Organic Aerosol Formation Downwind from the Deepwater Horizon Oil Spill

Gouw, J. A. de; Middlebrook, A. M.; Warneke, C.; Ahmadov, Ravan; Atlas, Elliot L.; Bahreini, R.; Blake, Donald R.; Brock, C. A.; Brioude, J.; Fahey, D. W.; Fehsenfeld, F. C.; Holloway, J. S.; Hénaff, Matthieu Le; Lueb, R.; McKeen, S. A.; Meagher, James F.; Murphy, D. M.; Paris, Claire B.; Parrish, D. D.; Perring, A. E.; Pollack, I. B.; Ravishankara, A. R.; Robinson, Allen L.; Ryerson, Thomas B.; Schwarz, J. P.; Spackman, J. R.; Srinivasan, Ashwanth; Watts, L. A.

doi:10.1126/science.1200320

Cited by 173 publications

(168 citation statements)

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“…It should also be noted that as the most volatile species in this study, HOA could be evaporated easily and thus have a larger potential to experience the "evaporation -oxidation in gas phase -condensation" process and then form SOA since previous studies showed that semi-volatile hydrocarbons from diesel exhaust (Robinson et al, 2007) and crude oil (de Gouw et al, 2011) can be easily oxidized in the gas phase to form less-volatile SOA. Huang et al (2012) also pointed out that HOA could be oxidized to SOA based on the analysis of their diurnal variations.…”

Section: Source Apportionmentmentioning

confidence: 99%

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

Cao

Huang

et al. 2018

Atmos. Chem. Phys.

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Abstract. Aerosol pollution has been a very serious environmental problem in China for many years. The volatility of aerosols can affect the distribution of compounds in the gas and aerosol phases, the atmospheric fates of the corresponding components, and the measurement of the concentration of aerosols. Compared to the characterization of chemical composition, few studies have focused on the volatility of aerosols in China. In this study, a thermodenuder aerosol mass spectrometer (TD-AMS) system was deployed to study the volatility of non-refractory submicron particulate matter (PM 1 ) species during winter in Shenzhen. To our knowledge, this paper is the first report of the volatilities of aerosol chemical components based on a TD-AMS system in China. The average PM 1 mass concentration during the experiment was 42.7±20.1 µg m −3 , with organic aerosol (OA) being the most abundant component (43.2 % of the total mass). The volatility of chemical species measured by the AMS varied, with nitrate showing the highest volatility, with a mass fraction remaining (MFR) of 0.57 at 50 • C. Organics showed semivolatile characteristics (the MFR was 0.88 at 50 • C), and the volatility had a relatively linear correlation with the TD temperature (from the ambient temperature to 200 • C), with an evaporation rate of 0.45 % • C −1 . Five subtypes of OA were resolved from total OA using positive matrix factorization (PMF) for data obtained under both ambient temperature and high temperatures through the TD, including a hydrocarbonlike OA (HOA, accounting for 13.5 %), a cooking OA (COA, 20.6 %), a biomass-burning OA (BBOA, 8.9 %), and two oxygenated OAs (OOAs): a less-oxidized OOA (LO-OOA, 39.1 %) and a more-oxidized OOA (MO-OOA, 17.9 %). Different OA factors presented different volatilities, and the volatility sequence of the OA factors at 50 • C was HOA (MFR of 0.56) > LO-OOA (0.70) > COA (0.85) ≈ BBOA (0.87) > MO-OOA (0.99), which was not completely consistent with the sequence of their O / C ratios. The high volatility of HOA implied that it had a high potential to be oxidized to secondary species in the gas phase. The aerosol volatility measurement results in this study provide useful parameters for the modeling work of aerosol evolution in China and are also helpful in understanding the formation mechanisms of secondary aerosols.

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Section: Source Apportionmentmentioning

confidence: 99%

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

Cao

Huang

et al. 2018

Atmos. Chem. Phys.

