Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer

Abstract. A series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA) concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC) instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA) production. After correcting for wall losses, the average increase in organic matter (OM) concentrations by SOA formation for the starting and flaming phase experiments with the two log wood burners was found to be a factor of 4.1±1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Including the measured SOA formation potential, average emission factors of BC+POA+SOA, calculated from CO2 emission, were found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C2H4O2+ at mass to charge ratio m/z 60, a commonly used marker for primary emissions of wood burning. This contribution at m/z 60 can overcompensate for the degradation of levoglucosan leading to an overestimation of the contribution of wood burning or biomass burning to the total OM. The primary organic emissions from the three different burners showed a wide range in O:C atomic ratio (0.19−0.60) for the starting and flaming conditions, which also increased during aging. Primary wood burning emissions have a rather low relative contribution at m/z 43 (f 43) to the total organic mass spectrum. The non-oxidized fragment C3H7+ has a considerable contribution at m/z 43 for the fresh OA with an increasing contribution of the oxygenated ion C2H3O+ during aging. After five hours of aging, the OA has a rather low C2H3O+ signal for a given CO2+ fraction, possibly indicating a higher ratio of acid to non-acid oxygenated compounds in wood burning OA compared to other oxygenated organic aerosol (OOA).

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Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-11-8081-2011 ◽

2011 ◽

Vol 11 (3) ◽

pp. 8081-8113 ◽

Cited By ~ 6

Author(s):

M. F. Heringa ◽

P. F. DeCarlo ◽

R. Chirico ◽

T. Tritscher ◽

J. Dommen ◽

...

Keyword(s):

High Resolution ◽

Mass Spectrometer ◽

Organic Aerosol ◽

Smog Chamber ◽

Resolution Time ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Wood Burning ◽

Primary Emissions ◽

Stable Burning

Abstract. A series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA) concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC) instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA) production. After correcting for wall losses, the average increase in organic matter (OM) concentrations by SOA formation for the starting and flaming phase experiments with the two logwood burners was found to be a factor of 4.1 ± 1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Average emission factors of BC + POA + SOA, calculated from CO2 emission, were found to be in the range of 0.04 to 3.9 g kg−1 wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C2H4O2+ at mass to charge ratio m/z 60, a commonly used marker for primary emissions of wood burning. The primary organic emissions from the three different burners showed a wide range in O/C atomic ratio (0.19–0.60) for the starting and flaming conditions, which also increased during aging. Primary wood burning emissions have a rather low relative contribution at m/z 43 (f43) to the total organic mass spectrum. The non-oxidized fragment C3H7+ has a considerable contribution at m/z 43 for the fresh OA with an increasing contribution of the oxygenated ion C2H3O+ during aging. After five hours of aging, the OA has a rather low C2H3O+ signal for a given CO2+ fraction, possibly indicating a higher ratio of acid to non-acid oxygenated compounds in wood burning OA compared to other OOA.

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Chemical characterization of secondary organic aerosol at a rural site in the southeastern US: insights from simultaneous high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and FIGAERO chemical ionization mass spectrometer (CIMS) measurements

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-8421-2020 ◽

2020 ◽

Vol 20 (14) ◽

pp. 8421-8440

Author(s):

Yunle Chen ◽

Masayuki Takeuchi ◽

Theodora Nah ◽

Lu Xu ◽

Manjula R. Canagaratna ◽

...

Keyword(s):

High Resolution ◽

Mass Spectrometer ◽

Chemical Ionization ◽

Secondary Organic Aerosol ◽

Time Of Flight ◽

Organic Aerosol ◽

Ionization Mass ◽

Resolution Time ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass

Abstract. The formation and evolution of secondary organic aerosol (SOA) were investigated at Yorkville, GA, in late summer (mid-August to mid-October 2016). The organic aerosol (OA) composition was measured using two online mass spectrometry instruments, the high-resolution time-of-flight aerosol mass spectrometer (AMS) and the Filter Inlet for Gases and AEROsols coupled to a high-resolution time-of-flight iodide-adduct chemical ionization mass spectrometer (FIGAERO-CIMS). Through analysis of speciated organics data from FIGAERO-CIMS and factorization analysis of data obtained from both instruments, we observed notable SOA formation from isoprene and monoterpenes during both day and night. Specifically, in addition to isoprene epoxydiol (IEPOX) uptake, we identified isoprene SOA formation from non-IEPOX pathways and isoprene organic nitrate formation via photooxidation in the presence of NOx and nitrate radical oxidation. Monoterpenes were found to be the most important SOA precursors at night. We observed significant contributions from highly oxidized acid-like compounds to the aged OA factor from FIGAERO-CIMS. Taken together, our results showed that FIGAERO-CIMS measurements are highly complementary to the extensively used AMS factorization analysis, and together they provide more comprehensive insights into OA sources and composition.

