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 Processing of biomass burning aerosol in the Eastern Mediterranean during summertime

2013 ◽  
Vol 13 (10) ◽  
pp. 25969-25999 ◽  
Author(s):  
A. Bougiatioti ◽  
I. Stavroulas ◽  
E. Kostenidou ◽  
P. Zarmpas ◽  
C. Theodosi ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Biomass Burning ◽  
Eastern Mediterranean ◽  
Late Summer ◽  
Organic Aerosol ◽  
High Temporal Resolution ◽  
Night Time ◽  
Air Masses ◽  
Aerosol Mass ◽  
Atmospheric Processing

Abstract. The aerosol chemical composition in air masses affected by wildfires from the Greek islands of Chios, Euboea and Andros, the Dalmatian Coast and Sicily, during late summer of 2012 was characterized at the remote background site of Finokalia, Crete. Air masses were transported several hundreds of kilometers, arriving at the measurement station after approximately half a day of transport, mostly during night-time. The chemical composition of the particulate matter was studied by different high temporal resolution instruments, including an Aerosol Chemical Speciation Monitor (ACSM) and a seven-wavelength aethalometer. Despite the large distance from emission and long atmospheric processing, a clear biomass burning organic aerosol (BBOA) profile containing characteristic markers is derived from BC measurements and Positive Matrix Factorization (PMF) analysis of the ACSM mass spectra. The ratio of fresh to aged BBOA decreases with increasing atmospheric processing time and BBOA components appear to be converted to oxygenated organic aerosol (OOA). Given that the smoke was mainly transported overnight, it appears that the processing can take place in the dark. These results show that a significant fraction of the BBOA loses its characteristic AMS signature and is transformed to OOA in less than a day. This implies that biomass burning can contribute almost half of the organic aerosol mass in the area during summertime.

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

scholarly journals Sources and processes that control the submicron organic aerosol in an urban Mediterranean environment (Athens) using high temporal resolution chemical composition measurements

2018 ◽  
Author(s):  
Iasonas Stavroulas ◽  
Aikaterini Bougiatioti ◽  
Despina Paraskevopoulou ◽  
Georgios Grivas ◽  
Eleni Liakakou ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Biomass Burning ◽  
Volatile Component ◽  
Organic Aerosol ◽  
Urban Environments ◽  
High Temporal Resolution ◽  
Organic Fraction ◽  
Scanning Mobility Particle Sizer ◽  
Secondary Aerosol ◽  
Combustion Sources

Abstract. Submicron aerosol chemical composition has been studied during a year-long period (26/07/2016–31/07/2017) and two winter-time intensive campaigns (18/12/2013–21/02/2014 and 23/12/2015–17/02/2016), at a central site in Athens, Greece, using an Aerosol Chemical Speciation Monitor (ACSM). Concurrent measurements include a Particle-Into-Liquid Sampler (PILS-IC), a Scanning Mobility Particle Sizer (SMPS), an AE-33 Aethalometer and Ion Chromatography analysis on 24 or 12 hour filter samples. Quality of the ACSM data was assured by comparison versus the above mentioned measurements. The aim of the study was to characterize the seasonal variability of the main fine aerosol constituents and decipher the sources of organic aerosol (OA). Organics were found to contribute almost half of the submicron mass, with concentrations during wintertime reaching up to 200 μg m−3, on occasions. During this season, the primary sources contribute about 34 % of the organic fraction, comprising of biomass burning (10 %), fossil fuel combustion (16 %) and cooking (8 %), while the remaining 66 % is attributed to secondary aerosol. The semi-volatile component of the oxidized organic aerosol (SV-OOA; 31 %) was found to be clearly linked to combustion sources and in particular biomass burning, and even a part of the very oxidized, low-volatility component (LV-OOA; 35 %) could also be attributed to the oxidation of emissions from these primary combustion sources. These results highlight the rising importance of biomass burning in urban environments during wintertime, as revealed through this characteristic example of Athens, Greece, where the economic recessions led to an abrupt shift to biomass burning for heating purposes in winter. During summer, when concentrations of fine aerosols are considerably lower, more than 80 % of the organic fraction is attributed to secondary aerosol (SV-OOA 30 % and LV-OOA 53 %). In contrast to winter, SV-OOA appears to result from a well-mixed type of aerosol, linked to fast photochemical processes and the oxidation of primary traffic and biogenic emissions. Finally, LV-OOA presents a more regional character in summer, owing to the oxidation, within a few days, of organic aerosol.

