Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass

Bahreini, R.; Middlebrook, A. M.; Gouw, J. A. de; Warneke, C.; Trainer, M.; Brock, C. A.; Stark, Harald; Brown, Steven S.; Dubé, W. P.; Gilman, J. B.; Hall, K.L.; Holloway, J. S.; Kuster, W. C.; Perring, A. E.; Prévôt, Andrê S. H.; Schwarz, J. P.; Spackman, J. R.; Szidat, Sönke; Wagner, Nick; Weber, R. J.; Zotter, Peter; Parrish, D. D.

doi:10.1029/2011gl050718

Cited by 210 publications

(219 citation statements)

References 56 publications

(72 reference statements)

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“…Accounting for unspeciated organics more than doubled the predicted contribution of gasoline vehicles to ambient SOA. Both models predicted that gasoline contributes much more SOA than diesel (e.g., six times more in the updated model), which is qualitatively similar to Bahreini et al (41) but in contrast to Gentner et al (19). The updated model also showed (not included in Fig.…”

supporting

confidence: 72%

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

Jathar

Gordon

Hennigan

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

226

294

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Secondary organic aerosol (SOA) formed from the atmospheric oxidation of nonmethane organic gases (NMOG) is a major contributor to atmospheric aerosol mass. Emissions and smog chamber experiments were performed to investigate SOA formation from gasoline vehicles, diesel vehicles, and biomass burning. About 10-20% of NMOG emissions from these major combustion sources are not routinely speciated and therefore are currently misclassified in emission inventories and chemical transport models. The smog chamber data demonstrate that this misclassification biases model predictions of SOA production low because the unspeciated NMOG produce more SOA per unit mass than the speciated NMOG. We present new source-specific SOA yield parameterizations for these unspeciated emissions. These parameterizations and associated source profiles are designed for implementation in chemical transport models. Box model calculations using these new parameterizations predict that NMOG emissions from the top six combustion sources form 0.7 Tg y −1 of first-generation SOA in the United States, almost 90% of which is from biomass burning and gasoline vehicles. About 85% of this SOA comes from unspeciated NMOG, demonstrating that chemical transport models need improved treatment of combustion emissions to accurately predict ambient SOA concentrations.particulate matter | air quality | photochemical oxidation | volatile organic compounds | emissions inventory

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supporting

confidence: 72%

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

Jathar

Gordon

Hennigan

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

226

294

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“…Recently Gentner et al (2012) concluded that diesel engine vehicle emissions were more important than gasoline engine vehicle emissions as a source of SOA for urban regions in California. The opposite conclusion was drawn by Bahreini et al (2012) for SOA formation in the Los Angeles, CA, urban plume. There is a need to better quantify the abundance of organic compounds associated with diesel engine exhausts so that we may better understand their role in urban air photochemistry and health.…”

Section: Introductionmentioning

confidence: 77%

Measuring long chain alkanes in diesel engine exhaust by thermal desorption PTR-MS

2014

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Abstract.A method using thermal desorption sampling and analysis by proton transfer reaction mass spectrometry (PTR-MS) to measure long chain alkanes (C 12 -C 18 ) and other larger organics associated with diesel engine exhaust emissions is described. Long chain alkanes undergo dissociative proton transfer reactions forming a series of fragment ions with formula C n H 2n+1 . The PTR-MS is insensitive to nalkanes less than C 8 but displays an increasing sensitivity for larger alkanes. Fragment ion distribution and sensitivity is a function of drift conditions. At 80 Td the most abundant ion fragments from C 10 to C 16 n-alkanes were m/z 57, 71 and 85. The mass spectrum of gasoline and diesel fuel at 80 Td displayed ion group patterns that can be related to known fuel constituents, such as alkanes, alkylbenzenes and cycloalkanes, and other compound groups that are inferred from molecular weight distributions such as dihydronapthalenes and naphthenic monoaromatics. It is shown that thermal desorption sampling of gasoline and diesel engine exhausts at 80 Td allows for discrimination against volatile organic compounds, allowing for quantification of long chain alkanes from the abundance of C n H 2n+1 fragment ions. The total abundance of long chain alkanes in diesel engine exhaust was measured to be similar to the total abundance of C 1 -C 4 alkylbenzene compounds. The abundance patterns of compounds determined by thermal desorption sampling may allow for emission profiles to be developed to better quantify the relative contributions of diesel and gasoline exhaust emissions on organic compounds concentrations in urban air.

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“…After propagation of error, these slopes correspond to a ratio of 1.1(±0.1) for weekdays to weekends. Following the estimation method described by Bahreini et al [2012], and using a 44% decrease in diesel traffic on Sundays as determined above, this ratio corresponds to diesel emissions accounting for 19(+17/À21)% of the OOA mass. Also, a consistently higher photochemical age is observed on Sunday versus weekdays due to the higher oxidant concentrations resulting from reduced NO x emissions.…”

Section: Correlation Of Oxygenated Organic Aerosols With the Photochementioning

confidence: 99%

Organic aerosol composition and sources in Pasadena, California, during the 2010 CalNex campaign

et al. 2013

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Organic aerosols (OA) in Pasadena are characterized using multiple measurements from the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign. Five OA components are identified using positive matrix factorization including hydrocarbon‐like OA (HOA) and two types of oxygenated OA (OOA). The Pasadena OA elemental composition when plotted as H : C versus O : C follows a line less steep than that observed for Riverside, CA. The OOA components from both locations follow a common line, however, indicating similar secondary organic aerosol (SOA) oxidation chemistry at the two sites such as fragmentation reactions leading to acid formation. In addition to the similar evolution of elemental composition, the dependence of SOA concentration on photochemical age displays quantitatively the same trends across several North American urban sites. First, the OA/ΔCO values for Pasadena increase with photochemical age exhibiting a slope identical to or slightly higher than those for Mexico City and the northeastern United States. Second, the ratios of OOA to odd‐oxygen (a photochemical oxidation marker) for Pasadena, Mexico City, and Riverside are similar, suggesting a proportional relationship between SOA and odd‐oxygen formation rates. Weekly cycles of the OA components are examined as well. HOA exhibits lower concentrations on Sundays versus weekdays, and the decrease in HOA matches that predicted for primary vehicle emissions using fuel sales data, traffic counts, and vehicle emission ratios. OOA does not display a weekly cycle—after accounting for differences in photochemical aging —which suggests the dominance of gasoline emissions in SOA formation under the assumption that most urban SOA precursors are from motor vehicles.

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Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass

Cited by 210 publications

References 56 publications

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

Unspeciated organic emissions from combustion sources and their influence on the secondary organic aerosol budget in the United States

Measuring long chain alkanes in diesel engine exhaust by thermal desorption PTR-MS

Organic aerosol composition and sources in Pasadena, California, during the 2010 CalNex campaign

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