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Elemental analysis of chamber organic aerosol using an aerodyne high-resolution aerosol mass spectrometer

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-9-27485-2009 ◽

2009 ◽

Vol 9 (6) ◽

pp. 27485-27542 ◽

Cited By ~ 1

Author(s):

P. S. Chhabra ◽

R. C. Flagan ◽

J. H. Seinfeld

Keyword(s):

High Resolution ◽

Elemental Composition ◽

Mass Spectrometer ◽

Organic Aerosol ◽

Resolution Time ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Single Ring ◽

Spectrometer Data ◽

Ambient Measurements

Abstract. The elemental composition of laboratory chamber secondary organic aerosol (SOA) from glyoxal uptake, α-pinene ozonolysis, isoprene photooxidation, single-ring aromatic photooxidation, and naphthalene photooxidation is evaluated using Aerodyne high-resolution time-of-flight mass spectrometer data. SOA O/C ratios ranged from 1.13 for glyoxal to 0.30–0.43 for α-pinene ozonolysis. The elemental composition of α-pinene and naphthalene SOA was also confirmed by offline mass spectrometry. The fraction of organic signal at m/z 44 is generally a good measure of SOA oxygenation for all systems except for glyoxal uptake, in which m/z 44 substantially underpredicts O/C. Although chamber SOA has generally been considered less oxygenated than ambient SOA, single-ring aromatic- and naphthalene-derived SOA can reach O/C ratios upward of 0.7, well within the range of OOA, though still not as high as some ambient measurements. The spectra of aromatic- and isoprene-high-NOx SOA resemble that of OOA, but the spectrum of glyoxal uptake does not resemble that of any PMF component.

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A comprehensive evaluation of aerosol extinction apportionment in Beijing using a high-resolution time-of-flight aerosol mass spectrometer

The Science of The Total Environment ◽

10.1016/j.scitotenv.2021.146976 ◽

2021 ◽

Vol 783 ◽

pp. 146976

Author(s):

Lingbin Kong ◽

Jinyuan Xin ◽

Wenkang Gao ◽

Guiqian Tang ◽

Xuemei Wang ◽

...

Keyword(s):

High Resolution ◽

Mass Spectrometer ◽

Comprehensive Evaluation ◽

Time Of Flight ◽

Aerosol Extinction ◽

Resolution Time ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass

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Characterization of the sources and processes of organic and inorganic aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-10-22669-2010 ◽

2010 ◽

Vol 10 (10) ◽

pp. 22669-22723 ◽

Cited By ~ 5

Author(s):

Y.-L. Sun ◽

Q. Zhang ◽

J. J. Schwab ◽

K. L. Demerjian ◽

W.-N. Chen ◽

...

Keyword(s):

New York ◽

New York City ◽

High Resolution ◽

Mass Spectrometer ◽

York City ◽

Time Of Flight ◽

Resolution Time ◽

Aerosol Mass Spectrometer ◽

Spectral Pattern ◽

Aerosol Mass

Abstract. Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during the summer 2009 Field Intensive Study at Queens College in New York City. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of total PM1 mass on average. The average mass size distribution of OA presents a small mode peaking at ~150 nm (Dva) in addition to an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of sulfate and OA both show pronounced peaks between 01:00–02:00 p.m. EST due to photochemical production. The average (±1σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012(±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62(±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified five OA components: a hydrocarbon-like OA (HOA), two types of oxygenated OA (OOA) including a low-volatility OOA (LV-OOA) and a semi-volatile OOA (SV-OOA), a cooking-emission related OA (COA), and a unique nitrogen-enriched OA (NOA). HOA appears to represent primary OA (POA) from urban traffic emissions. It comprises primarily of reduced species (H/C=1.83; O/C=0.06) and shows a mass spectral pattern very similar to those of POA from fossil fuel combustion, and correlates tightly with traffic emission tracers including elemental carbon and NOx. LV-OOA, which is highly oxidized (O/C=0.63) and correlates well with sulfate, appears to be representative for regional, aged secondary OA (SOA). SV-OOA, which is less oxidized (O/C=0.38) and correlates well with non-refractory chloride, likely represents less photo-chemically aged, semi-volatile SOA. COA shows a similar spectral pattern to the reference spectra of POA from cooking emissions and a distinct diurnal pattern peaking around local lunch and dinner times. In addition, NOA is characterized with prominent CxH2x+2N+ peaks likely from amine compounds. Our results indicate that cooking-related activities are a major source of POA in NYC, releasing comparable amounts of POA as traffic emissions. POA=HOA+COA) on average accounts for ~30% of the total OA mass during this study while SOA dominates the OA composition with SV-OOA and LV-OOA on average accounting for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC involves a~continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that nitrogen-containing organic species such as amines might have played an important role in the atmospheric processing of OA in NYC, likely involving acid-base chemistry. Analysis of air mass trajectories and satellite imagery of aerosol optical depth (AOD) indicates that the high potential source regions of secondary sulfate and aged OA are mainly located in regions to the west and southwest of the city.

