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Sample records for exhaust aerosol formation

  1. Aircraft exhaust aerosol formation and growth

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    Brown, R.C.; Miake-Lye, R.C.; Anderson, M.R.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

    1997-12-31

    Aerosol formation and growth in the exhaust plume of the ATTAS aircraft at an altitude of approximately 9 km, burning fuels with 2 ppmm sulfur (`low`) and 266 ppmm (`high`) sulfur has been modeled using an aerosol dynamics model for nucleation, vapor condensation and coagulation, coupled to a 2-dimensional, axisymmetric flow code to treat plume dilution and turbulent mixing. For both the `low` and `high` sulfur fuels, approximately 60% of the available water had condensed within the first 200 m downstream of the exhaust exit. The contrail particle diameters ranged between 0.4 to 1.6 {mu}m. However, the size distributions as a function of radial position for the `low` sulfur plume were broader than the corresponding distributions for the `high` sulfur plume. The model results indicate for a fuel sulfur mass loading of 2 ppmm, sulfuric acid remains a viable activating agent and that the differences in the contrail particle size distributions for sulfur mass loadings between 2 ppmm and 260 ppmm would be difficult to detect. (author) 12 refs.

  2. Computational Studies of Aerosol Growth, Formation and Measurement in Diesel Exhaust

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    Lemmetty, M.

    2008-07-01

    Epidemiological studies have shown a correlation between exposure to diesel exhaust aerosols and health problems. As diesel vehicles are widely used in traffic, and they are the most important contributor to the traffic aerosol emissions, the diesel aerosols from on-road engines constitute an important subject for aerosol research. The diesel aerosol from an on-road vehicle engine consists of two externally mixed modes with clearly different chemical compositions. The soot mode consists of carbonaceous, fractal-like particles with a diameter of 30-200 nm, while the nucleation mode is mostly volatile, and has a geometric median diameter of 5-30 nm. The emissions from mobile or stationary diesel power plants using medium or heavy fuel oil, which may have a considerable coarse mode and significantly different chemical charcteristics, are outside the scope of this study. In recent years, the interest into the nucleation mode has been steadily growing, as it seems that the appearance of this particle mode is promoted by some modern vehicle technologies. Unlike soot mode, which is formed mainly during combustion, the nucleation mode experiences significant changes or is even formed during the dilution of the exhaust after the exit from the tailpipe. In this thesis, computational methods are developed for the study of the nucleation mode in diesel exhaust. To improve the possibilities of the real-time measurement of the diesel exhaust, data reduction methodology of the Electrical Low-Pressure Impactor (ELPI) is developed, and a Bayesian algorithm is proposed for this purpose. The other objective of this thesis is the study of the growth and formation of the diesel exhaust nucleation mode during sampling and dilution. Tampere University of Technology Exhaust Aerosol Model (TUTEAM) and a simple, semi-empirical flow model are introduced to further this objective. In addition, we study the nucleation processes in diesel exhaust using classical nucleation theory for H{sub 2}SO

  3. Effect of Pellet Boiler Exhaust on Secondary Organic Aerosol Formation from α-Pinene.

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    Kari, Eetu; Hao, Liqing; Yli-Pirilä, Pasi; Leskinen, Ari; Kortelainen, Miika; Grigonyte, Julija; Worsnop, Douglas R; Jokiniemi, Jorma; Sippula, Olli; Faiola, Celia L; Virtanen, Annele

    2017-02-07

    Interactions between anthropogenic and biogenic emissions, and implications for aerosol production, have raised particular scientific interest. Despite active research in this area, real anthropogenic emission sources have not been exploited for anthropogenic-biogenic interaction studies until now. This work examines these interactions using α-pinene and pellet boiler emissions as a model test system. The impact of pellet boiler emissions on secondary organic aerosol (SOA) formation from α-pinene photo-oxidation was studied under atmospherically relevant conditions in an environmental chamber. The aim of this study was to identify which of the major pellet exhaust components (including high nitrogen oxide (NOx), primary particles, or a combination of the two) affected SOA formation from α-pinene. Results demonstrated that high NOx concentrations emitted by the pellet boiler reduced SOA yields from α-pinene, whereas the chemical properties of the primary particles emitted by the pellet boiler had no effect on observed SOA yields. The maximum SOA yield of α-pinene in the presence of pellet boiler exhaust (under high-NOx conditions) was 18.7% and in the absence of pellet boiler exhaust (under low-NOx conditions) was 34.1%. The reduced SOA yield under high-NOx conditions was caused by changes in gas-phase chemistry that led to the formation of organonitrate compounds.

  4. Formation of secondary aerosols from gasoline vehicle exhaust when mixing with SO2

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    T. Liu

    2016-01-01

    Full Text Available Sulfur dioxide (SO2 can enhance the formation of secondary aerosols from biogenic volatile organic compounds (VOCs, but its influence on secondary aerosol formation from anthropogenic VOCs, particularly complex mixtures like vehicle exhaust, remains uncertain. Gasoline vehicle exhaust (GVE and SO2, a typical pollutant from coal burning, are directly co-introduced into a smog chamber, in this study, to investigate the formation of secondary organic aerosols (SOA and sulfate aerosols through photooxidation. New particle formation was enhanced, while substantial sulfate was formed through the oxidation of SO2 in the presence of high concentration of SO2. Homogenous oxidation by OH radicals contributed a negligible fraction to the conversion of SO2 to sulfate, and instead the oxidation by stabilized Criegee intermediates (sCIs, formed from alkenes in the exhaust reacting with ozone, dominated the conversion of SO2. After 5 h of photochemical aging, GVE's SOA production factor revealed an increase by 60–200 % in the presence of high concentration of SO2. The increase could principally be attributed to acid-catalyzed SOA formation as evidenced by the strong positive linear correlation (R2 = 0.97 between the SOA production factor and in situ particle acidity calculated by the AIM-II model. A high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS resolved OA's relatively lower oxygen-to-carbon (O : C (0.44 ± 0.02 and higher hydrogen-to-carbon (H : C (1.40 ± 0.03 molar ratios for the GVE / SO2 mixture, with a significantly lower estimated average carbon oxidation state (OSc of −0.51 ± 0.06 than −0.19 ± 0.08 for GVE alone. The relative higher mass loading of OA in the experiments with SO2 might be a significant explanation for the lower SOA oxidation degree.

  5. Fuel composition and secondary organic aerosol formation: gas-turbine exhaust and alternative aviation fuels.

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    Miracolo, Marissa A; Drozd, Greg T; Jathar, Shantanu H; Presto, Albert A; Lipsky, Eric M; Corporan, Edwin; Robinson, Allen L

    2012-08-07

    A series of smog chamber experiments were performed to investigate the effects of fuel composition on secondary particulate matter (PM) formation from dilute exhaust from a T63 gas-turbine engine. Tests were performed at idle and cruise loads with the engine fueled on conventional military jet fuel (JP-8), Fischer-Tropsch synthetic jet fuel (FT), and a 50/50 blend of the two fuels. Emissions were sampled into a portable smog chamber and exposed to sunlight or artificial UV light to initiate photo-oxidation. Similar to previous studies, neat FT fuel and a 50/50 FT/JP-8 blend reduced the primary particulate matter emissions compared to neat JP-8. After only one hour of photo-oxidation at typical atmospheric OH levels, the secondary PM production in dilute exhaust exceeded primary PM emissions, except when operating the engine at high load on FT fuel. Therefore, accounting for secondary PM production should be considered when assessing the contribution of gas-turbine engine emissions to ambient PM levels. FT fuel substantially reduced secondary PM formation in dilute exhaust compared to neat JP-8 at both idle and cruise loads. At idle load, the secondary PM formation was reduced by a factor of 20 with the use of neat FT fuel, and a factor of 2 with the use of the blend fuel. At cruise load, the use of FT fuel resulted in no measured formation of secondary PM. In every experiment, the secondary PM was dominated by organics with minor contributions from sulfate when the engine was operated on JP-8 fuel. At both loads, FT fuel produces less secondary organic aerosol than JP-8 because of differences in the composition of the fuels and the resultant emissions. This work indicates that fuel reformulation may be a viable strategy to reduce the contribution of emissions from combustion systems to secondary organic aerosol production and ultimately ambient PM levels.

  6. Primary particulate emissions and secondary organic aerosol (SOA) formation from idling diesel vehicle exhaust in China.

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    Deng, Wei; Hu, Qihou; Liu, Tengyu; Wang, Xinming; Zhang, Yanli; Song, Wei; Sun, Yele; Bi, Xinhui; Yu, Jianzhen; Yang, Weiqiang; Huang, Xinyu; Zhang, Zhou; Huang, Zhonghui; He, Quanfu; Mellouki, Abdelwahid; George, Christian

    2017-09-01

    In China diesel vehicles dominate the primary emission of particulate matters from on-road vehicles, and they might also contribute substantially to the formation of secondary organic aerosols (SOA). In this study tailpipe exhaust of three typical in-use diesel vehicles under warm idling conditions was introduced directly into an indoor smog chamber with a 30m 3 Teflon reactor to characterize primary emissions and SOA formation during photo-oxidation. The emission factors of primary organic aerosol (POA) and black carbon (BC) for the three types of Chinese diesel vehicles ranged 0.18-0.91 and 0.15-0.51gkg-fuel -1 , respectively; and the SOA production factors ranged 0.50-1.8gkg-fuel -1 and SOA/POA ratios ranged 0.7-3.7 with an average of 2.2. The fuel-based POA emission factors and SOA production factors from this study for idling diesel vehicle exhaust were 1-3 orders of magnitude higher than those reported in previous studies for idling gasoline vehicle exhaust. The emission factors for total particle numbers were 0.65-4.0×10 15 particleskg-fuel -1 , and particles with diameters less than 50nm dominated in total particle numbers. Traditional C 2 -C 12 precursor non-methane hydrocarbons (NMHCs) could only explain less than 3% of the SOA formed during aging and contribution from other precursors including intermediate volatile organic compounds (IVOC) needs further investigation. Copyright © 2017 Elsevier B.V. All rights reserved.

  7. Primary Emission and the Potential of Secondary Aerosol Formation from Chinese Gasoline Engine Exhaust

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    Hu, Min; Peng, Jianfei; Qin, Yanhong; Du, Zhuofei; Li, Mengjin; Zheng, Rong; Zheng, Jing; Shang, Dongjie; Lu, Sihua; Wu, Yusheng; Zeng, Limin; Guo, Song; Shao, Min; Wang, Yinhui; Shuai, Shijin

    2017-04-01

    Along with the urbanization and economic growth, vehicle population in China reached 269 million, ranked the second in the world in 2015. Gasoline vehicle is identified to be the main source for urban PM2.5 in China, accounting for 15%-31%. In this study the impact of fuel components on PM2.5 and volatile organic compounds (VOCs) emissions from a gasoline port fuel injection (PFI) engine and a gasoline direct injection (GDI) engine are discussed. Results show that, higher proportion of aromatics, alkenes or sulfur in gasoline fuel will lead to higher PM emissions. The PM from the PFI engine mainly consists of OC and a small amount of EC and inorganic ions, while the PM discharge from the GDI engine mainly consists of EC, OM and a small amount of inorganic ions. Since the GDI engines can reduce fuel consumption and CO2 emissions, and it would become more and more popular in the near future. The characteristics of POM component, emission factors and source profile were investigated from GDI engine, particularly focused on the effect of engine speed, load and the catalyst, which will be very much helpful for source identification as source indicators. Chamber experiments were conducted to quantify the potential of secondary aerosol formation from exhaust of a PFI gasoline engine and China V gasoline fuel. During 4-5 h simulation, equivalent to10 days of atmospheric photo-oxidation in Beijing, the extreme SOA production was 426 ± 85 mg/kg fuel, with high precursors and OH exposure. 14% of SOA measured in the chamber experiments could be explained through the oxidation of speciated single-ring aromatics. Unspeciated precursors, such as intermediate-volatility organic compounds and semi-volatility organic compounds, might be significant for SOA formation from gasoline VOCs. We concluded that reduction of emissions of aerosol precursor gases from vehicles is essential to mediate pollution in China.

  8. Formation of secondary inorganic aerosols by power plant emissions exhausted through cooling towers in Saxony.

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    Hinneburg, Detlef; Renner, Eberhard; Wolke, Ralf

    2009-01-01

    The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of 'free' sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium-sulfate-nitrate-water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10

  9. Secondary aerosol formation from photochemical aging of aircraft exhaust in a smog chamber

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    M. A. Miracolo

    2011-05-01

    Full Text Available Field experiments were performed to investigate the effects of photo-oxidation on fine particle emissions from an in-use CFM56-2B gas turbine engine mounted on a KC-135 Stratotanker airframe. Emissions were sampled into a portable smog chamber from a rake inlet installed one-meter downstream of the engine exit plane of a parked and chocked aircraft. The chamber was then exposed to sunlight and/or UV lights to initiate photo-oxidation. Separate tests were performed at different engine loads (4, 7, 30, 85 %. Photo-oxidation created substantial secondary particulate matter (PM, greatly exceeding the direct PM emissions at each engine load after an hour or less of aging at typical summertime conditions. After several hours of photo-oxidation, the ratio of secondary-to-primary PM mass was on average 35 ± 4.1, 17 ± 2.5, 60 ± 2.2, and 2.7 ± 1.1 for the 4, 7, 30, and 85 % load experiments, respectively. The composition of secondary PM formed strongly depended on load. At 4 % load, secondary PM was dominated by secondary organic aerosol (SOA. At higher loads, the secondary PM was mainly secondary sulfate. A traditional SOA model that accounts for SOA formation from single-ring aromatics and other volatile organic compounds underpredicts the measured SOA formation by ~60 % at 4 % load and ~40 % at 85 % load. Large amounts of lower-volatiliy organic vapors were measured in the exhaust; they represent a significant pool of SOA precursors that are not included in traditional SOA models. These results underscore the importance of accounting for atmospheric processing when assessing the influence of aircraft emissions on ambient PM levels. Models that do not account for this processing will likely underpredict the contribution of aircraft emissions to local and regional air pollution.

