Fossil and non-fossil source contributions to atmospheric carbonaceous aerosols during extreme spring grassland fires in Eastern Europe

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-5513-2016 ◽

2016 ◽

Vol 16 (9) ◽

pp. 5513-5529 ◽

Cited By ~ 21

Author(s):

Vidmantas Ulevicius ◽

Steigvilė Byčenkienė ◽

Carlo Bozzetti ◽

Athanasia Vlachou ◽

Kristina Plauškaitė ◽

...

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

Nitrogen Isotopes ◽

Early Spring ◽

Total Carbon ◽

Carbonaceous Aerosols ◽

Pmf Model ◽

Source Contributions ◽

The Baltic ◽

The Impact

Abstract. In early spring the Baltic region is frequently affected by high-pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires. Non-refractory submicron particulate matter (NR-PM1) was measured by an Aerodyne aerosol chemical speciation monitor (ACSM) and a source apportionment with the multilinear engine (ME-2) running the positive matrix factorization (PMF) model was applied to the organic aerosol fraction to investigate the impact of biomass/grass burning. Satellite observations over regions of biomass burning activity supported the results and identification of air mass transport to the area of investigation. Sharp increases in biomass burning tracers, such as levoglucosan up to 683 ng m−3 and black carbon (BC) up to 17 µg m−3 were observed during this period. A further separation between fossil and non-fossil primary and secondary contributions was obtained by coupling ACSM PMF results and radiocarbon (14C) measurements of the elemental (EC) and organic (OC) carbon fractions. Non-fossil organic carbon (OCnf) was the dominant fraction of PM1, with the primary (POCnf) and secondary (SOCnf) fractions contributing 26–44 % and 13–23 % to the total carbon (TC), respectively. 5–8 % of the TC had a primary fossil origin (POCf), whereas the contribution of fossil secondary organic carbon (SOCf) was 4–13 %. Non-fossil EC (ECnf) and fossil EC (ECf) ranged from 13–24 and 7–13 %, respectively. Isotope ratios of stable carbon and nitrogen isotopes were used to distinguish aerosol particles associated with solid and liquid fossil fuel burning.

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A review of biomass burning emissions, part II: Intensive physical properties of biomass burning particles

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-4-5135-2004 ◽

2004 ◽

Vol 4 (5) ◽

pp. 5135-5200 ◽

Cited By ~ 29

Author(s):

J. S. Reid ◽

R. Koppmann ◽

T. F. Eck ◽

D. P. Eleuterio

Keyword(s):

Particle Size ◽

Biomass Burning ◽

Measurement Techniques ◽

Emission Factors ◽

Future Research ◽

Data Set ◽

Particle Properties ◽

In Situ Experiments ◽

Literature Base ◽

Biomass Burning Particles

Abstract. The last decade has seen tremendous advances in atmospheric aerosol particle research that is often performed in the context of climate and global change science. Biomass burning, one of the largest sources of accumulation mode particles globally, has been closely studied for its radiative, geochemical, and dynamic impacts. These studies have taken many forms including laboratory burns, in situ experiments, remote sensing, and modeling. While the differing perspectives of these studies have ultimately improved our qualitative understanding of biomass burning issues, the varied nature of the work make inter-comparisons and resolutions of some specific issues difficult. In short, the literature base has become a milieu of small pieces of the biomass-burning puzzle. This manuscript, the second part of four, examines the properties of biomass-burning particle emissions. Here we review and discuss the literature concerning the measurement of smoke particle size, chemistry, thermodynamic properties, and emission factors. Where appropriate, critiques of measurement techniques are presented. We show that very large differences in measured particle properties have appeared in the literature, in particular with regards to particle carbon budgets. We investigate emissions uncertainties using scale analyses, which shows that while emission factors for grass and brush are relatively well known, very large uncertainties still exist in emission factors of boreal, temperate and some tropical forests. Based on an uncertainty analysis of the community data set of biomass burning measurements, we present simplified models for particle size and emission factors. We close this review paper with a discussion of the community experimental data, point to lapses in the data set, and prioritize future research topics.

