Evolution of the chemical fingerprint of biomass burning organic aerosol during aging

Abstract

Abstract. A thermal desorption aerosol gas chromatograph coupled to a high resolution -time of flight -aerosol mass spectrometer (TAG-AMS) was connected to an atmospheric chamber for the molecular characterization of the evolution of organic aerosol (OA) emitted by woodstove appliances for residential heating. Two log woodstoves (old and modern) and one pellet stove were operated under typical conditions. Emissions were aged during a time equivalent to 5 h of atmospheric aging. The five to seven samples were collected and analyzed with the TAG-AMS during each experiment. We detected and quantified over 70 compounds, including levoglucosan and nitrocatechols. We calculate the emission factor (EF) of these tracers in the primary emissions and highlight the influence of the combustion efficiency on these emissions. Smoldering combustion contributes to a higher EF and a more complex composition. We also demonstrate the effect of atmospheric aging on the chemical fingerprint. The tracers are sorted into three categories according to the evolution of their concentration: primary compounds, non-conventional primary compounds, and secondary compounds. For each, we provide a quantitative overview of their contribution to the OA mass at different times of the photooxidative process.

Impact of anthropogenic and biogenic sources on the seasonal variation in the molecular composition of urban organic aerosols: a field and laboratory study using ultra-high-resolution mass spectrometry

“…These compounds are consistent with products from lignin pyrolysis ( Fig. S4, Bertrand et al, 2017Bertrand et al, , 2018 and contributed significantly to the CHO signal recorded for primary wood-burning emissions but less for aged emissions (57 %,49 %,44 % of CHO aromatic;5 %,3 %,3 % of condensed aromatic;and 38 %,48 %,53 % of non-aromatic for fresh, 10 h, and 30 h atmospherically aged emissions, respectively). The ambient wood-burning pollution showed a similar distribution of the CHO signal as aged laboratory wood-burning emissions (Magadino -46 % aromatic, 6 % condensed aromatic, 48 % non-aromatic; San Vittore -44 % aromatic, 4 % condensed aromatic, 52 % non-aromatic), and the detailed chemical composition was similar to the fresh laboratory woodburning emissions (Fig.…”

“…The chemical analyses were complemented with other filterbased analyses. Organic and elemental carbon (OC, EC) concentrations were determined for Zurich, Magadino, San Vittore, and Hyytiälä by a thermo-optical transmission (TOT) method with a Sunset OC/EC analyser (Birch and Cary, 1996), following the EUSAAR-2 thermal-optical transmission protocol (Cavalli et al, 2010). Water-soluble inorganic ions (K + , Na + , Mg 2+ , Ca 2+ , NH + 4 ; and SO 2− 4 , NO − 3 , Cl − ) were measured by ion chromatography for Zurich, Magadino, and San Vittore (Piazzalunga et al, 2013;Jaffrezo et al, 1998).…”

Molecular and physical characteristics of aerosol at a remote free troposphere site: implications for atmospheric aging

“…Rapid oxidation was also observed in studies of biomass burning organic aerosol in Africa (Capes et al, 2008;Vakkari et al, 2014), over the Mediterranean Sea (Bougiatioti et al, 2014), and Hyytiälä, Finland Vogel et al, 2013). Other studies focused on the oxidation of molecular tracers such as levoglucosan have shown that they can be degraded rapidly after emission, depending on the atmospheric conditions (Lai et al, 2014;Slade et al, 2014;Arrangio et al, 2015;Bertrand et al, 2018). These studies all demonstrate the importance of oxidation to the aging of organic aerosol and provide motivation for studies of long-range-transported organic aerosol.…”

“…Likewise, PMO-1 and PMO-3 exhibit an increase in the number frequency of higher DBE species, which is not observed in PMO-2, supporting the observation of an increased overall aromaticity for these free tropospheric aerosol samples. Many aromatic compounds, such as PAHs are known to be carcinogens, and are a product of incomplete combustion biomass burning and anthropogenic emissions (Perraudin et al, 2006;Bignal et al, 2008).…”

More Than Emissions and Chemistry: Fire Size, Dilution, and Background Aerosol Also Greatly Influence Near‐Field Biomass Burning Aerosol Aging

“…Biomass burning smoke is a significant source of primary and secondary atmospheric particles that have impacts on climate (Bond et al, ), air quality (e.g., Jaffe & Wigder, ; Nie et al, ; Xie et al, ), and health (e.g., Jassen et al, ; Johnston et al, ; Naeher et al, ; Zhang et al, ). Biomass burning emits primary carbonaceous aerosol (both as black carbon and primary organic aerosol; POA; Akagi et al, ; Reid, Koppmann, et al, , and references therein), inorganic aerosol, and vapors, where some vapors may serve as aerosol precursors (e.g., Alvarado & Prinn, ; Bertrand et al, ; Hatch et al, ; Jen et al, ). Biomass burning particle emissions are dominated by an accumulation mode, with a less‐concentrated coarse mode and occasionally a nucleation mode (Reid, Koppmann, et al, ).…”