  10. The Formation of Hydrochloric Acid Aerosol from the Interaction of the Space Shuttle Rocket Exhaust with the Atmosphere

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    Rhein, R. A.

    1973-01-01

    A description is given of conditions of atmospheric temperature and relative humidity under which hydrochloric acid aerosol is expected upon interaction of the proposed space shuttle rocket exhaust products with the atmosphere.

  11. Secondary organic aerosol formation from photochemical aging of light-duty gasoline vehicle exhausts in a smog chamber

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    Liu, T.; Wang, X.; Deng, W.; Hu, Q.; Ding, X.; Zhang, Y.; He, Q.; Zhang, Z.; Lü, S.; Bi, X.; Chen, J.; Yu, J.

    2015-08-01

    In China, a rapid increase in passenger vehicles has led to the growing concern of vehicle exhaust as an important source of anthropogenic secondary organic aerosol (SOA) in megacities hard hit by haze. In this study, the SOA formation of emissions from two idling light-duty gasoline vehicles (LDGVs) (Euro 1 and Euro 4) operated in China was investigated in a 30 m3 smog chamber. Five photo-oxidation experiments were carried out at 25 °C with relative humidity at around 50 %. After aging at an OH exposure of 5 × 106 molecules cm-3 h, the formed SOA was 12-259 times as high as primary organic aerosol (POA). The SOA production factors (PF) were 0.001-0.044 g kg-1 fuel, comparable with those from the previous studies at comparable OH exposure. This quite lower OH exposure than that in typical atmospheric conditions might however lead to the underestimation of the SOA formation potential from LDGVs. Effective SOA yields in this study were well fit by a one-product gas-particle partitioning model but quite lower than those of a previous study investigating SOA formation from three idling passenger vehicles (Euro 2-4). Traditional single-ring aromatic precursors and naphthalene could explain 51-90 % of the formed SOA. Unspeciated species such as branched and cyclic alkanes might be the possible precursors for the unexplained SOA. A high-resolution time-of-flight aerosol mass spectrometer was used to characterize the chemical composition of SOA. The relationship between f43 (ratio of m/z 43, mostly C2H3O+, to the total signal in mass spectrum) and f44 (mostly CO2+) of the gasoline vehicle exhaust SOA is similar to the ambient semi-volatile oxygenated organic aerosol (SV-OOA). We plot the O : C and H : C molar ratios of SOA in a Van Krevelen diagram. The slopes of ΔH : C / ΔO : C ranged from -0.59 to -0.36, suggesting that the oxidation chemistry in these experiments was a combination of carboxylic acid and alcohol/peroxide formation.

  12. Modeling the formation and properties of traditional and non-traditional secondary organic aerosol: problem formulation and application to aircraft exhaust

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    S. H. Jathar

    2012-10-01

    Full Text Available We present a methodology to model secondary organic aerosol (SOA formation from the photo-oxidation of unspeciated low-volatility organics (semi-volatile and intermediate volatile organic compounds emitted by combustion systems. It is formulated using the volatility basis-set approach. Unspeciated low-volatility organics are classified by volatility and then allowed to react with the hydroxyl radical. The new methodology allows for larger reductions in volatility with each oxidation step than previous volatility basis set models, which is more consistent with the addition of common functional groups and similar to those used by traditional SOA models. The methodology is illustrated using data collected during two field campaigns that characterized the atmospheric evolution of dilute gas-turbine engine emissions using a smog chamber. In those experiments, photo-oxidation formed a significant amount of SOA, much of which could not be explained based on the emissions of traditional speciated precursors; we refer to the unexplained SOA as non-traditional SOA (NT-SOA. The NT-SOA can be explained by emissions of unspeciated low-volatility organics measured using sorbents. We show that the parameterization proposed by Robinson et al. (2007 is unable to explain the timing of the NT-SOA formation in the aircraft experiments because it assumes a very modest reduction in volatility of the precursors with every oxidation reaction. In contrast the new method better reproduces the NT-SOA formation. The NT-SOA yields estimated for the unspeciated low-volatility organic emissions in aircraft exhaust are similar to literature data for large n-alkanes and other low-volatility organics. The estimated yields vary with fuel composition (Jet Propellent-8 versus Fischer-Tropsch and engine load (ground idle versus non-ground idle. The framework developed here is suitable for modeling SOA formation from emissions from other combustion systems.

  13. Modeling the Formation and Composition of Secondary Organic Aerosol from Diesel Exhaust Using Parameterized and Semi-Explicit Chemistry and Thermodynamic Models

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    Eluri, Sailaja

    Laboratory-based studies have shown that diesel-powered sources emit volatile organic compounds that can be photo-oxidized in the atmosphere to form secondary organic aerosol (SOA); in some cases, this SOA can exceed direct emissions of particulate matter (PM); PM is a criteria pollutant that is known to have adverse effects on air quality, climate, and human health. However, there are open questions surrounding how these laboratory experiments can be extrapolated to the real atmosphere and how they will help identify the most important species in diesel exhaust that contribute to SOA formation. Jathar et al. (2017) recently performed experiments using an oxidation flow reactor (OFR) to measure the photochemical production of SOA from a diesel engine operated at two different engine loads (idle, load), two fuel types (diesel, biodiesel) and two aftertreatment configurations (with and without an oxidation catalyst and particle filter). In this work, we will use two different SOA models, namely the volatility basis set (VBS) model and the statistical oxidation model (SOM), to simulate the formation, evolution and composition of SOA from the experiments of Jathar et al. (2017). Leveraging recent laboratory-based parameterizations, both frameworks accounted for a semi-volatile and reactive POA, SOA production from semi-volatile, intermediate-volatility and volatile organic compounds (SVOC, IVOC and VOC), NOx-dependent multigenerational gas-phase chemistry, and kinetic gas/particle partitioning. Both frameworks demonstrated that for model predictions of SOA mass and elemental composition to agree with measurements across all engine load-fuel-aftertreatment combinations, it was necessary to (a) model the kinetically-limited gas/particle partitioning likely in OFRs and (b) account for SOA formation from IVOCs (IVOCs were found to account for more than four-fifths of the model-predicted SOA). Model predictions of the gas-phase organic compounds (resolved in carbon and

  14. Modelling aerosol number distributions from a vehicle exhaust with an aerosol CFD model

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    Albriet, B.; Sartelet, K. N.; Lacour, S.; Carissimo, B.; Seigneur, C.

    2010-03-01

    Vehicular traffic contributes significantly to the aerosol number concentrations at the local scale by emitting primary soot particles and forming secondary nucleated nanoparticles. Because of their potential health effects, more attention is paid to the traffic induced aerosol number distributions. The aim of this work is to explain the phenomenology leading to the formation and the evolution of the aerosol number distributions in the vicinity of a vehicle exhaust using numerical modelling. The emissions are representative of those of a light-duty diesel truck without a diesel particle filter. The atmospheric flow is modelled with a computational fluid dynamics (CFD) code to describe the dispersion of pollutants at the local scale. The CFD code, coupled to a modal aerosol model (MAM) describing the aerosol dynamics, is used to model the tailpipe plume of a vehicle with emissions corresponding to urban driving conditions. On the basis of available measurements in Schauer et al. (1999), three surrogate species are chosen to treat the semi-volatile organic compounds in the emissions. The model simulates the formation of the aerosol distribution in the exhaust plume of a vehicle as follows. After emission to the atmosphere, particles are formed by nucleation of sulphuric acid and water vapour depending strongly on the thermodynamic state of the atmosphere and on the dilution conditions. The semi-volatile organic compounds are critical for the rapid growth of nanoparticles through condensation. The semi-volatile organic compounds are also important for the evolution of primary soot particles and can contribute substantially to their chemical composition. The most influential parameters for particle formation are the sulphur fuel content, the semi-volatile organic emissions and also the mass and initial diameter of the soot particles emitted. The model is able to take into account the complex competition between nucleation, condensation and dilution, as well as the

  15. Hydrochloric acid aerosol and gaseous hydrogen chloride partitioning in a cloud contaminated by solid rocket exhaust

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    Sebacher, D. I.; Bendura, R. J.; Wornom, D. E.

    1980-01-01

    Partitioning of hydrogen chloride between hydrochloric acid aerosol and gaseous HCl in the lower atmosphere was experimentally investigated in a solid rocket exhaust cloud diluted with humid ambient air. Airborne measurements were obtained of gaseous HCl, total HCl, relative humidity and temperature to evaluate the conditions under which aerosol formation occurs in the troposphere in the presence of hygroscopic HCl vapor. Equilibrium predictions of HCl aerosol formation accurately predict the measured HCl partitioning over a range of total HCl concentrations from 0.6 to 16 ppm.

  16. Sampling and measurement methods for diesel exhaust aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Ristimaeki, J.

    2006-07-01

    Awareness of adverse health effects of urban aerosols has increased general interest in aerosol sources. As diesel engines are one significant urban anthropogenic particle source, diesel aerosols have been under intense research during the last decades. This thesis discusses the measurement issues related to the diesel exhaust particles, focusing on the effective density measurement with Elpi-Sumps and Tda-Elpi methods and presents some additional performance issues not discussed in the papers. As the emergence of volatile nanoparticles in the diesel exhaust is sensitive to prevailing circumstances there is a need to properly control the dilution parameters in laboratory measurements in order to obtain repeatable and reproducible results. In addition to the dilution parameters, the effect of ambient temperature on the light duty vehicle exhaust particulate emission was studied. It was found that turbo charged diesel engines were relatively insensitive to changes in ambient temperature whereas particle emissions from naturally aspirated gasoline vehicles were significantly increased at low temperatures. The measurement of effective density and mass of aerosol particles with Dma and impactor was studied and applied to characterisation of diesel exhaust particles. The Tda-Elpi method was used for determination of the volatile mass of diesel exhaust particles as a function of particle size. Based on the measurement results, condensation was suggested to be the main phenomena driving volatile mass transfer to the exhaust particles. Identification of the process and the separation of volatile and solid mass may become important as some health effect studies suggest the volatile fraction to be a key component causing the biological effects of diesel exhaust particles. (orig.)

  17. Effect of aircraft exhaust sulfur emissions on near field plume aerosols

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    Brown, R.C.; Miake-Lye, R.C.; Anderson, M.R.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics

    1997-12-31

    Based on estimated exit plane sulfur speciation, a two dimensional, axisymmetric flow field model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the engine on the formation and growth of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols in the near field plume. The conversion of fuel sulfur to sulfur trioxide and sulfuric acid in the engine is predicted to significantly increase the number density and surface area density of volatile H{sub 2}SO{sub 4}/H{sub 2}O aerosols and the chemical activation of exhaust soot particulates. This analysis indicates the need for experimental measurements of exhaust SO{sub x} emissions to fully assess the atmospheric impact of aircraft emissions. (author) 18 refs.; Submitted to Geophysical Research Letters

  18. Effect of aircraft exhaust sulfur emissions on near field plume aerosols

    Science.gov (United States)

    Brown, R. C.; Miake-Lye, R. C.; Anderson, M. R.; Kolb, C. E.

    A two dimensional, axisymmetric flowfield model with coupled gas phase oxidation kinetics and aerosol nucleation and growth dynamics is used to evaluate the effect of fuel sulfur oxidation in the Concorde engine on the formation and growth of volatile H2SO4/H2O aerosols in the near field plume. Rased on estimated exit plane sulfur speciation, results are shown for between 2% and 20% conversion of the fuel sulfur to S(VI) (SO3 and H2SO4) in engine. The primary motivation is to provide estimates for the changes in the number density and surface area density of sulfuric acid aerosols due to sulfur oxidation in the engine. This analysis indicates the need for experimental measurements of sulfur emissions at the exhaust exit, in addition to soot properties, to fully assess the atmospheric impact of aircraft emissions.

  19. The role of sulfur emission in volatile particle formation in jet aircraft exhaust plumes

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    Kärcher, B.; Fahey, D. W.

    Recent in-situ emission measurements of the Concorde in the lower stratosphere point to a surprisingly efficient conversion of fuel sulfur to H2SO4 in the exhaust plume. By means of a comprehensive model, the formation and evolution of aerosol particles and precursors are calculated in the diluting aircraft wake. The results provide strong evidence that high levels of SO3 present in the nascent plume are required to explain the observations of large numbers of nanometer-sized aerosols. Limiting particle formation at emission to keep potential chemical effects on stratospheric ozone small will require control of the sulfur oxidation kinetics during fuel combustion. The similarities between super- and subsonic exhaust plumes suggest that the presence of SO3 in the latter will also be a key limiting factor in new aerosol production.

  20. Model studies of volatile diesel exhaust particle formation: organic vapours involved in nucleation and growth?

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    Pirjola, L.; Karl, M.; Rönkkö, T.; Arnold, F.

