Photodegradation of secondary organic aerosol generated from limonene oxidation by ozone studied with chemical ionization mass spectrometry

Pan, Xiang; Underwood, J. S.; Xing, Jiangkuan; Mang, Stephen A.; Nizkorodov, Sergey A.

doi:10.5194/acpd-9-4727-2009

Cited by 6 publications

(6 citation statements)

References 67 publications

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“…Our observations are consistent with work that shows the production of acetone during photodegradation of SOA (Lee et al, ; Malecha & Nizkorodov, ). However, our dark ozonolysis experiments also generated some acetone, consistent with SOA formation also yielding acetone as a by‐product (Pan et al, ).…”

Section: Resultssupporting

confidence: 85%

Production of Secondary Organic Aerosol During Aging of Biomass Burning Smoke From Fresh Fuels and Its Relationship to VOC Precursors

et al. 2019

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After smoke from burning biomass is emitted into the atmosphere, chemical and physical processes change the composition and amount of organic aerosol present in the aged, diluted plume. During the fourth Fire Lab at Missoula Experiment, we performed smog‐chamber experiments to investigate formation of secondary organic aerosol (SOA) and multiphase oxidation of primary organic aerosol (POA). We simulated atmospheric aging of diluted smoke from a variety of biomass fuels while measuring particle composition using high‐resolution aerosol mass spectrometry. We quantified SOA formation using a tracer ion for low‐volatility POA as a reference standard (akin to a naturally occurring internal standard). These smoke aging experiments revealed variable organic aerosol (OA) enhancements, even for smoke from similar fuels and aging mechanisms. This variable OA enhancement correlated well with measured differences in the amounts of emitted volatile organic compounds (VOCs) that could subsequently be oxidized to form SOA. For some aging experiments, we were able to predict the SOA production to within a factor of 2 using a fuel‐specific VOC emission inventory that was scaled by burn‐specific toluene measurements. For fires of coniferous fuels that were dominated by needle burning, volatile biogenic compounds were the dominant precursor class. For wiregrass fires, furans were the dominant SOA precursors. We used a POA tracer ion to calculate the amount of mass lost due to gas‐phase oxidation and subsequent volatilization of semivolatile POA. Less than 5% of the POA mass was lost via multiphase oxidation‐driven evaporation during up to 2 hr of equivalent atmospheric oxidation.

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Section: Resultssupporting

confidence: 85%

Production of Secondary Organic Aerosol During Aging of Biomass Burning Smoke From Fresh Fuels and Its Relationship to VOC Precursors

et al. 2019

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“…The photochemical degradation of secondary organic aerosol can be another source of CH 3 COOH in the urban areas (Malecha & Nizkorodov, ; Pan et al, ; Sareen et al, ). Considering the photolysis rate of SOA as J SOA = 4 × 10 −4 .…”

Section: Resultsmentioning

confidence: 99%

Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI

et al. 2018

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Acetic acid (CH3COOH) is one of the most abundant carboxylic acids in the troposphere. In the study, the tropospheric chemistry of CH3COOH is investigated using the 3‐D global chemistry transport model, STOCHEM‐CRI. The highest mixing ratios of surface CH3COOH are found in the tropics by as much as 1.6 ppb in South America. The model predicts the seasonality of CH3COOH reasonably well and correlates with some surface and flight measurement sites, but the model drastically underpredicts levels in urban and midlatitudinal regions. The possible reasons for the underprediction are discussed. The simulations show that the lifetime and global burden of CH3COOH are 1.6–1.8 days and 0.45–0.61 Tg, respectively. The reactions of the peroxyacetyl radical (CH3CO3) with the hydroperoxyl radical (HO2) and other organic peroxy radicals (RO2) are found to be the principal sources of tropospheric CH3COOH in the model, but the model‐measurement discrepancies suggest the possible unknown or underestimated sources which can contribute large fractions of the CH3COOH burden. The major sinks of CH3COOH in the troposphere are wet deposition, dry deposition, and OH loss. However, the reaction of CH3COOH with Criegee intermediates is proposed to be a potentially significant chemical loss process of tropospheric CH3COOH that has not been previously accounted for in global modeling studies. Inclusion of this loss process reduces the tropospheric CH3COOH level significantly which can give even larger discrepancies between model and measurement data, suggesting that the emissions inventory and the chemical production sources of CH3COOH are underpredicted even more so in current global models.

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“…Other identified primary sources include agriculture (Ngwabie et al, ) and combustion of biomass (Chaliyakunnel et al, ; Goode et al, ) and fossil fuels (Kawamura et al, ; Talbot et al, ). Heterogeneous sources have also been proposed, including in‐cloud formaldehyde oxidation (Jacob, ; Lelieveld & Crutzen, ), as well as aging of organic aerosol via OH (Vlasenko et al, ), O 3 (Eliason et al, ; Pan et al, ), and photolysis (Malecha & Nizkorodov, ; Park et al, ). Wet and dry deposition are the predominant HCOOH sinks; together with photochemical loss and a minor contribution from dust uptake, these yield an overall atmospheric lifetime of 2–4 days (Chebbi & Carlier, ; Paulot et al, ; Stavrakou et al, ).…”

Section: Introductionmentioning

confidence: 99%

Oxidation of Volatile Organic Compounds as the Major Source of Formic Acid in a Mixed Forest Canopy

Alwe

Millet

Chen

et al. 2019

Geophysical Research Letters

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Formic acid (HCOOH) is among the most abundant carboxylic acids in the atmosphere, but its budget is poorly understood. We present eddy flux, vertical gradient, and soil chamber measurements from a mixed forest and apply the data to better constrain HCOOH source/sink pathways. While the cumulative above‐canopy flux was downward, HCOOH exchange was bidirectional, with extended periods of net upward and downward flux. Net above‐canopy fluxes were mostly upward during warmer/drier periods. The implied gross canopy HCOOH source corresponds to 3% and 38% of observed isoprene and monoterpene carbon emissions and is 15× underestimated in a state‐of‐science atmospheric model (GEOS‐Chem). Gradient and soil chamber measurements identify the canopy layer as the controlling source of HCOOH or its precursors to the forest environment; below‐canopy sources were minor. A correlation analysis using an ensemble of marker volatile organic compounds suggests that secondary formation, not direct emission, is the major source driving ambient HCOOH.

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Photodegradation of secondary organic aerosol generated from limonene oxidation by ozone studied with chemical ionization mass spectrometry

Cited by 6 publications

References 67 publications

Production of Secondary Organic Aerosol During Aging of Biomass Burning Smoke From Fresh Fuels and Its Relationship to VOC Precursors

Production of Secondary Organic Aerosol During Aging of Biomass Burning Smoke From Fresh Fuels and Its Relationship to VOC Precursors

Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI

Oxidation of Volatile Organic Compounds as the Major Source of Formic Acid in a Mixed Forest Canopy

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