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“…For instance, gasoline vehicles emit 9-15 times or even 2 orders of magnitude higher secondary organic particulate matter than primary organic particle mass (Karjalainen et al, 2016;Nordin et al, 2013;Platt et al, 2013;Tkacik et al, 2014). Indeed, Bahreini et al (2012) found that secondary organic aerosol originating from gasoline engines forms the majority of the SOA in and downwind of large metropolitan areas. From diesel vehicles without a particle filter, the SOA mass formation potential is of the same magnitude as or lower than the primary particle mass emission Gordon et al, 2014b;.…”

Section: Introductionmentioning

confidence: 99%

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

et al. 2017

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Abstract. Natural gas usage in the traffic and energy production sectors is a growing trend worldwide; thus, an assessment of its effects on air quality, human health and climate is required. Engine exhaust is a source of primary particulate emissions and secondary aerosol precursors, which both contribute to air quality and can cause adverse health effects. Technologies, such as cleaner engines or fuels, that produce less primary and secondary aerosols could potentially significantly decrease atmospheric particle concentrations and their adverse effects. In this study, we used a potential aerosol mass (PAM) chamber to investigate the secondary aerosol formation potential of natural gas engine exhaust. The PAM chamber was used with a constant UV-light voltage, which resulted in relatively long equivalent atmospheric ages of 11 days at most. The studied retro-fitted natural gas engine exhaust was observed to form secondary aerosol. The mass of the total aged particles, i.e., particle mass measured downstream of the PAM chamber, was 6-268 times as high as the mass of the emitted primary exhaust particles. The secondary organic aerosol (SOA) formation potential was measured to be 9-20 mg kg −1 fuel . The total aged particles mainly consisted of organic matter, nitrate, sulfate and ammonium, with the fractions depending on exhaust after-treatment and the engine parameters used. Also, the volatility, composition and concentration of the total aged particles were found to depend on the engine operating mode, catalyst temperature and catalyst type. For example, a high catalyst temperature promoted the formation of sulfate particles, whereas a low catalyst temperature promoted nitrate formation. However, in particular, the concentration of nitrate needed a long time to stabilize -more than half an hour -which complicated the conclusions but also indicates the sensitivity of nitrate measurements on experimental parameters such as emission source and system temperatures. Sulfate was measured to have the highest evaporation temperature, and nitrate had the lowest. The evaporation temperature of ammonium depended on the fractions of nitrate and sulfate in the particles. The average volatility of the total aged particles was measured to be lower than that of primary particles, indicating better stability of the aged natural gas engine-emitted aerosol in the atmosphere. According to the results of this study, the exhaust of a natural gas engine equipped with a catalyst forms secondary aerosol when the atmospheric ages in a PAM chamber are several days long. The secondary aerosol matter has different physical characteristics from those of primary particulate emissions.

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“…The underestimation of SOA has been studied by many researchers. The existing models do not include certain precursors, such as semi-volatile organic compounds (SVOCs) and intermediate-volatility organic compounds (IVOCs) (Goldstein and Galbally, 2007;Robinson et al, 2007;de Gouw et al, 2011). Additionally, the existing precursors used in these models may lead to the underestimation of SOA (Tsimpidi et al, 2010), and the definitions of SOA and POA can vary (Cheng et al, 2011).…”

Section: Introductionmentioning

confidence: 99%

The Construction and Application of a Multipoint Sampling System for Vehicle Exhaust Plumes

Shen

Yao

et al. 2017

Aerosol Air Qual. Res.

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To study the formation process of secondary organic aerosols (SOA) in a vehicle exhaust plume near the exhaust gas discharge outlet, a new multipoint sampling system was established. The system has five sampling heads and includes a particulate matter multi-channel film sampling system, a CO 2 /CO analyzer system, a volatile organic compound (VOC) sampling system, a particulate matter real-time analyzer system, and sensor interfaces. The vehicle exhaust near the exhaust nozzle can be sampled at multiple locations simultaneously using the new multipoint sampling system. Additionally, the system can be used to measure and analyze variations in the fine particulate matter, including the carbonaceous and ionic components, and organic compounds in the plume near the exhaust nozzle. This paper introduces the construction and application of the multipoint sampling system. The motor vehicle exhaust multipoint sampling system is reliable and can accurately capture the characteristics of the exhaust plume near the discharge outlet area. Changes in the CO 2 concentration were used to determine whether exhaust was accurately collected at the sampling points. The relationship between the dilution rate and distance was calculated on the basis of on-road test results using the following equation: DR = 21.4X 1.16 . This equation can be used for modeling purposes, especially in comparisons of model results and observations and in the evaluation of dispersion models.

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Organic Aerosol Formation Downwind from the Deepwater Horizon Oil Spill

Cited by 173 publications

References 19 publications

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

Volatility measurement of atmospheric submicron aerosols in an urban atmosphere in southern China

Comparison of primary and secondary particle formation from natural gas engine exhaust and of their volatility characteristics

The Construction and Application of a Multipoint Sampling System for Vehicle Exhaust Plumes

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