    2015-02-01

    High concentration of volatile nucleation mode particles (NUP) formed in the atmosphere during exhaust cools and dilutes have hazardous health effects and impair visibility in urban areas. Nucleation mechanisms in diesel exhaust are only poorly understood. We performed model studies using two sectional aerosol dynamics process models AEROFOR and MAFOR on the formation of particles in the exhaust of a diesel engine, equipped with an oxidative after-treatment system and running with low fuel sulphur content (FSC), under laboratory sampling conditions where the dilution system mimics real-world conditions. Different nucleation mechanisms were tested; based on the measured gaseous sulphuric acid (GSA) and non-volatile core and soot particle number concentrations of the raw exhaust, the model simulations showed that the best agreement between model predictions and measurements in terms of particle number size distribution was obtained by barrierless heteromolecular homogeneous nucleation between GSA and semi-volatile organic vapour (for example adipic acid) combined with the homogeneous nucleation of GSA alone. Major growth of the particles was predicted to occur by the same organic vapour at concentrations of (1-2) ×1012cm-3. The pre-existing core and soot mode concentrations had opposite trend on the NUP formation, and maximum NUP formation was predicted if a diesel particle filter (DPF) was used. On the other hand, NUP formation was ceased if the GSA concentration was less than 1010cm-3 which suggests, based on the measurements, the usage of biofuel to prevent volatile particles in diesel exhaust.

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

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    Alanen, Jenni; Simonen, Pauli; Saarikoski, Sanna; Timonen, Hilkka; Kangasniemi, Oskari; Saukko, Erkka; Hillamo, Risto; Lehtoranta, Kati; Murtonen, Timo; Vesala, Hannu; Keskinen, Jorma; Rönkkö, Topi

    2017-07-01

    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 kgfuel-1. 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

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

    Directory of Open Access Journals (Sweden)

    J. Alanen

    2017-07-01

    Full Text Available 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 kgfuel−1. 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

  3. Photochemical Formation of Sulfur-Containing Aerosols

    Science.gov (United States)

    Kroll, Jay A.; Vaida, Veronica

    2017-06-01

    In order to understand planetary climate systems, modeling the properties of atmospheric aerosols is vital. Aerosol formation plays an important role in planetary climates and is tied to feedback loops that can either warm or cool a planet. Sulfur compounds are known to play an important role in new particle aerosol formation and have been observed in a number of planetary atmospheres throughout our solar system. Our current understanding of sulfur chemistry explains much of what we observe in Earth's atmosphere; however, several discrepancies arise when comparing observations of the Venusian atmosphere with model predictions. This suggests that there are still problems in our fundamental understanding of sulfur chemistry. This is concerning given recent renewed interest in sulfate injections in the stratosphere for solar radiation management geo-engineering schemes. We investigate the role of sunlight as a potential driver of the formation of sulfur-containing aerosols. I will present recent work investigating the generation of large quantities of aerosol from the irradiation of mixtures of SO_2 with water and organic species, using a solar simulator that mimics the light that is available in the Earth's troposphere and the Venusian middle atmosphere. I will present on recent work done in our lab suggesting the formation of sulfurous acid, H_2SO_3, and describe experimental work that supports this proposed mechanism. Additionally I will present on new work showing the highly reactive nature of electronically excited SO_2 with saturated alkane species. The implications of this photochemically induced sulfur aerosol formation in the atmosphere of Earth and other planetary atmospheres will be discussed.

  4. Photochemical organonitrate formation in wet aerosols

    Directory of Open Access Journals (Sweden)

    Y. B. Lim

    2016-10-01

    Full Text Available Water is the most abundant component of atmospheric fine aerosol. However, despite rapid progress, multiphase chemistry involving wet aerosols is still poorly understood. In this work, we report results from smog chamber photooxidation of glyoxal- and OH-containing ammonium sulfate or sulfuric acid particles in the presence of NOx and O3 at high and low relative humidity. Particles were analyzed using ultra-performance liquid chromatography coupled to quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS. During the 3 h irradiation, OH oxidation products of glyoxal that are also produced in dilute aqueous solutions (e.g., oxalic acids and tartaric acids were formed in both ammonium sulfate (AS aerosols and sulfuric acid (SA aerosols. However, the major products were organonitrogens (CHNO, organosulfates (CHOS, and organonitrogen sulfates (CHNOS. These were also the dominant products formed in the dark chamber, indicating non-radical formation. In the humid chamber (> 70 % relative humidity, RH, two main products for both AS and SA aerosols were organonitrates, which appeared at m ∕ z− 147 and 226. They were formed in the aqueous phase via non-radical reactions of glyoxal and nitric acid, and their formation was enhanced by photochemistry because of the photochemical formation of nitric acid via reactions of peroxy radicals, NOx and OH during the irradiation.

  5. Modeling Secondary Organic Aerosol Formation From Emissions of Combustion Sources

    Science.gov (United States)

    Jathar, Shantanu Hemant

    -only model suggested that differences in the volatility of the precursors were able to explain most of the variability observed in the SOA formation. For aircraft exhaust, the previous methods to simulate SOA formation from SVOC and IVOC performed poorly. A more physically-realistic modeling framework was developed, which was then used to show that SOA formation from aircraft exhaust was (a) higher for petroleum-based than synthetically derived jet fuel and (b) higher at lower engine loads and vice versa. All of the SOA data from combustion emissions experiments were used to determine source-specific parameterizations to model SOA formation from SVOC, IVOC and other unspeciated emissions. The new parameterizations were used to investigate their influence on the OA budget in the United States. Combustion sources were estimated to emit about 2.61 Tg yr-1 of SVOC, 1VOC and other unspeciated emissions (sixth of the total anthropogenic organic emissions), which are predicted to double SOA production from combustion sources in the United States. The contribution of SVOC and IVOC emissions to global SOA formation was assessed using a global climate model. Simulations were performed using a modified version of GISS GCM 11'. The modified model predicted that SVOC and IVOC contributed to half of the OA mass in the atmosphere. Their inclusion improved OA model-measurement comparisons for absolute concentrations, POA-SOA split and volatility (gas-particle partitioning) globally suggesting that atmospheric models need to incorporate SOA formation from SVOC and IVOC if they are to reasonably predict the abundance and properties of aerosols. This thesis demonstrates that SVOC/IVOC and possibly other unspeciated organics emitted by combustion sources are very important precursors of SOA and potentially large contributors to the atmospheric aerosol mass. Models used for research and policy applications need to represent them to improve model-predictions of aerosols on climate and health

  6. Buildup of aerosol precursor gases and sulfur-induced activation of soot in nascent jet aircraft exhaust plumes

    Energy Technology Data Exchange (ETDEWEB)

    Kaercher, B.; Hirschberg, M.M.; Fabian, P. [Muenchen Univ. (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung; Gerz, T. [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Oberpfaffenhofen (Germany). Inst. fuer Physik der Atmosphaere

    1997-12-31

    Research issues concerning the chemical transformation of exhaust trace gases are summarized. The photochemical evolution of NO{sub x} early in the plume is strongly coupled to plume mixing. Substantial amounts of HNO{sub 3} are generated in nascent plumes even if no NO{sub 2} is emitted. The production of H{sub 2}SO{sub 4} becomes very efficient if part of the fuel sulfur is emitted as SO{sub 3}. Each emitted soot particle can acquire 1-10% by mass fully oxidized sulfur molecules prior to binary homogeneous nucleation, if a few percent of the exhaust SO{sub x} are emitted as SO{sub 3}, indicating an important activation pathway for soot, and leading to a marked enhancement of new aerosol formation and growth rates. (author) 11 refs.

  7. Model studies of volatile diesel exhaust particle formation: are organic vapours involved in nucleation and growth?

    Science.gov (United States)

    Pirjola, L.; Karl, M.; Rönkkö, T.; Arnold, F.

    2015-09-01

    A high concentration of volatile nucleation mode particles (NUP) formed in the atmosphere when the exhaust cools and dilutes has hazardous health effects and it impairs the visibility in urban areas. Nucleation mechanisms in diesel exhaust are only poorly understood. We performed model studies using two sectional aerosol dynamics process models AEROFOR and MAFOR on the formation of particles in the exhaust of a diesel engine, equipped with an oxidative after-treatment system and running with low fuel sulfur content (FSC) fuel, under laboratory sampling conditions where the dilution system mimics real-world conditions. Different nucleation mechanisms were tested. Based on the measured gaseous sulfuric acid (GSA) and non-volatile core and soot particle number concentrations of the raw exhaust, the model simulations showed that the best agreement between model predictions and measurements in terms of particle number size distribution was obtained by barrier-free heteromolecular homogeneous nucleation between the GSA and a semi-volatile organic vapour combined with the homogeneous nucleation of GSA alone. Major growth of the particles was predicted to occur due to the similar organic vapour at concentrations of (1-2) × 1012 cm-3. The pre-existing core and soot mode concentrations had an opposite trend on the NUP formation, and the maximum NUP formation was predicted if a diesel particle filter (DPF) was used. On the other hand, the model predicted that the NUP formation ceased if the GSA concentration in the raw exhaust was less than 1010 cm-3, which was the case when biofuel was used.

  8. A model study of the size and composition distribution of aerosols in an aircraft exhaust

    Energy Technology Data Exchange (ETDEWEB)

    Sorokin, A.A. [SRC `ECOLEN`, Moscow (Russian Federation)

    1997-12-31

    A two-dimensional, axisymmetric flow field model which includes water and sulphate aerosol formation represented by moments of the size and composition distribution function is used to calculate the effect of radial turbulent jet mixing on the aerosol size distribution and mean modal composition. (author) 6 refs.

  9. Formation of the natural sulfate aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Kerminen, V.M.; Hillamo, R.; Maekinen, M.; Virkkula, A.; Maekelae, T.; Pakkanen, T. [Helsinki Univ. (Finland). Dept. of Physics

    1996-12-31

    Anthropogenic sulfate aerosol, together with particles from biomass burning, may significantly reduce the climatic warming due to man-made greenhouse gases. The radiative forcing of aerosol particles is based on their ability to scatter and absorb solar radiation (direct effect), and on their influences on cloud albedos and lifetimes (indirect effect). The direct aerosol effect depends strongly on the size, number and chemical composition of particles, being greatest for particles of 0.1-1 {mu}m in diameter. The indirect aerosol effect is dictated by the number of particles being able to act as cloud condensation nuclei (CCN). For sulfate particles, the minimum CCN size in tropospheric clouds is of the order of 0.05-0.2 {mu}m. To improve aerosol parameterizations in future climate models, it is required that (1) both primary and secondary sources of various particle types will be characterized at a greater accuracy, and (2) the influences of various atmospheric processes on the spatial and temporal distribution of these particles and their physico-chemical properties are known much better than at the present. In estimating the climatic forcing due to the sulfate particles, one of the major problems is to distinguish between sulfur from anthropogenic sources and that of natural origin. Global emissions of biogenic and anthropogenic sulfate pre-cursors are comparable in magnitude, but over regional scales either of these two source types may dominate. The current presentation is devoted to discussing the natural sulfate aerosol, including the formation of sulfur-derived particles in the marine environment, and the use of particulate methanesulfonic acid (MSA) as a tracer for the natural sulfate

  10. Secondary organic aerosols: Formation potential and ambient data

    DEFF Research Database (Denmark)

    Barthelmie, R.J.; Pryor, S.C.

    1997-01-01

    Organic aerosols comprise a significant fraction of the total atmospheric particle loading and are associated with radiative forcing and health impacts. Ambient organic aerosol concentrations contain both a primary and secondary component. Herein, fractional aerosol coefficients (FAC) are used...... in conjunction with measurements of volatile organic compounds (VOC) to predict the formation potential of secondary organic aerosols (SOA) in the Lower Fraser Valley (LEV) of British Columbia. The predicted concentrations of SOA show reasonable accord with ambient aerosol measurements and indicate considerable...

  11. Organic aerosol formation during the atmospheric degradation of toluene.

    Science.gov (United States)

    Hurley, M D; Sokolov, O; Wallington, T J; Takekawa, H; Karasawa, M; Klotz, B; Barnes, I; Becker, K H

    2001-04-01

    Organic aerosol formation during the atmospheric oxidation of toluene was investigated using smog chamber systems. Toluene oxidation was initiated by the UV irradiation of either toluene/air/NOx or toluene/air/CH3ONO/NO mixtures. Aerosol formation was monitored using scanning mobility particle sizers and toluene loss was monitored by in-situ FTIR spectroscopy or GC-FID techniques. The experimental results show that the reaction of OH radicals, NO3 radicals and/or ozone with the first generation products of toluene oxidation are sources of organic aerosol during the atmospheric oxidation of toluene. The aerosol results fall into two groups, aerosol formed in the absence and presence of ozone. An analytical expression for aerosol formation is developed and values are obtained for the yield of the aerosol species. In the absence of ozone the aerosol yield, defined as aerosol formed per unit toluene consumed once a threshold for aerosol formation has been exceeded, is 0.075 +/- 0.004. In the presence of ozone the aerosol yield is 0.108 +/- 0.004. This work provides experimental evidence and a simple theory confirming the formation of aerosol from secondary reactions.

