Methyl-Nitrocatechols: Atmospheric Tracer Compounds for Biomass Burning Secondary Organic Aerosols

2010 ◽  
Vol 44 (22) ◽  
pp. 8453-8459 ◽  
Author(s):  
Yoshiteru Iinuma ◽  
Olaf Böge ◽  
Ricarda Gräfe ◽  
Hartmut Herrmann
Keyword(s):  
Biomass Burning ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Atmospheric Tracer

How quality and quantity of brown carbon influence singlet oxygen production in aqueous organic aerosols

2021 ◽  
Author(s):  
Sophie Bogler ◽  
Nadine Borduas-Dedekind ◽  
Imad el Haddad ◽  
David Bell ◽  
Kaspar Dällenbach
Keyword(s):  
Reactive Oxygen Species ◽  
Steady State ◽  
Quantum Yield ◽  
Singlet Oxygen ◽  
Molecular Oxygen ◽  
Biomass Burning ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Oxygen Species ◽  
Brown Carbon

<p>Singlet oxygen (<sup>1</sup>O<sub>2</sub>) is a reactive oxygen species that has recently gained attention as a competitive oxidant in the atmosphere. This excited state of molecular oxygen is formed by indirect photochemistry in the presence of chromophoric dissolved organic matter (DOM) as sensitizers, molecular oxygen and sunlight. The produced highly reactive intermediate <sup>1</sup>O<sub>2 </sub>is then capable of oxidizing and degrading many organic atmospheric components, thereby affecting their lifetime in the atmosphere. Despite this influence on atmospheric fate, the spatiotemporal distribution of <sup>1</sup>O<sub>2</sub> in particular matter (PM) is currently unknown. We hypothesized that brown carbon in biomass burning organic aerosols emitted during winter in Switzerland would lead to higher <sup>1</sup>O<sub>2</sub> steady-state concentrations in PM compared to summer. Therefore, to advance atmospheric <sup>1</sup>O<sub>2 </sub>research, we investigated the <sup>1</sup>O<sub>2</sub> sensitizing ability of organic aerosols sampled on 24-hour PM10 filters. Specifically, these filters were collected throughout 2013 in Frauenfeld and San Vittore in Switzerland, characterized as urban background and rural traffic measurement stations, respectively. We extracted the water-soluble organic components and quantified <sup>1</sup>O<sub>2 </sub>steady state concentrations as well as <sup>1</sup>O<sub>2</sub> quantum yield. The quantum yield enhances the data intercomparison as this value shows the normalization of <sup>1</sup>O<sub>2 </sub>production as a function of the rate of absorbance of the organic aerosols. In our ongoing efforts of expanding the spatiotemporal scale of our measurements, our results from Frauenfeld so far show a range between 0.38 – 6.05 · 10<sup>-13 </sup>M for <sup>1</sup>O<sub>2 </sub>steady state concentrations and quantum yields up to 2.1± 0.5<sup></sup>%. In preliminary experiments, samples from the rural site San Vittore show similar values, with potentially higher values during periods of significant biomass burning contributions. The values underline <sup>1</sup>O<sub>2</sub>’s<sub></sub>potential importance for atmospheric processing, e.g. comparing to Manfrin et al. (ES&T, 2019)<sup>1</sup> who reported <sup>1</sup>O<sub>2 </sub>steady state concentrations of 3 ± 1 · 10<sup>-14 </sup>M from secondary organic aerosols extracts. More importantly, the filter extracts analyzed thus far show a strong seasonal trend, with increased <sup>1</sup>O<sub>2 </sub>values and higher variability in winter as compared to summer. This result corroborates the hypothesis that there is more chromophoric DOM present in winter, due to a higher fraction of brown carbon emitted e.g. in biomass burning for residential heating. To extend this analysis, we are currently correlating the results for <sup>1</sup>O<sub>2 </sub>with molecular markers based on mass spectrometry data available from previous filter analysis provided by Daellenbach et al., (ACP, 2017)<sup>2</sup>. Finding these correlations will enable the prediction of <sup>1</sup>O<sub>2 </sub>sensitizing abilities of organic material present in the aerosols both qualitatively and quantitatively. In all, our work will help constrain the seasonal relevance of <sup>1</sup>O<sub>2 </sub>photochemistry in the atmosphere.</p><p><strong>References</strong></p><p>1. Manfrin, A. et al. Reactive Oxygen Species Production from Secondary Organic Aerosols: The Importance of Singlet Oxygen. Environmental Science & Technology 53, 8553–8562 (2019).<br>2. Daellenbach, K. R. et al. Long-term chemical analysis and organic aerosol source apportionment at nine sites in central Europe: source identification and uncertainty assessment. Atmospheric Chemistry and Physics 17, 13265–13282 (2017).</p>

Mechanisms and kinetic studies of OH-initiated atmospheric oxidation of methoxyphenols in the presence of O2 and NOx

2019 ◽  
Vol 21 (39) ◽  
pp. 21856-21866 ◽  
Author(s):  
Yanhui Sun ◽  
Fei Xu ◽  
Xiaofan Li ◽  
Qingzhu Zhang ◽  
Yuanxiang Gu
Keyword(s):  
Biomass Burning ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Kinetic Studies ◽  
Atmospheric Oxidation

Methoxyphenols, as the main products and tracers of biomass burning, have been demonstrated to play an important role in the formation of secondary organic aerosols.

scholarly journals Differentiating between primary and secondary organic aerosols of biomass burning in an environmental chamber with FTIR and AMS

2021 ◽  
Author(s):  
Amir Yazdani ◽  
Satoshi Takahama ◽  
Jack K. Kodros ◽  
Marco Paglione ◽  
Mauro Masiol ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Temporal Resolution ◽  
Biomass Burning ◽  
Secondary Organic Aerosols ◽  
Bulk Composition ◽  
Organic Aerosols ◽  
Chamber Wall ◽  
High Temporal Resolution ◽  
Environmental Chamber ◽  
Primary Emissions

<p>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.</p><p>    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.</p><p>    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.  A time-of-flight (ToF) AMS reported the composition of non-refractory PM<sub>1 </sub>every three minutes and PM<sub>1 </sub>was collected on PTFE filters over 20-minute periods before and after aging for off-line FTIR analysis.</p><p>    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 – 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.</p>

scholarly journals Large Discrepancy in the Formation of Secondary Organic Aerosols from Structurally Similar Monoterpenes

2021 ◽  
Vol 5 (3) ◽  
pp. 632-644
Author(s):  
Ditte Thomsen ◽  
Jonas Elm ◽  
Bernadette Rosati ◽  
Jane Tygesen Skønager ◽  
Merete Bilde ◽  
...  
Keyword(s):  
Secondary Organic Aerosols ◽  
Organic Aerosols

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

2006 ◽  
Vol 6 (11) ◽  
pp. 3257-3280 ◽  
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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