Secondary organic aerosol formation from idling gasoline passenger vehicle emissions investigated in a smog chamber

Gasoline vehicles have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA for- mation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from three passenger vehicles (EURO2-EURO4) were investigated with photo-oxidation experiments in a 6 m 3 smog chamber. The experiments were carried out down to at- mospherically relevant organic aerosol mass concentrations. The characterization instruments included a high-resolution aerosol mass spectrometer and a proton transfer mass spec- trometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the or- ganic aerosol mass spectra downwind of urban areas. After a cumulative OH exposure of 5◊ 10 6 cm 3 h, the formed SOA was 1-2 orders of magnitude higher than the primary OA emissions. The SOA mass spectrum from a relevant mix- ture of traditional light aromatic precursors gave f43 (mass fraction at m/z = 43), approximately two times higher than to the gasoline SOA. However O : C and H : C ratios were similar for the two cases. Classical C6-C9 light aromatic precursors were responsible for up to 60 % of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher- order aromatic compounds such as C10 and C11 light aro- matics, naphthalene and methyl-naphthalenes. We conclude that approaches using only light aromatic precursors give an incomplete picture of the magnitude of SOA formation and the SOA composition from gasoline exhaust.

[1]  A. Vicet,et al.  Effects of low temperature on the cold start gaseous emissions from light duty vehicles fuelled by ethanol-blended gasoline , 2013 .

[2]  U. Baltensperger,et al.  Secondary organic aerosol formation from gasoline vehicle emissions in a new mobile environmental reaction chamber , 2012 .

[3]  Timothy R. Dallmann,et al.  Elucidating secondary organic aerosol from diesel and gasoline vehicles through detailed characterization of organic carbon emissions , 2012, Proceedings of the National Academy of Sciences.

[4]  A. Middlebrook,et al.  Gasoline emissions dominate over diesel in formation of secondary organic aerosol mass , 2012 .

[5]  Edward Charles Fortner,et al.  Soot Particle Aerosol Mass Spectrometer: Development, Validation, and Initial Application , 2012 .

[6]  P. DeCarlo,et al.  OH clock determination by proton transfer reaction mass spectrometry at an environmental chamber , 2011 .

[7]  John H. Seinfeld,et al.  Elemental composition and oxidation of chamber organic aerosol , 2011 .

[8]  Jared D. Smith,et al.  Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol. , 2011, Nature chemistry.

[9]  P. DeCarlo,et al.  Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments , 2010 .

[10]  A. Robinson,et al.  Secondary aerosol formation from photochemical aging of aircraft exhaust in a smog chamber , 2010 .

[11]  I. Schifter,et al.  Cold‐start and chemical characterization of emissions from mobile sources in Mexico , 2010, Environmental technology.

[12]  A. Arneth,et al.  Development and evaluation of the aerosol dynamics and gas phase chemistry model ADCHEM , 2010 .

[13]  Miroslaw L. Wyszynski,et al.  Vapour-phase and particulate-bound PAHs profile generated by a (SI/HCCI) engine from a winter grade commercial gasoline fuel , 2010 .

[14]  Giorgio Martini,et al.  Hydrocarbon emission fingerprints from contemporary vehicle/engine technologies with conventional and new fuels , 2010 .

[15]  John H. Seinfeld,et al.  Organic aerosol components observed in Northern Hemispheric datasets from Aerosol Mass Spectrometry , 2010 .

[16]  Kei Sato,et al.  Mass spectrometric study of secondary organic aerosol formed from the photo-oxidation of aromatic hydrocarbons , 2010 .

[17]  B. Lamb,et al.  Comparison of Aromatic Hydrocarbon Measurements made by PTR-MS, DOAS and GC-FID during the MCMA 2003 Field Experiment , 2010 .

[18]  A. Robinson,et al.  Photo-oxidation of low-volatility organics found in motor vehicle emissions: production and chemical evolution of organic aerosol mass. , 2010, Environmental science & technology.

[19]  R. Vautard,et al.  Atmospheric composition change – global and regional air quality , 2009 .

[20]  J. D. de Gouw,et al.  Organic aerosols in the Earth's atmosphere. , 2009, Environmental science & technology.

[21]  B. Zielińska,et al.  Secondary organic aerosol production from modern diesel engine emissions , 2010 .

[22]  John H. Seinfeld,et al.  The formation, properties and impact of secondary organic aerosol: current and emerging issues , 2009 .

[23]  John H. Seinfeld,et al.  Secondary organic aerosol formation from photooxidation of naphthalene and alkylnaphthalenes: implications for oxidation of intermediate volatility organic compounds (IVOCs) , 2009 .

[24]  S. Pandis,et al.  High formation of secondary organic aerosol from the photo-oxidation of toluene , 2009 .

[25]  M. Weilenmann,et al.  Cold-start emissions of modern passenger cars at different low ambient temperatures and their evolution over vehicle legislation categories , 2009 .

[26]  R. Harley,et al.  Trends in on-road vehicle emissions of ammonia , 2009 .