  12. Observational insights into aerosol formation from isoprene.

    Science.gov (United States)

    Worton, David R; Surratt, Jason D; Lafranchi, Brian W; Chan, Arthur W H; Zhao, Yunliang; Weber, Robin J; Park, Jeong-Hoo; Gilman, Jessica B; de Gouw, Joost; Park, Changhyoun; Schade, Gunnar; Beaver, Melinda; Clair, Jason M St; Crounse, John; Wennberg, Paul; Wolfe, Glenn M; Harrold, Sara; Thornton, Joel A; Farmer, Delphine K; Docherty, Kenneth S; Cubison, Michael J; Jimenez, Jose-Luis; Frossard, Amanda A; Russell, Lynn M; Kristensen, Kasper; Glasius, Marianne; Mao, Jingqiu; Ren, Xinrong; Brune, William; Browne, Eleanor C; Pusede, Sally E; Cohen, Ronald C; Seinfeld, John H; Goldstein, Allen H

    2013-10-15

    Atmospheric photooxidation of isoprene is an important source of secondary organic aerosol (SOA) and there is increasing evidence that anthropogenic oxidant emissions can enhance this SOA formation. In this work, we use ambient observations of organosulfates formed from isoprene epoxydiols (IEPOX) and methacrylic acid epoxide (MAE) and a broad suite of chemical measurements to investigate the relative importance of nitrogen oxide (NO/NO2) and hydroperoxyl (HO2) SOA formation pathways from isoprene at a forested site in California. In contrast to IEPOX, the calculated production rate of MAE was observed to be independent of temperature. This is the result of the very fast thermolysis of MPAN at high temperatures that affects the distribution of the MPAN reservoir (MPAN / MPA radical) reducing the fraction that can react with OH to form MAE and subsequently SOA (F(MAE formation)). The strong temperature dependence of F(MAE formation) helps to explain our observations of similar concentrations of IEPOX-derived organosulfates (IEPOX-OS; ~1 ng m(-3)) and MAE-derived organosulfates (MAE-OS; ~1 ng m(-3)) under cooler conditions (lower isoprene concentrations) and much higher IEPOX-OS (~20 ng m(-3)) relative to MAE-OS (water content when aerosol pH is constant. However, the higher fraction of MAE ring opening products does not compensate for the lower MAE production under warmer conditions (higher isoprene concentrations) resulting in lower formation of MAE-derived products relative to IEPOX at the surface. In regions of high NOx, high isoprene emissions and strong vertical mixing the slower MPAN thermolysis rate aloft could increase the fraction of MPAN that forms MAE resulting in a vertically varying isoprene SOA source.

  13. Characterizing the formation of secondary organic aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Lunden, Melissa; Black, Douglas; Brown, Nancy

    2004-02-01

    combination of the aerosol and gas phase data, will continue to provide important information on the extent to which biogenic emissions contribute to secondary organic aerosol and may elucidate important interactions between anthropogenic and biogenic sources. The results of these studies, performed in the field, will contribute to the growing effort to produce robust models for particulate formation that are necessary for air quality planning and source apportionment.

  14. Dilution and aerosol dynamics within a diesel car exhaust plume—CFD simulations of on-road measurement conditions

    Science.gov (United States)

    Uhrner, U.; von Löwis, S.; Vehkamäki, H.; Wehner, B.; Bräsel, S.; Hermann, M.; Stratmann, F.; Kulmala, M.; Wiedensohler, A.

    Vehicle particle emissions are studied extensively because of their health effects, contribution to ambient PM levels and possible impact on climate. The aim of this work was to obtain a better understanding of secondary particle formation and growth in a diluting vehicle exhaust plume using 3-d information of simulations together with measurements. Detailed coupled computational fluid dynamics (CFD) and aerosol dynamics simulations have been conducted for H 2SO 4-H 2O and soot particles based on measurements within a vehicle exhaust plume under real conditions on public roads. Turbulent diffusion of soot and nucleation particles is responsible for the measured decrease of number concentrations within the diesel car exhaust plume and decreases coagulation rates. Particle size distribution measurements at 0.45 and 0.9 m distance to the tailpipe indicate a consistent soot mode (particle diameter Dp˜50 nm) at variable operating conditions. Soot mode number concentrations reached up to 10 13 m -3 depending on operating conditions and mixing. For nucleation particles the simulations showed a strong sensitivity to the spatial dilution pattern, related cooling and exhaust H 2SO 4(g). The highest simulated nucleation rates were about 0.05-0.1 m from the axis of the plume. The simulated particle number concentration pattern is in approximate accordance with measured concentrations, along the jet centreline and 0.45 and 0.9 m from the tailpipe. Although the test car was run with ultralow sulphur fuel, high nucleation particle ( Dp⩽15 nm) concentrations (>10 13 m -3) were measured under driving conditions of strong acceleration or the combination of high vehicle speed (>140 km h -1) and high engine rotational speed (>3800 revolutions per minute (rpm)). Strong mixing and cooling caused rapid nucleation immediately behind the tailpipe, so that the highest particle number concentrations were recorded at a distance, x=0.45 m behind the tailpipe. The simulated growth of H 2SO 4

  15. Organic Aerosol Formation Photoenhanced by the Formation of Secondary Photo-sensitizers in ageing Aerosols

    Science.gov (United States)

    Aregahegn, Kifle; Nozière, Barbara; George, Christian

    2013-04-01

    Humankind is facing a changing environment possibly due to anthropogenic stress on the atmosphere. In this context, aerosols play a key role by affecting the radiative climate forcing, hydrological cycle, and by their adverse effect on health. The role of organic compounds in these processes is however still poorly understood because of their massive chemical complexity and numerous transformations. This is particularly true for Secondary Organic Aerosol (SOA), which are produced in the atmosphere by organic gases. Traditionally, the driving forces for SOA growth is believed to be the partitioning onto aerosol seeds of condensable gases, either emitted primarily or resulting from the gas phase oxidation of organic gases. However, even the most up-to-date models based on such mechanisms can not account for the SOA mass observed in the atmosphere, suggesting the existence of other, yet unknown formation processes. The present study shows experimental evidence that particulate phase chemistry produces photo-sensitizers that lead to photo-induced formation and growth of secondary organic aerosol in the near UV and the presence of volatile organic compounds (VOC) such as terpenes. By means of an aerosol flow tube reactor equipped with Scanning Mobility Particle Sizer (SMPS) having Kr-85 source aerosol neutralizer, Differential Mobility Analyser (DMA) and Condensation Particle Sizer (CPC), we identified that traces of the aerosol phase product of glyoxal chemistry as is explained in Gallway et al., and Yu et al., namely imidazole-2-carboxaldehyde (IC) is a strong photo-sensitizer when irradiated by near-UV in the presence of volatile organic compounds such as terpenes. Furthermore, the influence of pH, type and concentration of VOCs, composition of seed particles, relative humidity and irradiation intensity on particle growth were studied. This novel photo-sensitizer contributed to more than 30% of SOA growth in 19min irradiation time in the presence of terpenes in the

  16. Carbonaceous aerosol in jet engine exhaust: emission characteristics and implications for heterogeneous chemical reactions

    Energy Technology Data Exchange (ETDEWEB)

    Petzold, A.; Schroeder, F.P.; Kaercher, B. [Deutsches Zentrum fuer Luft- und Raumfahrt, Wessling (Germany). Institut fuer Physik der Atmosphaere; Stroem, J. [Stockholm University (Sweden). Dept. of Meteorology

    1999-08-01

    Characteristic parameters of black carbon aerosol (BC) emitted from jet engine were measured during ground tests and in-flight behind the same aircraft. Size distribution features were a primary BC mode at a model diameter D {approx} 0.045 {mu}m, and a BC agglomeration mode at D < 0.2 {mu}m. The total BC number concentration at the engine exit was 2.9 x 10{sup 7} cm{sup -3} with good agreement between model results and in-flight measured number concentrations of non-volatile particles with D {>=} 0.014 {mu}m. A comparison between total number concentration of BC particles and the non-volatile fraction of the total aerosol at the exit plane suggests that the non-volatile fraction of jet engine exhaust aerosol consists almost completely of BC. In-flight BC mass emission indices ranged from 0.11 to 0.15 g BC (kg fuel){sup -1}. The measured in-flight particle emission value was 1.75 {+-} 0.15 x 10{sup 15} kg{sup -1} with corresponding ground test values of 1.0-8.7 x 10{sup 14} kg{sup -1}. Both size distribution properties and mass emission indices can be scaled from ground test to in-flight conditions. Implications for atmosphere BC loading, BC and cirrus interaction and the potential of BC for perturbation of atmospheric chemistry are briefly outlined. (author)

  17. Secondary organic aerosol formation from photo-oxidation of unburned fuel: experimental results and implications for aerosol formation from combustion emissions.

    Science.gov (United States)

    Jathar, Shantanu H; Miracolo, Marissa A; Tkacik, Daniel S; Donahue, Neil M; Adams, Peter J; Robinson, Allen L

    2013-11-19

    We conducted photo-oxidation experiments in a smog chamber to investigate secondary organic aerosol (SOA) formation from eleven different unburned fuels: commercial gasoline, three types of jet fuel, and seven different diesel fuels. The goals were to investigate the influence of fuel composition on SOA formation and to compare SOA production from unburned fuel to that from diluted exhaust. The trends in SOA production were largely consistent with differences in carbon number and molecular structure of the fuel, i.e., fuels with higher carbon numbers and/or more aromatics formed more SOA than fuels with lower carbon numbers and/or substituted alkanes. However, SOA production from different diesel fuels did not depend strongly on aromatic content, highlighting the important contribution of large alkanes to SOA formation from mixtures of high carbon number (lower volatility) precursors. In comparison to diesels, SOA production from higher volatility fuels such as gasoline appeared to be more sensitive to aromatic content. On the basis of a comparison of SOA mass yields (SOA mass formed per mass of fuel reacted) and SOA composition (as measured by an aerosol mass spectrometer) from unburned fuels and diluted exhaust, unburned fuels may be reasonable surrogates for emissions from uncontrolled engines but not for emissions from engines with after treatment devices such as catalytic converters.

  18. Instant foam physics : formation and stability of aerosol whipped cream

    NARCIS (Netherlands)

    Wijnen, M.E.

    1997-01-01

    The formation and stability of aerosol whipped cream, as an example of an instant foam, were studied from a physical point of view. Instant foam production out of an aerosol can is based on the principle that a soluble gas (laughing gas) is dissolved under elevated pressure (5-10 bar) in

  19. The influence of metallurgy on the formation of welding aerosols.

    Science.gov (United States)

    Zimmer, Anthony T

    2002-10-01

    Recent research has indicated that insoluble ultrafine aerosols (ie., particles whose physical diameters are less than 100 nm) may cause adverse health effects due to their small size, and that toxicological response may be more appropriately represented by particle number or particle surface area. Unfortunately, current exposure criteria and the associated air-sampling techniques are primarily mass-based. Welding processes are high-temperature operations that generate substantial number concentrations of ultrafine aerosols. Welding aerosols are formed primarily through the nucleation of metal vapors followed by competing growth mechanisms such as coagulation and condensation. Experimental results and mathematical tools are presented to illustrate how welding metallurgy influences the chemical aspects and dynamic processes that initiate and evolve the resultant aerosol. This research suggests that a fundamental understanding of metallurgy and aerosol physics can be exploited to suppress the formation of undesirable chemical species as well as the amount of aerosol generated during a welding process.

  20. Modeling Photosensitized Secondary Organic Aerosol Formation in Laboratory and Ambient Aerosols.

    Science.gov (United States)

    Tsui, William G; Rao, Yi; Dai, Hai-Lung; McNeill, V Faye

    2017-07-05

    Photosensitized reactions involving imidazole-2-carboxaldehyde (IC) have been experimentally observed to contribute to secondary organic aerosol (SOA) growth. However, the extent of photosensitized reactions in ambient aerosols remains poorly understood and unaccounted for in atmospheric models. Here we use GAMMA 4.0, a photochemical box model that couples gas-phase and aqueous-phase aerosol chemistry, along with recent laboratory measurements of the kinetics of IC photochemistry, to analyze IC-photosensitized SOA formation in laboratory and ambient settings. Analysis of the laboratory results of Aregahegn et al. (2013) suggests that photosensitized production of SOA from limonene, isoprene, α-pinene, β-pinene, and toluene by 3IC* occurs at or near the surface of the aerosol particle. Reactive uptake coefficients were derived from the experimental data using GAMMA 4.0. Simulations of aqueous aerosol SOA formation at remote ambient conditions including IC photosensitizer chemistry indicate less than 0.3% contribution to SOA growth from direct reactions of 3IC* with limonene, isoprene, α-pinene, β-pinene, and toluene, and an enhancement of less than 0.04% of SOA formation from other precursors due to the formation of radicals in the bulk aerosol aqueous phase. Other, more abundant photosensitizer species, such as humic-like substances (HULIS), may contribute more significantly to aqueous aerosol SOA production.

