Secondary organic aerosols produced from photochemical oxidation of secondarily evaporated biomass burning organic gases: Chemical composition, toxicity, optical properties, and climate effect

Fine particulate matter (PM) affects visibility, climate and public health. Organic matter (OM), which is hard to characterize due to its complex chemical composition, can constitute more than half of the PM. Biomass burning from residential wood burning, wildfires, and prescribed burning is a major source of OM with an ever-increasing importance.&#160; &#160; Aerosol mass spectrometry (AMS) and Fourier transform infrared spectroscopy (FTIR) are two complementary methods of identifying the chemical composition of OM. AMS measures the bulk composition of OM with relatively high temporal resolution but provides limited parent compound information. FTIR, carried out on samples collected on Teflon filters, provides detailed functional groupinformation at the expense of relatively low temporal resolution.&#160; &#160; In this study, we used these two methods to better understand the evolution of biomass burning OM in the atmosphere with aging. For this purpose, primary emissions from wood and pellet stoves were injected into the Center for Studies of Air Qualities and Climate Change (C-STACC) environmental chamber at ICE-HT/FORTH. Primary emissions were aged using hydroxyl and nitrate radicals (with atmospherically relevant exposures) simulating atmospheric day-time and night-time oxidation.&#160; A time-of-flight (ToF) AMS reported the composition of non-refractory PM1&#160;every three minutes and PM1&#160;was collected on PTFE filters over 20-minute periods before and after aging for off-line FTIR analysis.&#160; &#160; We found that AMS and FTIR measurements agreed well in terms of measured OM mass concentration, the OM:OC ratio, and concentration of biomass burning tracers &#8211; lignin and levoglucosan. AMS OM concentration was used to estimate chamber wall loss rates which were then used separate the contribution of primary and secondary organic aerosols (POA and SOA) to the aged OM. AMS mass spectra and FTIR spectra of biomass burning SOA and estimates of bulk composition were obtained by this procedure. FTIR and AMS spectra of SOA produced by OH oxidation of biomass burning volatile organic compounds (VOCs) were dominated by acid signatures. Organonitrates, on the other hand, appeared to be important in the SOA aged by the nitrate radical. The spectra from the two instruments also indicated that the signatures of certain compounds such as levoglucosan, lignin and hydrocarbons, which are abundant in biomass burning POA, diminish with aging significantly more than what can be attributed to chamber wall losses. The latter suggests biomass burning POA chemical composition might change noticeably due to heterogeneous reactions or partitioning in the atmosphere. Therefore, the common assumption of stable POA composition is only partially true. In addition, more stable biomass burning tracers should be used to be able to identify highly aged biomass burning aerosols in the atmosphere.

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Aerosol chemical and optical properties over the Paris area within ESQUIF project

Atmospheric Chemistry and Physics ◽

10.5194/acp-6-3257-2006 ◽

2006 ◽

Vol 6 (11) ◽

pp. 3257-3280 ◽

Cited By ~ 29

Author(s):

A. Hodzic ◽

R. Vautard ◽

P. Chazette ◽

L. Menut ◽

B. Bessagnet

Keyword(s):

Optical Properties ◽

Secondary Organic Aerosols ◽

Organic Aerosols ◽

Dust Particles ◽

Aerosol Size Distribution ◽

Aerosol Composition ◽

Aerosol Mass ◽

Coarse Mode ◽

Paris Area ◽

Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

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Optical properties of secondary organic aerosols generated by photooxidation of aromatic hydrocarbons

Scientific Reports ◽

10.1038/srep04922 ◽

2014 ◽

Vol 4 (1) ◽

Cited By ~ 36

Author(s):

Kun Li ◽

Weigang Wang ◽

Maofa Ge ◽

Jiangjun Li ◽

Dong Wang

Keyword(s):

Optical Properties ◽

Aromatic Hydrocarbons ◽

Secondary Organic Aerosols ◽

Organic Aerosols

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Tracing the Relative Significance of Primary versus Secondary Organic Aerosols from Biomass Burning Plumes over Coastal Ocean Using Sugar Compounds and Stable Carbon Isotopes

ACS Earth and Space Chemistry ◽

10.1021/acsearthspacechem.9b00140 ◽

2019 ◽

Vol 3 (8) ◽

pp. 1471-1484 ◽

Cited By ~ 4

Author(s):

Srinivas Bikkina ◽

Md. Mozammel Haque ◽

Manmohan Sarin ◽

Kimitaka Kawamura

Keyword(s):

Carbon Isotopes ◽

Biomass Burning ◽

Stable Carbon Isotopes ◽

Secondary Organic Aerosols ◽

Organic Aerosols ◽

Coastal Ocean ◽

Stable Carbon ◽

Relative Significance

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Aerosol chemical and optical properties over the Paris area within ESQUIF project

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-6-401-2006 ◽

2006 ◽

Vol 6 (1) ◽

pp. 401-454 ◽

Cited By ~ 3

Author(s):

A. Hodzic ◽

R. Vautard ◽

P. Chazette ◽

L. Menut ◽

B. Bessagnet

Keyword(s):

Optical Properties ◽

Secondary Organic Aerosols ◽

Organic Aerosols ◽

Dust Particles ◽

Aerosol Size Distribution ◽

Aerosol Composition ◽

Aerosol Mass ◽

Coarse Mode ◽

Paris Area ◽

Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environment against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce fairly well the plume structure and location both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirmed the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicated that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated of about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%) and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrated the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

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