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Diurnal variations of organic molecular tracers and stable carbon isotopic compositions in atmospheric aerosols over Mt. Tai in North China Plain: an influence of biomass burning

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-9079-2012 ◽

2012 ◽

Vol 12 (4) ◽

pp. 9079-9124

Author(s):

P. Q. Fu ◽

K. Kawamura ◽

J. Chen ◽

J. Li ◽

Y. L. Sun ◽

...

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

North China Plain ◽

North China ◽

Secondary Organic Aerosol ◽

Organic Aerosol ◽

Total Carbon ◽

Stable Carbon ◽

Isotopic Compositions ◽

Carbon Isotopic

Abstract. Organic tracer compounds of tropospheric aerosols, as well as organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC), and stable carbon isotope ratios (δ13C) of total carbon (TC) have been investigated for aerosol samples collected during early and late periods of Mount Tai eXperiment 2006 (MTX2006) field campaign in North China Plain. Total solvent extracts were investigated by gas chromatography/mass spectrometry. More than 130 organic compounds were detected in the aerosol samples. They were grouped into twelve organic compound classes, including biomass burning tracers, biogenic primary sugars, biogenic secondary organic aerosol (SOA) tracers, and anthropogenic tracers such as phthalates, hopanes and polycyclic aromatic hydrocarbons (PAHs). In early June when the field burning activities of wheat straws in North China Plain were very active, the total identified organics (2090 ± 1170 ng m−3) were double those in late June (926 ± 574 ng m−3). All the compound classes were more abundant in early June than in late June, except phthalate esters, which were higher in late June. Levoglucosan (88–1210 ng m−3, 403 ng m−3) was found as the most abundant single compound in early June, while diisobutyl phthalate was the predominant species in late June. During the biomass-burning period in early June, the diurnal trends of most of the primary and secondary organic aerosol tracers were characterized by the concentration peaks observed at mid-night or in early morning, while in late June most of the organic species peaked in late afternoon. This suggests that smoke plumes from biomass burning can uplift the aerosol particulate matter to a certain altitude and then transported to and encountered the summit of Mt. Tai during nighttime. On the basis of the tracer-based method for the estimation of biomass-burning OC, fungal-spore OC and biogenic secondary organic carbon (SOC), we estimate that an average of 24% (up to 64%) of the OC in the Mt. Tai aerosols was due to biomass burning in early June, followed by the contribution of isoprene SOC (mean 4.3%). In contrast, isoprene SOC was the main contributor (6.6%) to OC, and only 3.0% of the OC was due to biomass burning in late June. In early June, δ13C of TC (−26.6‰ to −23.2‰, mean −25.0‰) were lower than those (−23.9‰ to −21.9‰, mean −22.9‰) in late June. In addition, a strong anti-correlation was found between levoglucosan and δ13C values. This study demonstrates that crop-residue burning activities can significantly enhance the organic aerosol loading and alter the organic molecular compositions and stable carbon isotopic compositions of aerosol particles in the troposphere over North China Plain.

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Investigation of atmospheric aerosols over semi-urban and urban areas in Eastern Indo-Gangetic Plain: seasonal variability and source apportionment using PMF

10.5194/egusphere-egu21-14205 ◽

2021 ◽

Author(s):

Kanishtha Dubey ◽

Shubha Verma

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

Atmospheric Aerosols ◽

Urban Areas ◽

Relative Concentration ◽

Road Dust ◽

Water Soluble ◽

Carbonaceous Aerosols ◽

Gangetic Plain ◽

Brick Kilns

The study investigates the chemical composition and source of aerosol origin at a semi-urban (Kharagpur&#8211;Kgp) and urban (Kolkata&#8211;Kol) region during the period February 2015 to January 2016 and September 2010 to August 2011 respectively. Major water-soluble inorganic aerosols (WSII) were determined using Ion chromatography and carbonaceous aerosols (CA) using OC&#8211;EC analyser. A multivariate factor analysis Positive Matrix Factorization (PMF) was used in resolving source of aerosols at the study locations. Seasonal analysis of WSII at Kgp and Kol indicated relative dominance of calcium at both the places followed by sodium, chloride, and magnesium ions. Non-sea salt potassium (nss&#8211;K+), a biomass burning tracer was found higher at Kol than at Kgp. Sum of secondary aerosols sulphate (SO42-), nitrate (NO3-) and ammonium (NH4+) was higher at Kol than Kgp with relative concentration of SO42- being higher than NO3- at Kgp which was vice-versa at Kol. Examination of carbonaceous aerosols showed three times higher concentration of organic carbon (OC) than elemental carbon (EC) with monthly mean of OC/EC ratio > 2, indicating likely formation of secondary organic carbon formation. Seasonal influence of biomass burning inferred from nss&#8211;K+ (OC/EC) ratio relationship indicated dissimilarity in seasonality of biomass burning at Kgp (Kol). PMF resolved sources for Kgp constituted of secondary aerosol emissions, biomass burning, fugitive dust, marine aerosols, crustal dust and emissions from brick kilns while for Kol factors constituted of burning of waste, resuspended paved road dust, coal combustion, sea spray aerosols, vehicular emissions and biomass burning.