  1. Secondary aerosol formation from atmospheric reactions of aliphatic amines

    Directory of Open Access Journals (Sweden)

    S. M. Murphy

    2007-01-01

    Full Text Available Although aliphatic amines have been detected in both urban and rural atmospheric aerosols, little is known about the chemistry leading to particle formation or the potential aerosol yields from reactions of gas-phase amines. We present here the first systematic study of aerosol formation from the atmospheric reactions of amines. Based on laboratory chamber experiments and theoretical calculations, we evaluate aerosol formation from reaction of OH, ozone, and nitric acid with trimethylamine, methylamine, triethylamine, diethylamine, ethylamine, and ethanolamine. Entropies of formation for alkylammonium nitrate salts are estimated by molecular dynamics calculations enabling us to estimate equilibrium constants for the reactions of amines with nitric acid. Though subject to significant uncertainty, the calculated dissociation equilibrium constant for diethylammonium nitrate is found to be sufficiently small to allow for its atmospheric formation, even in the presence of ammonia which competes for available nitric acid. Experimental chamber studies indicate that the dissociation equilibrium constant for triethylammonium nitrate is of the same order of magnitude as that for ammonium nitrate. All amines studied form aerosol when photooxidized in the presence of NOx with the majority of the aerosol mass present at the peak of aerosol growth consisting of aminium (R3NH+ nitrate salts, which repartition back to the gas phase as the parent amine is consumed. Only the two tertiary amines studied, trimethylamine and triethylamine, are found to form significant non-salt organic aerosol when oxidized by OH or ozone; calculated organic mass yields for the experiments conducted are similar for ozonolysis (15% and 5% respectively and photooxidation (23% and 8% respectively. The non-salt organic aerosol formed appears to be more stable than the nitrate salts and does not quickly repartition back to the gas phase.

  2. Heterogeneous formation of HONO on carbonaceous aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Ammann, M.; Kalberer, M.; Tabor, K. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)] [and others

    1997-09-01

    Based on an on-line and in situ experimental approach, for the first time heterogeneous production of nitrous acid (HONO) on carbon aerosol at ambient pressure and low NO{sub 2} concentration has been quantified by use of a {sup 13}N tracer technique. (author) 1 fig., 4 refs.

  3. Formation of nitrogenated organic aerosols in the Titan upper atmosphere

    Science.gov (United States)

    Imanaka, Hiroshi; Smith, Mark A.

    2010-01-01

    Many aspects of the nitrogen fixation process by photochemistry in the Titan atmosphere are not fully understood. The recent Cassini mission revealed organic aerosol formation in the upper atmosphere of Titan. It is not clear, however, how much and by what mechanism nitrogen is incorporated in Titan’s organic aerosols. Using tunable synchrotron radiation at the Advanced Light Source, we demonstrate the first evidence of nitrogenated organic aerosol production by extreme ultraviolet–vacuum ultraviolet irradiation of a N2/CH4 gas mixture. The ultrahigh-mass-resolution study with laser desorption ionization-Fourier transform-ion cyclotron resonance mass spectrometry of N2/CH4 photolytic solid products at 60 and 82.5 nm indicates the predominance of highly nitrogenated compounds. The distinct nitrogen incorporations at the elemental abundances of H2C2N and HCN, respectively, are suggestive of important roles of H2C2N/HCCN and HCN/CN in their formation. The efficient formation of unsaturated hydrocarbons is observed in the gas phase without abundant nitrogenated neutrals at 60 nm, and this is confirmed by separately using 13C and 15N isotopically labeled initial gas mixtures. These observations strongly suggest a heterogeneous incorporation mechanism via short lived nitrogenated reactive species, such as HCCN radical, for nitrogenated organic aerosol formation, and imply that substantial amounts of nitrogen is fixed as organic macromolecular aerosols in Titan’s atmosphere. PMID:20616074

  4. Secondary Aerosol: Precursors and Formation Mechanisms. Technical Report on Grant

    Energy Technology Data Exchange (ETDEWEB)

    Weinstein-Lloyd, Judith B

    2009-05-04

    This project focused on studying trace gases that participate in chemical reactions that form atmospheric aerosols. Ammonium sulfate is a major constituent of these tiny particles, and one important pathway to sulfate formation is oxidation of dissolved sulfur dioxide by hydrogen peroxide in cloud, fog and rainwater. Sulfate aerosols influence the number and size of cloud droplets, and since these factors determine cloud radiative properties, sulfate aerosols also influence climate. Peroxide measurements, in conjunction with those of other gaseous species, can used to distinguish the contribution of in-cloud reaction to new sulfate aerosol formation from gas-phase nucleation reactions. This will lead to more reliable global climate models. We constructed and tested a new 4-channel fluorescence detector for airborne detection of peroxides. We integrated the instrument on the G-1 in January, 2006 and took a test flight in anticipation of the MAX-Mex field program, where we planned to fly under pressurized conditions for the first time. We participated in the 2006 Megacity Initiative: Local and Global Research Observations (MILAGRO) - Megacity Aerosol EXperiment Mexico City (MAX-Mex) field measurement campaign. Peroxide instrumentation was deployed on the DOE G-1 research aircraft based in Veracruz, and at the surface site at Tecamac University.

  5. Automobile diesel exhaust particles induce lipid droplet formation in macrophages in vitro

    DEFF Research Database (Denmark)

    Cao, Yi; Jantzen, Kim; Gouveia, Ana Cecilia Damiao

    2015-01-01

    Exposure to diesel exhaust particles (DEP) has been associated with adverse cardiopulmonary health effects, which may be related to dysregulation of lipid metabolism and formation of macrophage foam cells. In this study, THP-1 derived macrophages were exposed to an automobile generated DEP (A...... that exposure to A-DEP may induce formation of lipid droplets in macrophages in vitro possibly via lysosomal dysfunction....

  6. Effect of measurement protocol on organic aerosol measurements of exhaust emissions from gasoline and diesel vehicles

    Science.gov (United States)

    Kim, Youngseob; Sartelet, Karine; Seigneur, Christian; Charron, Aurélie; Besombes, Jean-Luc; Jaffrezo, Jean-Luc; Marchand, Nicolas; Polo, Lucie

    2016-09-01

    Exhaust emissions of semi-volatile organic compounds (SVOC) from passenger vehicles are usually estimated only for the particle phase via the total particulate matter measurements. However, they also need to be estimated for the gas phase, as they are semi-volatile. To better estimate SVOC emission factors of passenger vehicles, a measurement campaign using a chassis dynamometer was conducted with different instruments: (1) a constant volume sampling (CVS) system in which emissions were diluted with filtered air and sampling was performed on filters and polyurethane foams (PUF) and (2) a Dekati Fine Particle Sampler (FPS) in which emissions were diluted with purified air and sampled with on-line instruments (PTR-ToF-MS, HR-ToF-AMS, MAAP, CPC). Significant differences in the concentrations of organic carbon (OC) measured by the instruments are observed. The differences can be explained by sampling artefacts, differences between (1) the time elapsed during sampling (in the case of filter and PUF sampling) and (2) the time elapsed from emission to measurement (in the case of on-line instruments), which vary from a few seconds to 15 min, and by the different dilution factors. To relate elapsed times and measured concentrations of OC, the condensation of SVOC between the gas and particle phases is simulated with a dynamic aerosol model. The simulation results allow us to understand the relation between elapsed times and concentrations in the gas and particle phases. They indicate that the characteristic times to reach thermodynamic equilibrium between gas and particle phases may be as long as 8 min. Therefore, if the elapsed time is less than this characteristic time to reach equilibrium, gas-phase SVOC are not at equilibrium with the particle phase and a larger fraction of emitted SVOC will be in the gas phase than estimated by equilibrium theory, leading to an underestimation of emitted OC if only the particle phase is considered or if the gas-phase SVOC are estimated

  7. New Particle Formation and Secondary Organic Aerosol in Beijing

    Science.gov (United States)

    Hu, M.; Yue, D.; Guo, S.; Hu, W.; Huang, X.; He, L.; Wiedensohler, A.; Zheng, J.; Zhang, R.

    2011-12-01

    Air pollution in Beijing has been a major concern due to being a mega-city and green Olympic Games requirements. Both long term and intensive field measurements have been conducted at an Urban Air Quality Monitoring Station in the campus of Peking University since 2004. Aerosol characteristics vary seasonally depending on meteorological conditions and source emissions. Secondary compositions of SNA (sum of sulfate, nitrate, and ammonium) and SOA (secondary organic aerosol) become major fraction of fine particles, which may enhance aerosol impacts on visibility and climate change. The transformation processes of new particle formation (NPF) and secondary organic aerosol have been focused on. It was found that gaseous sulfuric acid, ammonia, and organic compounds are important precursors to NPF events in Beijing and H2SO4-NH3-H2O ternary nucleation is one of the important mechanisms. The contributions of condensation and neutralization of sulfuric acid, coagulation, and organics to the growth of the new particles are estimated as 45%, 34%, and 21%, respectively. Tracer-based method to estimate biogenic and anthropogenic SOA was established by using gas chromatography-mass spectrometry. Secondary organic tracers derived from biogenic (isoprene, α-pinene, β-caryophyllene) and anthropogenic (toluene) contributed 32% at urban site and 35% at rural site, respectively. Other source apportionment techniques were also used to estimate secondary organic aerosols, including EC tracer method, water soluble organic carbon content, chemical mass balance model, and AMS-PMF method.

  8. Secondary organic aerosol formation from intermediate-volatility organic compounds: cyclic, linear, and branched alkanes.

    Science.gov (United States)

    Tkacik, Daniel S; Presto, Albert A; Donahue, Neil M; Robinson, Allen L

    2012-08-21

    Intermediate volatility organic compounds (IVOCs) are an important class of secondary organic aerosol (SOA) precursors that have not been traditionally included in chemical transport models. A challenge is that the vast majority of IVOCs cannot be speciated using traditional gas chromatography-based techniques; instead they are classified as an unresolved complex mixture (UCM) that is presumably made up of a complex mixture of branched and cyclic alkanes. To better understand SOA formation from IVOCs, a series of smog chamber experiments was conducted with different alkanes, including cyclic, branched, and linear compounds. The experiments focused on freshly formed SOA from hydroxyl (OH) radical-initiated reactions under high-NO(x) conditions at typical atmospheric organic aerosol concentrations (C(OA)). SOA yields from cyclic alkanes were comparable to yields from linear alkanes three to four carbons larger in size. For alkanes with equivalent carbon numbers, branched alkanes had the lowest SOA mass yields, ranging between 0.05 and 0.08 at a C(OA) of 15 μg m(-3). The SOA yield of branched alkanes also depends on the methyl branch position on the carbon backbone. High-resolution aerosol mass spectrometer data indicate that the SOA oxygen-to-carbon ratios were largely controlled by the carbon number of the precursor compound. Depending on the precursor size, the mass spectrum of SOA produced from IVOCs is similar to the semivolatile-oxygenated and hydrocarbon-like organic aerosol factors derived from ambient data. Using the new yield data, we estimated SOA formation potential from diesel exhaust and predict the contribution from UCM vapors to be nearly four times larger than the contribution from single-ring aromatics and comparable to that of polycyclic aromatic hydrocarbons after several hours of oxidation at typical atmospheric conditions. Therefore, SOA from IVOCs may be an important contributor to urban OA and should be included in SOA models; the yield data

  9. Effects of gaseous sulphuric acid on diesel exhaust nanoparticle formation and characteristics.

    Science.gov (United States)

    Rönkkö, Topi; Lähde, Tero; Heikkilä, Juha; Pirjola, Liisa; Bauschke, Ulrike; Arnold, Frank; Schlager, Hans; Rothe, Dieter; Yli-Ojanperä, Jaakko; Keskinen, Jorma

    2013-10-15

    Diesel exhaust gaseous sulphuric acid (GSA) concentrations and particle size distributions, concentrations, and volatility were studied at four driving conditions with a heavy duty diesel engine equipped with oxidative exhaust after-treatment. Low sulfur fuel and lubricant oil were used in the study. The concentration of the exhaust GSA was observed to vary depending on the engine driving history and load. The GSA affected the volatile particle fraction at high engine loads; higher GSA mole fraction was followed by an increase in volatile nucleation particle concentration and size as well as increase of size of particles possessing nonvolatile core. The GSA did not affect the number of nonvolatile particles. At low and medium loads, the exhaust GSA concentration was low and any GSA driven changes in particle population were not observed. Results show that during the exhaust cooling and dilution processes, besides critical in volatile nucleation particle formation, GSA can change the characteristics of all nucleation mode particles. Results show the dual nature of the nucleation mode particles so that the nucleation mode can include simultaneously volatile and nonvolatile particles, and fulfill the previous results for the nucleation mode formation, especially related to the role of GSA in formation processes.

  10. Review of Urban Secondary Organic Aerosol Formation from Gasoline and Diesel Motor Vehicle Emissions.

    Science.gov (United States)

    Gentner, Drew R; Jathar, Shantanu H; Gordon, Timothy D; Bahreini, Roya; Day, Douglas A; El Haddad, Imad; Hayes, Patrick L; Pieber, Simone M; Platt, Stephen M; de Gouw, Joost; Goldstein, Allen H; Harley, Robert A; Jimenez, Jose L; Prévôt, André S H; Robinson, Allen L

    2017-02-07

    Secondary organic aerosol (SOA) is formed from the atmospheric oxidation of gas-phase organic compounds leading to the formation of particle mass. Gasoline- and diesel-powered motor vehicles, both on/off-road, are important sources of SOA precursors. They emit complex mixtures of gas-phase organic compounds that vary in volatility and molecular structure-factors that influence their contributions to urban SOA. However, the relative importance of each vehicle type with respect to SOA formation remains unclear due to conflicting evidence from recent laboratory, field, and modeling studies. Both are likely important, with evolving contributions that vary with location and over short time scales. This review summarizes evidence, research needs, and discrepancies between top-down and bottom-up approaches used to estimate SOA from motor vehicles, focusing on inconsistencies between molecular-level understanding and regional observations. The effect of emission controls (e.g., exhaust aftertreatment technologies, fuel formulation) on SOA precursor emissions needs comprehensive evaluation, especially with international perspective given heterogeneity in regulations and technology penetration. Novel studies are needed to identify and quantify "missing" emissions that appear to contribute substantially to SOA production, especially in gasoline vehicles with the most advanced aftertreatment. Initial evidence suggests catalyzed diesel particulate filters greatly reduce emissions of SOA precursors along with primary aerosol.