Combined Determination of the Chemical Composition and of Health Effects of Secondary Organic Aerosols: The POLYSOA Project

2008 ◽  
Vol 0 (0) ◽  
pp. 080207080519480-10 ◽  
Author(s):  
Urs Baltensperger ◽  
Josef Dommen ◽  
M. Rami Alfarra ◽  
Jonathan Duplissy ◽  
Kathrin Gaeggeler ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Health Effects ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols

scholarly journals Comparison between simulated and observed chemical composition of fine aerosols in Paris (France) during springtime: contribution of regional versus continental emissions

2010 ◽  
Vol 10 (24) ◽  
pp. 11987-12004 ◽  
Author(s):  
J. Sciare ◽  
O. d'Argouges ◽  
Q. J. Zhang ◽  
R. Sarda-Estève ◽  
C. Gaimoz ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Secondary Organic Aerosols ◽  
Transport Model ◽  
Organic Aerosols ◽  
Carbonaceous Material ◽  
Chemical Components ◽  
Carbonaceous Aerosols ◽  
Time Resolved ◽  
Air Masses ◽  
North Western

Abstract. Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. <2.5 μm) have been determined experimentally from fast measurements performed for a 3-week period in spring 2007 in Paris (France). The sum of these two chemical components (ions and carbonaceous aerosols) has shown to account for most of the fine aerosol mass (PM2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5 > 15 μg m−3 were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM2.5 concentrations (typically of about 10 μg m−3); carbonaceous aerosols contributing for most of this mass (typically 75%). In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM2.5 over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM2.5 and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols.

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

&lt;p&gt;Singlet oxygen (&lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt;) 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 &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;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 &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; 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 &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; steady-state concentrations in PM compared to summer. Therefore, to advance atmospheric &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;research, we investigated the &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; 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 &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;steady state concentrations as well as &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt; quantum yield. The quantum yield enhances the data intercomparison as this value shows the normalization of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;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 &amp;#8211; 6.05 &amp;#183; 10&lt;sup&gt;-13 &lt;/sup&gt;M for &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;steady state concentrations and quantum yields up to 2.1&amp;#177; 0.5&lt;sup&gt;&lt;/sup&gt;%. 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 &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2&lt;/sub&gt;&amp;#8217;s&lt;sub&gt;&lt;/sub&gt;potential importance for atmospheric processing, e.g. comparing to Manfrin et al. (ES&amp;T, 2019)&lt;sup&gt;1&lt;/sup&gt; who reported &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;steady state concentrations of 3 &amp;#177; 1 &amp;#183; 10&lt;sup&gt;-14 &lt;/sup&gt;M from secondary organic aerosols extracts. More importantly, the filter extracts analyzed thus far show a strong seasonal trend, with increased &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;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 &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;with molecular markers based on mass spectrometry data available from previous filter analysis provided by Daellenbach et al., (ACP, 2017)&lt;sup&gt;2&lt;/sup&gt;. Finding these correlations will enable the prediction of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;sensitizing abilities of organic material present in the aerosols both qualitatively and quantitatively. In all, our work will help constrain the seasonal relevance of &lt;sup&gt;1&lt;/sup&gt;O&lt;sub&gt;2 &lt;/sub&gt;photochemistry in the atmosphere.&lt;/p&gt;&lt;p&gt;&lt;strong&gt;References&lt;/strong&gt;&lt;/p&gt;&lt;p&gt;1. Manfrin, A. et al. Reactive Oxygen Species Production from Secondary Organic Aerosols: The Importance of Singlet Oxygen. Environmental Science &amp; Technology 53, 8553&amp;#8211;8562 (2019).&lt;br&gt;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&amp;#8211;13282 (2017).&lt;/p&gt;

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