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Optical Properties of Laboratory and Ambient Biomass Burning Aerosols: Elucidating Black, Brown, and Organic Carbon Components and Mixing Regimes

Journal of Geophysical Research Atmospheres ◽

10.1029/2018jd029892 ◽

2019 ◽

Vol 124 (9) ◽

pp. 5088-5105 ◽

Cited By ~ 10

Author(s):

Dian E. Romonosky ◽

Samantha L. Gomez ◽

Jared Lam ◽

Christian M. Carrico ◽

Allison C. Aiken ◽

...

Keyword(s):

Optical Properties ◽

Organic Carbon ◽

Biomass Burning

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Fossil vs. non-fossil sources of fine carbonaceous aerosols in four Chinese cities during the extreme winter haze episode of 2013

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-1299-2015 ◽

2015 ◽

Vol 15 (3) ◽

pp. 1299-1312 ◽

Cited By ~ 113

Author(s):

Y.-L. Zhang ◽

R.-J. Huang ◽

I. El Haddad ◽

K.-F. Ho ◽

J.-J. Cao ◽

...

Keyword(s):

Particulate Matter ◽

Organic Carbon ◽

Biomass Burning ◽

Water Soluble ◽

Total Carbon ◽

World Health ◽

Biomass Combustion ◽

Carbonaceous Aerosols ◽

Haze Episode ◽

Mass Concentrations

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.

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Dynamic light absorption of biomass-burning organic carbon photochemically aged under natural sunlight

Atmospheric Chemistry and Physics ◽

10.5194/acp-14-1517-2014 ◽

2014 ◽

Vol 14 (3) ◽

pp. 1517-1525 ◽

Cited By ~ 110

Author(s):

M. Zhong ◽

M. Jang

Keyword(s):

Organic Carbon ◽

Biomass Burning ◽

Light Absorption ◽

Dynamic Change ◽

Wood Smoke ◽

Integrating Sphere ◽

Natural Sunlight ◽

Wood Burning ◽

Polycyclic Aromatic ◽

Uv Visible

Abstract. Wood-burning aerosol produced under smoldering conditions was photochemically aged with different relative humidity (RH) and NOx conditions using a 104 m3 dual outdoor chamber under natural sunlight. Light absorption of organic carbon (OC) was measured over the course of photooxidation using a UV–visible spectrometer connected to an integrating sphere. At high RH, the color decayed rapidly. NOx slightly prolonged the color of wood smoke, suggesting that NOx promotes the formation of chromophores via secondary processes. Overall, the mass absorption cross section (integrated between 280 and 600 nm) of OC increased by 11–54% (except high RH) in the morning and then gradually decreased by 19–68% in the afternoon. This dynamic change in light absorption of wood-burning OC can be explained by two mechanisms: chromophore formation and sunlight bleaching. To investigate the effect of chemical transformation on light absorption, wood smoke particles were characterized using various spectrometers. The intensity of fluorescence, which is mainly related to polycyclic aromatic hydrocarbons (PAHs), rapidly decreased with time, indicating the potential bleaching of PAHs. A decline of levoglucosan concentrations evinced the change of primary organic aerosol with time. The aerosol water content measured by Fourier transform infrared spectroscopy showed that wood-burning aerosol became less hygroscopic as photooxidation proceeded. A similar trend in light absorption changes has been observed in ambient smoke aerosol originating from the 2012 County Line wildfire in Florida. We conclude that the biomass-burning OC becomes less light absorbing after 8–9 h sunlight exposure compared to fresh wood-burning OC.

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