  11. Aerosol vertical distribution, new particle formation, and jet aircraft particle emissions in the free troposhere and tropopause region; Vertikalverteilung und Neubildungsprozesse des Aerosols und partikelfoermige Flugzeugemissionen in der freien Troposphaere und Tropopausenregion

    Energy Technology Data Exchange (ETDEWEB)

    Schroeder, F.P.

    2000-07-01

    A contribution to the understanding of natural and anthropogenously induced particle formation as well as aerosol physical transformation processes within the free troposphere (FT) is introduced. Documentation and interpretation of empirical data relevant with respect to possible climatologic impact of anthropogenous aerosol emissions into the atmosphere is presented. The first section describes new technique for high spatial resolution measurements of ultrafine aerosol particles by condensation nucleus counters (CNCs), a necessary prerequisite for the observation of natural particle formation and jet aircraft emissions. The second section illustrates vertical distribution and variability ranges of the aerosol in the FT and the tropopause region (TP). Typical microphysical states of the atmospheric aerosol within the Northern Hemisphere are documented by means of systematic measurements during more than 60 flight missions. Simple mathematical parameterizations of the aerosol vertical distribution and aerosol size distributions are developed. Important aerosol sources within the FT are localized and possible aerosol formation processes are discussed. The third section is focussed on jet-engine particle emissions within the FT and TP. A unique inflight experiment for detection of extremely high concentrations (>10{sup 6} cm{sup -3}) of extremely small (donw to <3 nm) aerosols inside the exhaust plumes of several jet aircraft is described. Particle emission indices and emission-controlling parameters are deduced. Most important topic is the impact of fuel sulfur content of kerosine on number, size and chemical composition of jet particle emissions. Generalized results are parameterized in form of lognormal aerosol particle size distributions. (orig.) [German] Ein Beitrag zum Verstaendnis natuerlicher und anthropogen induzierter Aerosolneubildung sowie physikalischer Aerosolumwandlung in der freien Troposphaere wird vorgestellt. Empirisch gewonnenes Datenmaterial wird

  12. Gasoline aromatics: a critical determinant of urban secondary organic aerosol formation

    Science.gov (United States)

    Peng, Jianfei; Hu, Min; Du, Zhuofei; Wang, Yinhui; Zheng, Jing; Zhang, Wenbin; Yang, Yudong; Qin, Yanhong; Zheng, Rong; Xiao, Yao; Wu, Yusheng; Lu, Sihua; Wu, Zhijun; Guo, Song; Mao, Hongjun; Shuai, Shijin

    2017-09-01

    Gasoline vehicle exhaust is an important contributor to secondary organic aerosol (SOA) formation in urban atmosphere. Fuel composition has a potentially considerable impact on gasoline SOA production, but the link between fuel components and SOA production is still poorly understood. Here, we present chamber experiments to investigate the impacts of gasoline aromatic content on SOA production through chamber oxidation approach. A significant amplification factor of 3-6 for SOA productions from gasoline exhausts is observed as gasoline aromatic content rose from 29 to 37 %. Considerably higher emission of aromatic volatile organic compounds (VOCs) using high-aromatic fuel plays an essential role in the enhancement of SOA production, while semi-volatile organic compounds (e.g., gas-phase PAHs) may also contribute to the higher SOA production. Our findings indicate that gasoline aromatics significantly influence ambient PM2. 5 concentration in urban areas and emphasize that more stringent regulation of gasoline aromatic content will lead to considerable benefits for urban air quality.

  13. Ice Formation by Soot-Containing Aerosol Particles

    Science.gov (United States)

    Demott, P. J.; Petters, M. D.; Prenni, A. J.; Kreidenweis, S. M.; Carrico, C. M.; Bennett, M. R.; Stanglmaier, R.; Volckens, J.; Popovicheva, O. B.

    2006-12-01

    A role for soot particles as atmospheric ice forming nuclei remains highly uncertain and poorly quantified. A relatively small amount of data exists and most of this is for laboratory surrogates that may not be well characterized or of assured relevance to the atmosphere. It is important to constrain the role of soot particles as ice nuclei due to their abundance in the atmosphere and the large contribution from anthropogenic activities. Further, global climate models are beginning to be capable of treating the impact of different aerosol types, including soot particles. This paper reports on studies of ice formation by or within surrogates for hydrophobic soot and realistic carbonaceous particles from combustion of fuel in a diesel engine, burning of an assortment biomass materials, and real jet fuel combustor particles. Measurements of primarily monodisperse particles were focused below -30°C to emphasize the transition between temperatures where heterogeneous ice nucleation is required for ice formation and those for which homogeneous freezing processes are also possible. Ice nucleation measurements were made with a continuous flow diffusion chamber. Simultaneous measurements of hygroscopic water uptake and cloud condensation nucleation behavior were also made at 30°C for each aerosol type. Small fractions of hydrophobic soot particles are found capable of initiating heterogeneous ice formation at low temperatures. Results of studies of more realistic particles suggest that any process that increases hygroscopicity tends to limit the conditions for ice formation within soot particles. Most biomass burning particles, showing a range of dry/wet diameter hygroscopic growth factors (1.03 activity as CCN to 102% RH, yet behaved as particles containing solutions in which homogeneous freezing was supported at temperatures below -38°C. This is tentatively attributed to condensation of semi-volatiles during cooling. Ice forming ability as warm as -30°C was limited to

  14. New aerosol particles formation in the Sao Paulo Metropolitan Area

    Science.gov (United States)

    Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

    2016-04-01

    performance. For secondary aerosols, a simulation scenario (Case_1) with only emission of primary gases (biogenic and anthropogenic) is performed to evaluate its formation potential. The study period from 7th August to 6th September 2012 has been selected due to the avaliability of experimental data from the Narrowing the Uncertainties on Aerosol and Climate Changes in Sao Paulo State (NUANCE) project. Aerosol measurements consist basically on PM2.5 and PM10 concentration. OC, EC, ion, and aerosol mass size distribution measurements were also carried out in one of the measurement sites (IAG-USP). Results show that overall the emissions of primary gases coming mainly from vehicles have a potential to form new particles between 20 and 30% in relation to the baseline PM2.5 mass concentration found in the downtown SPMA. In addition, both the observed and predicted OC and EC at the IAG-USP measurement site make up the largest fraction of PM2.5 mass with contributions around 55 and 40%, respectively.

  15. Combustion-related pollutants of polydisperse single-composition aerosols and advection fog formation

    Science.gov (United States)

    Hung, R. J.; Liaw, G. S.

    1982-01-01

    The most noticeable effect of air pollution on the properties of the atmosphere is the reduction in visibility, with and without the occurrence of condensation, which frequently accompanies polluted air. The present study concerns the formation of advection fog associated with aerosols, due to combustion-related pollutants, with a polydisperse population distribution and a single composition model. The results show that an aerosol population with high particle concentration-shifted distribution provides a more favorable condition for the formation of dense fog than an aerosol population with a low particle concentration-shifted distribution if the value of the mass concentration of the aerosols is kept constant.

  16. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

    Science.gov (United States)

    Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

    2013-12-17

    The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

  17. Formation of Mesostructured Nanoparticles through Self-Assembly and Aerosol Process

    Energy Technology Data Exchange (ETDEWEB)

    Brinker, C. Jeffrey; Fan, Hongyou; Lu, Yunfeng; Rieker, Thomas; Stump, Arron; Ward, Timothy L.

    1999-05-07

    Silica nanoparticles exhibiting hexagonal, cubic, and vesicular mesostructures have been prepared using aerosol assisted, self-assembled process. This process begins with homogennous aerosol droplets containing silica source, water, ethanol, and surfactant, in which surfactant concentration is far below the critical micelle concentration (cmc). Solvent evaporation enriches silica and surfactant inducing interfacial self-assembly confined to a spherical aerosol droplet and results in formation of completely solid, ordered spherical particles with stable hexagonal, cubic, or vesicular mesostructures.

  18. Aerosol Formation from OH Oxidation of the Volatile Cyclic Methyl Siloxane (cVMS) Decamethylcyclopentasiloxane.

    Science.gov (United States)

    Wu, Yue; Johnston, Murray V

    2017-04-18

    Aerosol formation from OH oxidation of decamethylcyclopentasiloxane (D5, C10H30O5Si5), a cyclic volatile methyl siloxane (cVMS) found in consumer products, was studied in a flow-through photo-oxidation chamber with and without the presence of ammonium sulfate seed aerosol. For the unseeded experiments, chemical characterization with high-performance mass spectrometry showed that the molecular composition changed substantially with aerosol mass loading in the 1-12 μg/m3 range. Monomers (5 Si atoms/molecule) and dimers (10 Si atoms/molecule) dominated the mass spectra of aerosols at higher mass loadings, while ring-opened species (neither 5 nor 10 Si atoms/molecule) dominated the mass spectra of aerosols at lower mass loadings. Molecular signal intensity dependencies upon the aerosol volume/surface area ratio suggest that non-volatile ring-opened species are formed in the gas phase and assist particle formation through condensation, while dimers are formed by accretion reactions within the particle phase as the particles grow. These conclusions are supported by experiments in the presence of seed aerosol with a similar siloxane aerosol mass loading but higher volume/surface area ratio, where ring-opened species are much less prevalent than monomers or dimers and the aerosol yield is higher. Because of the importance of accretion chemistry, the aerosol yield from D5 oxidation is likely to be strongly dependent upon the particle size and morphology.

  19. Simulating the effects of semivolatile aerosol species on cloud formation and lifecycle

    Science.gov (United States)

    Kokkola, Harri; Kudzotsa, Innocent; Tonttila, Juha; Raatikainen, Tomi; Romakkaniemi, Sami

    2017-04-01

    The effect of aerosol has been acknowledged to cause a significant uncertainty in estimating the anthropogenic aerosol effect on climate. Research efforts on the formation and growth of atmospheric particles to sizes where they become cloud condensation nuclei have been extensive. In comparison, much less attention is given on cloud processing of particles and aerosol removal through wet deposition. However, aerosol removal processes largely dictate how well aerosol is transported from source regions. This means that in order to model the global distribution aerosol, both in vertical and horizontal, wet deposition processes have to be properly modelled. However, in large scale models, the description of wet removal and the vertical redistribution of aerosol by cloud processes is very limited. Here we present a novel aerosol-cloud model SALSA, where the aerosol properties are tracked though cloud processes including: cloud droplet activation, precipitation formation, ice nucleation, melting, and evaporation. It is a sectional model that includes separate size sections for non-activated aerosol, cloud droplets, precipitation droplets, and ice crystals. The aerosol-cloud model was coupled to a large eddy model UCLALES which simulates the boundary-layer dynamics. In this study, the model has been applied in studying the wet removal as well as interactions between clouds and semi-volatile compounds, ammonia and nitric acid. These compounds are special in the sense that they co-condense together with water during cloud activation and have been suggested to form droplets that can be considered cloud-droplet-like already in subsaturated conditions. In our model, we calculate the kinetic partitioning of ammonia and sulfate thus explicitly taking into account the effect of ammonia and nitric acid in the cloud formation. Our simulations indicate that especially in polluted conditions, these compounds significantly affect the properties of cloud droplets thus significantly

  20. Observational evidence for the formation of DMS-derived aerosols during Arctic phytoplankton blooms

    Science.gov (United States)

    Park, Ki-Tae; Jang, Sehyun; Lee, Kitack; Yoon, Young Jun; Kim, Min-Seob; Park, Kihong; Cho, Hee-Joo; Kang, Jung-Ho; Udisti, Roberto; Lee, Bang-Yong; Shin, Kyung-Hoon

    2017-08-01

    The connection between marine biogenic dimethyl sulfide (DMS) and the formation of aerosol particles in the Arctic atmosphere was evaluated by analyzing atmospheric DMS mixing ratio, aerosol particle size distribution and aerosol chemical composition data that were concurrently collected at Ny-Ålesund, Svalbard (78.5° N, 11.8° E), during April and May 2015. Measurements of aerosol sulfur (S) compounds showed distinct patterns during periods of Arctic haze (April) and phytoplankton blooms (May). Specifically, during the phytoplankton bloom period the contribution of DMS-derived SO42- to the total aerosol SO42- increased by 7-fold compared with that during the proceeding Arctic haze period, and accounted for up to 70 % of fine SO42- particles (< 2.5 µm in diameter). The results also showed that the formation of submicron SO42- aerosols was significantly associated with an increase in the atmospheric DMS mixing ratio. More importantly, two independent estimates of the formation of DMS-derived SO42- aerosols, calculated using the stable S-isotope ratio and the non-sea-salt SO42- / methanesulfonic acid ratio, respectively, were in close agreement, providing compelling evidence that the contribution of biogenic DMS to the formation of aerosol particles was substantial during the Arctic phytoplankton bloom period.