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Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-8933-2010 ◽

2010 ◽

Vol 10 (18) ◽

pp. 8933-8945 ◽

Cited By ~ 231

Author(s):

X.-F. Huang ◽

L.-Y. He ◽

M. Hu ◽

M. R. Canagaratna ◽

Y. Sun ◽

...

Keyword(s):

High Resolution ◽

Mass Spectrometer ◽

Olympic Games ◽

Aerosol Particles ◽

Organic Aerosol ◽

Organic Mass ◽

Aerosol Mass Spectrometer ◽

Beijing Olympic Games ◽

Aerosol Mass ◽

2008 Beijing Olympic Games

Abstract. As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008), an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008). The campaign mean PM1 mass concentration was 63.1 ± 39.8 μg m−3; the mean composition consisted of organics (37.9%), sulfate (26.7%), ammonium (15.9%), nitrate (15.8%), black carbon (3.1%), and chloride (0.87%). The average size distributions of the species (except BC) were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF) analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA), cooking-related (COA), and two oxygenated organic aerosols (OOA-1 and OOA-2), which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C) compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses contained a large fraction of primary HOA and COA species, probably due to stronger influences from local emissions. The lowest concentration levels for all major species were obtained during the Olympic game days (8 to 24 August 2008), possibly due to the effects of both strict emission controls and favorable meteorological conditions.

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Elemental analysis of chamber organic aerosol using an aerodyne high-resolution aerosol mass spectrometer

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-4111-2010 ◽

2010 ◽

Vol 10 (9) ◽

pp. 4111-4131 ◽

Cited By ~ 132

Author(s):

P. S. Chhabra ◽

R. C. Flagan ◽

J. H. Seinfeld

Keyword(s):

High Resolution ◽

Elemental Composition ◽

Mass Spectrometer ◽

Organic Aerosol ◽

Uptake System ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Single Ring ◽

Spectrometer Data ◽

Ambient Measurements

Abstract. The elemental composition of laboratory chamber secondary organic aerosol (SOA) from glyoxal uptake, α-pinene ozonolysis, isoprene photooxidation, single-ring aromatic photooxidation, and naphthalene photooxidation is evaluated using Aerodyne high-resolution time-of-flight mass spectrometer data. SOA O/C ratios range from 1.13 for glyoxal uptake experiments to 0.30–0.43 for α-pinene ozonolysis. The elemental composition of α-pinene and naphthalene SOA is also confirmed by offline mass spectrometry. The fraction of organic signal at m/z 44 is generally a good measure of SOA oxygenation for α-pinene/O3, isoprene/high-NOx, and naphthalene SOA systems. The agreement between measured and estimated O/C ratios tends to get closer as the fraction of organic signal at m/z 44 increases. This is in contrast to the glyoxal uptake system, in which m/z 44 substantially underpredicts O/C. Although chamber SOA has generally been considered less oxygenated than ambient SOA, single-ring aromatic- and naphthalene-derived SOA can reach O/C ratios upward of 0.7, well within the range of ambient PMF component OOA, though still not as high as some ambient measurements. The spectra of aromatic and isoprene-high-NOx SOA resemble that of OOA, but the spectrum of glyoxal uptake does not resemble that of any ambient organic aerosol PMF component.

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The contribution of wood burning and other pollution sources to wintertime organic aerosol levels in two Greek cities

10.5194/acp-2016-721 ◽

2016 ◽

Cited By ~ 3

Author(s):

Kalliopi Florou ◽

Dimitrios K. Papanastasiou ◽

Michael Pikridas ◽

Christos Kaltsonoudis ◽

Evangelos Louvaris ◽

...

Keyword(s):

Peak Concentration ◽

Fine Particulate Matter ◽

Organic Aerosol ◽

Resolution Time ◽

Major Goal ◽

Aerosol Mass Spectrometer ◽

Aerosol Mass ◽

Fine Particulate ◽

Wood Burning ◽

Range Transport

Abstract. The composition of fine particulate matter (PM) in two major Greek cities (Athens and Patras) was measured during two wintertime campaigns conducted in 2013 and 2012, respectively. A major goal of this study is to quantify the sources of organic aerosol (OA) and especially residential wood burning, which has dramatically increased due to the Greek financial crisis. A high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in both sites. PM with diameter less than 1 μm (PM1) consisted mainly of organics (60–75 %), black carbon (5–20 %) and inorganic salts (around 20 %) in both Patras and Athens. In Patras, during evening hours, PM1 concentrations were as high as 100 μg m–, of which 85 % were OA. In Athens, the maximum hourly value observed during nighttime was 140 μg m−3, of which 120 μg m−3 was OA. 40–60 % of the average OA was due to biomass burning for both cities, while the remaining mass originated from traffic (12–17 %), cooking (12–16 %) and long-range transport (18–24%). The contribution of residential wood burning was even higher (80–90 %) during the nighttime peak concentration periods, and less than 10 % during daytime. Cooking OA contributed up to 75 % during mealtime hours in Patras, while traffic-related OA was responsible for 60–70 % of the OA during the morning rush hour.

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