[27]  E. Swietlicki,et al.  Chemical composition and mass emission factors of candle smoke particles , 2009 .

[28]  H. Hakola,et al.  Atmospheric Chemistry and Physics Technical Note: Quantitative Long-term Measurements of Voc Concentrations by Ptr-ms – Measurement, Calibration, and Volume Mixing Ratio Calculation Methods , 2022 .

[29]  A. Robinson,et al.  Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 2: analysis of aerosol mass spectrometer data , 2008 .

[30]  P. Mcmurry,et al.  Variability in morphology, hygroscopicity, and optical properties of soot aerosols during atmospheric processing , 2008, Proceedings of the National Academy of Sciences.

[31]  Qi Zhang,et al.  O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry. , 2008, Environmental science & technology.

[32]  J. A. de Gouw,et al.  summer: 1. Direct emissions and secondary formation of organic matter in urban plumes , 2008 .

[33]  T. Sandström,et al.  Deposition of biomass combustion aerosol particles in the human respiratory tract. , 2008, Inhalation toxicology.

[34]  P. Mcmurry,et al.  Processing of Soot by Controlled Sulphuric Acid and Water Condensation—Mass and Mobility Relationship , 2009 .

[35]  S. Reimann,et al.  Measurements of OVOCs and NMHCs in a Swiss highway tunnel for estimation of road transport emissions. , 2007, Environmental science & technology.

[36]  D. Cocker,et al.  Impact of propene on secondary organic aerosol formation from m-xylene. , 2007, Environmental science & technology.

[37]  Allen L Robinson,et al.  Organic aerosol formation from photochemical oxidation of diesel exhaust in a smog chamber. , 2007, Environmental science & technology.

[38]  John H. Seinfeld,et al.  Secondary organic aerosol formation from m-xylene, toluene, and benzene , 2007 .

[39]  Allen L Robinson,et al.  Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging , 2007, Science.

[40]  J. D. de Gouw,et al.  Measurements of volatile organic compounds in the earth's atmosphere using proton-transfer-reaction mass spectrometry. , 2007, Mass spectrometry reviews.

[41]  P. Lienemann,et al.  Three-way-catalyst induced benzene formation: A precursor study , 2007 .

[42]  T S Nawrot,et al.  Stronger associations between daily mortality and fine particulate air pollution in summer than in winter: evidence from a heavily polluted region in western Europe , 2007, Journal of Epidemiology and Community Health.

[43]  Katrin Fuhrer,et al.  Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. , 2006, Analytical chemistry.

[44]  P. Hug,et al.  Three-way catalyst-induced formation of ammonia : velocity- and acceleration-dependent emission factors , 2006 .

[45]  John T. Pisano,et al.  A new environmental chamber for evaluation of gas-phase chemical mechanisms and secondary aerosol formation , 2005 .

[46]  Albert A Presto,et al.  Secondary organic aerosol production from terpene ozonolysis. 1. Effect of UV radiation. , 2005, Environmental science & technology.

[47]  David R Cocker,et al.  Impact of the hydrocarbon to NOx ratio on secondary organic aerosol formation. , 2005, Environmental science & technology.

[48]  Ernest Weingartner,et al.  Secondary organic aerosol formation by irradiation of 1,3,5-trimethylbenzene-NOx-H2O in a new reaction chamber for atmospheric chemistry and physics. , 2005, Environmental science & technology.

[49]  Michel Gerboles,et al.  Assessment of uncertainty of NO2 measurements by the chemiluminescence method and discussion of the quality objective of the NO2 European Directive. , 2003, Journal of environmental monitoring : JEM.

[50]  Michael J Kleeman,et al.  Measurement of emissions from air pollution sources. 5. C1-C32 organic compounds from gasoline-powered motor vehicles. , 2002, Environmental science & technology.

[51]  W. Weathers,et al.  Secondary Organic Aerosol Formation from the Irradiation of Simulated Automobile Exhaust , 2002, Journal of the Air & Waste Management Association.

[52]  David R. Cocker,et al.  The effect of water on gas-particle partitioning of secondary organic aerosol: II. m-xylene and 1,3,5-trimethylbenzene photooxidation systems , 2001 .

[53]  R. Harley,et al.  On-road measurement of fine particle and nitrogen oxide emissions from light- and heavy-duty motor vehicles , 1999 .

[54]  A. Hansel,et al.  On-line monitoring of volatile organic compounds at pptv levels by means of proton-transfer-reaction mass spectrometry (PTR-MS) medical applications, food control and environmental research , 1998 .

[55]  John H. Seinfeld,et al.  Aromatics, Reformulated Gasoline, and Atmospheric Organic Aerosol Formation , 1997 .

[56]  Daniel J. Rader,et al.  Aerosol Wall Losses in Electrically Charged Chambers , 1985 .

[57]  C H E N S O N G,et al.  Impact of the Hydrocarbon to NO x Ratio on Secondary Organic Aerosol Formation , 2022 .