  1. Ice nucleation in sulfuric acid/organic aerosols: implications for cirrus cloud formation

    Directory of Open Access Journals (Sweden)

    M. R. Beaver

    2006-01-01

    Full Text Available Using an aerosol flow tube apparatus, we have studied the effects of aliphatic aldehydes (C3 to C10 and ketones (C3 and C9 on ice nucleation in sulfuric acid aerosols. Mixed aerosols were prepared by combining an organic vapor flow with a flow of sulfuric acid aerosols over a small mixing time (~60 s at room temperature. No acid-catalyzed reactions were observed under these conditions, and physical uptake was responsible for the organic content of the sulfuric acid aerosols. In these experiments, aerosol organic content, determined by a Mie scattering analysis, was found to vary with the partial pressure of organic, the flow tube temperature, and the identity of the organic compound. The physical properties of the organic compounds (primarily the solubility and melting point were found to play a dominant role in determining the inferred mode of nucleation (homogenous or heterogeneous and the specific freezing temperatures observed. Overall, very soluble, low-melting organics, such as acetone and propanal, caused a decrease in aerosol ice nucleation temperatures when compared with aqueous sulfuric acid aerosol. In contrast, sulfuric acid particles exposed to organic compounds of eight carbons and greater, of much lower solubility and higher melting temperatures, nucleate ice at temperatures above aqueous sulfuric acid aerosols. Organic compounds of intermediate carbon chain length, C4-C7, (of intermediate solubility and melting temperatures nucleated ice at the same temperature as aqueous sulfuric acid aerosols. Interpretations and implications of these results for cirrus cloud formation are discussed.

  2. Parameterising secondary organic aerosol from α-pinene using a detailed oxidation and aerosol formation model

    Directory of Open Access Journals (Sweden)

    K. Ceulemans

    2012-06-01

    Full Text Available A new parameter model for α-pinene secondary organic aerosol (SOA is presented, based on simulations with the detailed model BOREAM (Biogenic hydrocarbon Oxidation and Related Aerosol formation Model. The parameterisation takes into account the influence of temperature, type of oxidant, NOx-regime, photochemical ageing and water uptake, and is suitable for use in global chemistry transport models. BOREAM is validated against recent photooxidation smog chamber experiments, for which it reproduces SOA yields to within a factor of 2 in most cases. In the simple chemical mechanism of the parameter model, oxidation of α-pinene generates peroxy radicals, which, upon reaction with NO or HO2, yield products corresponding to high or low-NOx conditions, respectively. The model parameters – i.e. the temperature-dependent stoichiometric coefficients and partitioning coefficients of 10 semi-volatile products – are obtained from simulations with BOREAM, including a prescribed diurnal cycle for the radiation, oxidant and emission levels, as well as a deposition sink for the particulate and gaseous products. The effects of photooxidative ageing are implicitly included in the parameterisation, since it is based on near-equilibrium SOA concentrations, obtained through simulations of a two-week period. In order to mimic the full BOREAM model results both during SOA build-up and when SOA has reached an equilibrium concentration, the revolatilisation of condensable products due to photochemical processes is taken into account through a fitted pseudo-photolysis reaction of the lumped semi-volatile products. Modelled SOA mass yields are about ten times higher in low-NOx than in high-NOx conditions, with yields of more than 50% in the low-NOx OH-initiated oxidation of α-pinene, considerably more than in previous parameterisations based on smog chamber experiments. Sensitivity calculations indicate

  3. Mechanisms of Formation of Secondary Organic Aerosols and Implications for Global Radiative Forcing

    Energy Technology Data Exchange (ETDEWEB)

    Seinfeld, John H. [California Inst. of Technology (CalTech), Pasadena, CA (United States)

    2011-12-02

    Organic material constitutes about 50% of global atmospheric aerosol mass, and the dominant source of organic aerosol is the oxidation of volatile hydrocarbons, to produce secondary organic aerosol (SOA). Understanding the formation of SOA is crucial to predicting present and future climate effects of atmospheric aerosols. The goal of this program is to significantly increase our understanding of secondary organic aerosol (SOA) formation in the atmosphere. Ambient measurements indicate that the amount of SOA in the atmosphere exceeds that predicted in current models based on existing laboratory chamber data. This would suggest that either the SOA yields measured in laboratory chambers are understated or that all major organic precursors have not been identified. In this research program we are systematically exploring these possibilities.

  4. MISR Level 3 FIRSTLOOK Global Aerosol product in netCDF format covering a day V002

    Data.gov (United States)

    National Aeronautics and Space Administration — The MISR Level 3 FIRSTLOOK Global Aerosol Product in netCDF format covering a day contains a statistical summary of column aerosol 555 nanometer optical depth, and a...

  5. Organic photolysis reactions in tropospheric aerosols: effect on secondary organic aerosol formation and lifetime

    Science.gov (United States)

    Hodzic, A.; Madronich, S.; Kasibhatla, P. S.; Tyndall, G.; Aumont, B.; Jimenez, J. L.; Lee-Taylor, J.; Orlando, J.

    2015-08-01

    This study presents the first modeling estimates of the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Typically only photolysis of smaller organic molecules (e.g., formaldehyde) for which explicit data exist is included in chemistry-climate models. Here, we specifically examine the photolysis of larger molecules that actively partition between the gas and particle phases. The chemical mechanism generator GECKO-A is used to explicitly model SOA formation from α-pinene, toluene, and C12 and C16 n-alkane reactions with OH at low and high NOx. Simulations are conducted for typical mid-latitude conditions and a solar zenith angle of 45° (permanent daylight). The results show that after 4 days of chemical aging under those conditions (equivalent to 8 days in the summer mid-latitudes), gas-phase photolysis leads to a moderate decrease in SOA yields, i.e., ~15 % (low NOx) to ~45 % (high NOx) for α-pinene, ~15 % for toluene, ~25 % for C12 n-alkane, and ~10 % for C16 n-alkane. The small effect of gas-phase photolysis on low-volatility n-alkanes such as C16 n-alkane is due to the rapid partitioning of early-generation products to the particle phase, where they are protected from gas-phase photolysis. Minor changes are found in the volatility distribution of organic products and in oxygen to carbon ratios. The decrease in SOA mass is increasingly more important after a day of chemical processing, suggesting that most laboratory experiments are likely too short to quantify the effect of gas-phase photolysis on SOA yields. Our results also suggest that many molecules containing chromophores are preferentially partitioned into the particle phase before they can be photolyzed in the gas phase. Given the growing experimental evidence that these molecules can undergo in-particle photolysis, we performed sensitivity simulations using an empirically estimated SOA photolysis rate of JSOA

  6. Gaseous ion-composition measurements in the young exhaust plume of jet aircraft at cruising altitudes. Implications for aerosols and gaseous sulfuric acid

    Energy Technology Data Exchange (ETDEWEB)

    Arnold, F.; Wohlfrom, K.H.; Klemm, M.; Schneider, J.; Gollinger, K. [Max-Planck-Inst. for Nuclear Physics, Heidelberg (Germany); Schumann, U.; Busen, R. [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Wessling (Germany). Inst. fuer Physik der Atmosphaere

    1997-12-31

    Mass spectrometric measurements were made in the young exhaust plume of an Airbus (A310) at cruising altitudes at distances between 400 and 800 m behind the Airbus (averaged plume age: 3.4 sec). The measurements indicate that gaseous sulfuric acid (GSA) number densities were less than 1.3 x 10{sup 8} cm{sup -3} which is smaller than the expected total sulfuric acid. Hence the missing sulfuric acid must have been in the aerosol phase. These measurements also indicate a total aerosol surface area density A{sub T} {<=} 5.4 x 10{sup -5} cm{sup 2} per cm{sup 3} which is consistent with simultaneously measured soot and water contrail particles. However, homogeneous nucleation leading to (H{sub 2}SO{sub 4}){sub x}(H{sub 2}O){sub y}-clusters can not be ruled out. (author) 16 refs.

  7. Numerical simulation of advection fog formation on multi-disperse aerosols due to combustion-related pollutants

    Science.gov (United States)

    Hung, R. J.; Liaw, G. S.

    1980-01-01

    The effects of multi-disperse distribution of the aerosol population are presented. Single component and multi-component aerosol species on the condensation/nucleation processes which affect the reduction in visibility are described. The aerosol population with a high particle concentration provided more favorable conditions for the formation of a denser fog than the aerosol population with a greater particle size distribution when the value of the mass concentration of the aerosols was kept constant. The results were used as numerical predictions of fog formation. Two dimensional observations in horizontal and vertical coordinates, together with time-dependent measurements were needed as initial values for the following physical parameters: (1)wind profiles; (2) temperature profiles; (3) humidity profiles; (4) mass concentration of aerosol particles; (5) particle size distribution of aerosols; and (6) chemical composition of aerosols. Formation and dissipation of advection fog, thus, can be forecasted numerically by introducing initial values obtained from the observations.

  8. Satellite remote sensing of dust aerosol indirect effects on ice cloud formation.

    Science.gov (United States)

    Ou, Steve Szu-Cheng; Liou, Kuo-Nan; Wang, Xingjuan; Hansell, Richard; Lefevre, Randy; Cocks, Stephen

    2009-01-20

    We undertook a new approach to investigate the aerosol indirect effect of the first kind on ice cloud formation by using available data products from the Moderate-Resolution Imaging Spectrometer (MODIS) and obtained physical understanding about the interaction between aerosols and ice clouds. Our analysis focused on the examination of the variability in the correlation between ice cloud parameters (optical depth, effective particle size, cloud water path, and cloud particle number concentration) and aerosol optical depth and number concentration that were inferred from available satellite cloud and aerosol data products. Correlation results for a number of selected scenes containing dust and ice clouds are presented, and dust aerosol indirect effects on ice clouds are directly demonstrated from satellite observations.

  9. Modelling of formation and distribution of secondary aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Andreani-Aksoyoglu, S.; Keller, J.; Baertsch-Ritter, N.; Prevot, A.S.H.; Dommen, J.; Baltensperger, U.

    2003-03-01

    The performance of aerosol modules of the 3-dimensional CAMx model was evaluated for the first time in a domain covering the Po Basin in northern Italy. The preliminary results for particulate species (especially those containing nitrate) smaller than 2.5 {mu}m were comparable to the values measured both in urban and rural stations. In most of the model domain, particulate NO{sub 3}{sup -} and NH{sub 4}{sup +} concentrations decreased with reduced NO{sub x} emissions. On the other hand, the levels of secondary organic carbon aerosols decreased with reduced VOC emissions, but increased with reduced NO{sub x} emissions similarly to ozone. Including aerosol chemistry in the model also affected the indicator values which are used for the ozone production sensitivities. (author)

  10. Potential of Aerosol Liquid Water to Facilitate Organic Aerosol Formation: Assessing Knowledge Gaps about Precursors and Partitioning.

    Science.gov (United States)

    Sareen, Neha; Waxman, Eleanor M; Turpin, Barbara J; Volkamer, Rainer; Carlton, Annmarie G

    2017-03-21

    Isoprene epoxydiol (IEPOX), glyoxal, and methylglyoxal are ubiquitous water-soluble organic gases (WSOGs) that partition to aerosol liquid water (ALW) and clouds to form aqueous secondary organic aerosol (aqSOA). Recent laboratory-derived Setschenow (or salting) coefficients suggest glyoxal's potential to form aqSOA is enhanced by high aerosol salt molality, or "salting-in". In the southeastern U.S., aqSOA is responsible for a significant fraction of ambient organic aerosol, and correlates with sulfate mass. However, the mechanistic explanation for this correlation remains elusive, and an assessment of the importance of different WSOGs to aqSOA is currently missing. We employ EPA's CMAQ model to the continental U.S. during the Southern Oxidant and Aerosol Study (SOAS) to compare the potential of glyoxal, methylglyoxal, and IEPOX to partition to ALW, as the initial step toward aqSOA formation. Among these three studied compounds, IEPOX is a dominant contributor, ∼72% on average in the continental U.S., to potential aqSOA mass due to Henry's Law constants and molecular weights. Glyoxal contributes significantly, and application of the Setschenow coefficient leads to a greater than 3-fold model domain average increase in glyoxal's aqSOA mass potential. Methylglyoxal is predicted to be a minor contributor. Acid or ammonium - catalyzed ring-opening IEPOX chemistry as well as sulfate-driven ALW and the associated molality may explain positive correlations between SOA and sulfate during SOAS and illustrate ways in which anthropogenic sulfate could regulate biogenic aqSOA formation, ways not presently included in atmospheric models but relevant to development of effective control strategies.

  11. Investigation of Deposit Formation Mechanisms for Engine In-cylinder Combustion and Exhaust Systems Using Quantitative Analysis and Sustainability Study

    Science.gov (United States)

    Ye, Z.; Meng, Q.; Mohamadian, H. P.; Wang, J. T.; Chen, L.; Zhu, L.

    2007-06-01

    The formation of SI engine combustion deposits is a complex phenomenon which depends on various factors of fuel, oil, additives, and engine. The goal of this study is to examine the effects of operating conditions, gasoline, lubricating oil, and additives on deposit formation. Both an experimental investigation and theoretical analysis are conducted on a single cylinder engine. As a result, the impact of deposits on engine performance and exhaust emissions (HC, NO x ) has been indicated. Using samples from a cylinder head and exhaust pipe as well as switching gases via the dual-gas method (N2, O2), the deposit formation mechanism is thoroughly investigated via the thermogravity analysis approach, where the roles of organic, inorganic, and volatile components of fuel, additives, and oil on deposit formation are identified from thermogravity curves. Sustainable feedback control design is then proposed for potential emission control and performance optimization

  12. Single particle mass spectral signatures from vehicle exhaust particles and the source apportionment of on-line PM2.5 by single particle aerosol mass spectrometry.

    Science.gov (United States)

    Yang, Jian; Ma, Shexia; Gao, Bo; Li, Xiaoying; Zhang, Yanjun; Cai, Jing; Li, Mei; Yao, Ling'ai; Huang, Bo; Zheng, Mei

    2017-09-01

    In order to accurately apportion the many distinct types of individual particles observed, it is necessary to characterize fingerprints of individual particles emitted directly from known sources. In this study, single particle mass spectral signatures from vehicle exhaust particles in a tunnel were performed. These data were used to evaluate particle signatures in a real-world PM2.5 apportionment study. The dominant chemical type originating from average positive and negative mass spectra for vehicle exhaust particles are EC species. Four distinct particle types describe the majority of particles emitted by vehicle exhaust particles in this tunnel. Each particle class is labeled according to the most significant chemical features in both average positive and negative mass spectral signatures, including ECOC, NaK, Metal and PAHs species. A single particle aerosol mass spectrometry (SPAMS) was also employed during the winter of 2013 in Guangzhou to determine both the size and chemical composition of individual atmospheric particles, with vacuum aerodynamic diameter (dva) in the size range of 0.2-2μm. A total of 487,570 particles were chemically analyzed with positive and negative ion mass spectra and a large set of single particle mass spectra was collected and analyzed in order to identify the speciation. According to the typical tracer ions from different source types and classification by the ART-2a algorithm which uses source fingerprints for apportioning ambient particles, the major sources of single particles were simulated. Coal combustion, vehicle exhaust, and secondary ion were the most abundant particle sources, contributing 28.5%, 17.8%, and 18.2%, respectively. The fraction with vehicle exhaust species particles decreased slightly with particle size in the condensation mode particles. Copyright © 2017 Elsevier B.V. All rights reserved.

  13. Influence of fuel ethanol content on primary emissions and secondary aerosol formation potential for a modern flex-fuel gasoline vehicle

    Science.gov (United States)

    Timonen, Hilkka; Karjalainen, Panu; Saukko, Erkka; Saarikoski, Sanna; Aakko-Saksa, Päivi; Simonen, Pauli; Murtonen, Timo; Dal Maso, Miikka; Kuuluvainen, Heino; Bloss, Matthew; Ahlberg, Erik; Svenningsson, Birgitta; Pagels, Joakim; Brune, William H.; Keskinen, Jorma; Worsnop, Douglas R.; Hillamo, Risto; Rönkkö, Topi

    2017-04-01

    The effect of fuel ethanol content (10, 85 and 100 %) on primary emissions and on subsequent secondary aerosol formation was investigated for a Euro 5 flex-fuel gasoline vehicle. Emissions were characterized during a New European Driving Cycle (NEDC) using a comprehensive set-up of high time-resolution instruments. A detailed chemical composition of the exhaust particulate matter (PM) was studied using a soot particle aerosol mass spectrometer (SP-AMS), and secondary aerosol formation was studied using a potential aerosol mass (PAM) chamber. For the primary gaseous compounds, an increase in total hydrocarbon emissions and a decrease in aromatic BTEX (benzene, toluene, ethylbenzene and xylenes) compounds was observed when the amount of ethanol in the fuel increased. In regard to particles, the largest primary particulate matter concentrations and potential for secondary particle formation was measured for the E10 fuel (10 % ethanol). As the ethanol content of the fuel increased, a significant decrease in the average primary particulate matter concentrations over the NEDC was found. The PM emissions were 0.45, 0.25 and 0.15 mg m-3 for E10, E85 and E100, respectively. Similarly, a clear decrease in secondary aerosol formation potential was observed with a larger contribution of ethanol in the fuel. The secondary-to-primary PM ratios were 13.4 and 1.5 for E10 and E85, respectively. For E100, a slight decrease in PM mass was observed after the PAM chamber, indicating that the PM produced by secondary aerosol formation was less than the PM lost through wall losses or the degradation of the primary organic aerosol (POA) in the chamber. For all fuel blends, the formed secondary aerosol consisted mostly of organic compounds. For E10, the contribution of organic compounds containing oxygen increased from 35 %, measured for primary organics, to 62 % after the PAM chamber. For E85, the contribution of organic compounds containing oxygen increased from 42 % (primary) to 57

  14. Synergetic formation of secondary inorganic and organic aerosol: effect of SO2 and NH3 on particle formation and growth

    Science.gov (United States)

    Chu, Biwu; Zhang, Xiao; Liu, Yongchun; He, Hong; Sun, Yele; Jiang, Jingkun; Li, Junhua; Hao, Jiming

    2016-11-01

    The effects of SO2 and NH3 on secondary organic aerosol formation have rarely been investigated together, while the interactive effects between inorganic and organic species under highly complex pollution conditions remain uncertain. Here we studied the effects of SO2 and NH3 on secondary aerosol formation in the photooxidation system of toluene/NOx in the presence or absence of Al2O3 seed aerosols in a 2 m3 smog chamber. The presence of SO2 increased new particle formation and particle growth significantly, regardless of whether NH3 was present. Sulfate, organic aerosol, nitrate, and ammonium were all found to increase linearly with increasing SO2 concentrations. The increases in these four species were more obvious under NH3-rich conditions, and the generation of nitrate, ammonium, and organic aerosol increased more significantly than sulfate with respect to SO2 concentration, while sulfate was the most sensitive species under NH3-poor conditions. The synergistic effects between SO2 and NH3 in the heterogeneous process contributed greatly to secondary aerosol formation. Specifically, the generation of NH4NO3 was found to be highly dependent on the surface area concentration of suspended particles, and increased most significantly with SO2 concentration among the four species under NH3-rich conditions. Meanwhile, the absorbed NH3 might provide a liquid surface layer for the absorption and subsequent reaction of SO2 and organic products and, therefore, enhance sulfate and secondary organic aerosol (SOA) formation. This effect mainly occurred in the heterogeneous process and resulted in a significantly higher growth rate of seed aerosols compared to without NH3. By applying positive matrix factorisation (PMF) analysis to the AMS data, two factors were identified for the generated SOA. One factor, assigned to less-oxidised organic aerosol and some oligomers, increased with increasing SO2 under NH3-poor conditions, mainly due to the well-known acid catalytic effect of

  15. Quantifying compositional impacts of ambient aerosol on cloud droplet formation

    Science.gov (United States)

    Lance, Sara

    It has been historically assumed that most of the uncertainty associated with the aerosol indirect effect on climate can be attributed to the unpredictability of updrafts. In Chapter 1, we analyze the sensitivity of cloud droplet number density, to realistic variations in aerosol chemical properties and to variable updraft velocities using a 1-dimensional cloud parcel model in three important environmental cases (continental, polluted and remote marine). The results suggest that aerosol chemical variability may be as important to the aerosol indirect effect as the effect of unresolved cloud dynamics, especially in polluted environments. We next used a continuous flow streamwise thermal gradient Cloud Condensation Nuclei counter (CCNc) to study the water-uptake properties of the ambient aerosol, by exposing an aerosol sample to a controlled water vapor supersaturation and counting the resulting number of droplets. In Chapter 2, we modeled and experimentally characterized the heat transfer properties and droplet growth within the CCNc. Chapter 3 describes results from the MIRAGE field campaign, in which the CCNc and a Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) were deployed at a ground-based site during March, 2006. Size-resolved CCN activation spectra and growth factor distributions of the ambient aerosol in Mexico City were obtained, and an analytical technique was developed to quantify a probability distribution of solute volume fractions for the CCN in addition to the aerosol mixing-state. The CCN were shown to be much less CCN active than ammonium sulfate, with water uptake properties more consistent with low molecular weight organic compounds. The pollution outflow from Mexico City was shown to have CCN with an even lower fraction of soluble material. "Chemical Closure" was attained for the CCN, by comparing the inferred solute volume fraction with that from direct chemical measurements. A clear diurnal pattern was observed for the CCN solute

  16. Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

    Directory of Open Access Journals (Sweden)

    B. Ervens

    2010-09-01

    Full Text Available This study presents a modeling framework based on laboratory data to describe the kinetics of glyoxal reactions that form secondary organic aerosol (SOA in aqueous aerosol particles. Recent laboratory results on glyoxal reactions are reviewed and a consistent set of empirical reaction rate constants is derived that captures the kinetics of glyoxal hydration and subsequent reversible and irreversible reactions in aqueous inorganic and water-soluble organic aerosol seeds. Products of these processes include (a oligomers, (b nitrogen-containing products, (c photochemical oxidation products with high molecular weight. These additional aqueous phase processes enhance the SOA formation rate in particles and yield two to three orders of magnitude more SOA than predicted based on reaction schemes for dilute aqueous phase (cloud chemistry for the same conditions (liquid water content, particle size.

    The application of the new module including detailed chemical processes in a box model demonstrates that both the time scale to reach aqueous phase equilibria and the choice of rate constants of irreversible reactions have a pronounced effect on the predicted atmospheric relevance of SOA formation from glyoxal. During day time, a photochemical (most likely radical-initiated process is the major SOA formation pathway forming ∼5 μg m−3 SOA over 12 h (assuming a constant glyoxal mixing ratio of 300 ppt. During night time, reactions of nitrogen-containing compounds (ammonium, amines, amino acids contribute most to the predicted SOA mass; however, the absolute predicted SOA masses are reduced by an order of magnitude as compared to day time production. The contribution of the ammonium reaction significantly increases in moderately acidic or neutral particles (5 < pH < 7.

    Glyoxal uptake into ammonium sulfate seed under dark conditions can be represented with a single reaction parameter keffupt that does not depend

  17. Effects of Diesel Engine Exhaust Origin Secondary Organic Aerosols on Novel Object Recognition Ability and Maternal Behavior in BALB/C Mice

    Directory of Open Access Journals (Sweden)

    Tin-Tin Win-Shwe

    2014-10-01

    Full Text Available Epidemiological studies have reported an increased risk of cardiopulmonary and lung cancer mortality associated with increasing exposure to air pollution. Ambient particulate matter consists of primary particles emitted directly from diesel engine vehicles and secondary organic aerosols (SOAs are formed by oxidative reaction of the ultrafine particle components of diesel exhaust (DE in the atmosphere. However, little is known about the relationship between exposure to SOA and central nervous system functions. Recently, we have reported that an acute single intranasal instillation of SOA may induce inflammatory response in lung, but not in brain of adult mice. To clarify the whole body exposure effects of SOA on central nervous system functions, we first created inhalation chambers for diesel exhaust origin secondary organic aerosols (DE-SOAs produced by oxidation of diesel exhaust particles caused by adding ozone. Male BALB/c mice were exposed to clean air (control, DE and DE-SOA in inhalation chambers for one or three months (5 h/day, 5 days/week and were examined for memory function using a novel object recognition test and for memory function-related gene expressions in the hippocampus by real-time RT-PCR. Moreover, female mice exposed to DE-SOA for one month were mated and maternal behaviors and the related gene expressions in the hypothalamus examined. Novel object recognition ability and N-methyl-D-aspartate (NMDA receptor expression in the hippocampus were affected in male mice exposed to DE-SOA. Furthermore, a tendency to decrease maternal performance and significantly decreased expression levels of estrogen receptor (ER-a, and oxytocin receptor were found in DE-SOA exposed dams compared with the control. This is the first study of this type and our results suggest that the constituents of DE-SOA may be associated with memory function and maternal performance based on the impaired gene expressions in the hippocampus and hypothalamus

  18. Secondary organic aerosol formation from biomass burning intermediates: phenol and methoxyphenols

    Directory of Open Access Journals (Sweden)

    L. D. Yee

    2013-08-01

    Full Text Available The formation of secondary organic aerosol from oxidation of phenol, guaiacol (2-methoxyphenol, and syringol (2,6-dimethoxyphenol, major components of biomass burning, is described. Photooxidation experiments were conducted in the Caltech laboratory chambers under low-NOx (2O2 as the OH source. Secondary organic aerosol (SOA yields (ratio of mass of SOA formed to mass of primary organic reacted greater than 25% are observed. Aerosol growth is rapid and linear with the primary organic conversion, consistent with the formation of essentially non-volatile products. Gas- and aerosol-phase oxidation products from the guaiacol system provide insight into the chemical mechanisms responsible for SOA formation. Syringol SOA yields are lower than those of phenol and guaiacol, likely due to novel methoxy group chemistry that leads to early fragmentation in the gas-phase photooxidation. Atomic oxygen to carbon (O : C ratios calculated from high-resolution-time-of-flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS measurements of the SOA in all three systems are ~ 0.9, which represent among the highest such ratios achieved in laboratory chamber experiments and are similar to that of aged atmospheric organic aerosol. The global contribution of SOA from intermediate volatility and semivolatile organic compounds has been shown to be substantial (Pye and Seinfeld, 2010. An approach to representing SOA formation from biomass burning emissions in atmospheric models could involve one or more surrogate species for which aerosol formation under well-controlled conditions has been quantified. The present work provides data for such an approach.

  19. Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation.

    Science.gov (United States)

    Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K; Wagner, Robert; Dunne, Eimear M; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P; Pringle, Kirsty J; Richards, Nigel A D; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E; Seinfeld, John H; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C; Wagner, Paul E; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M; Worsnop, Douglas R; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S

    2016-10-25

    The magnitude of aerosol radiative forcing caused by anthropogenic emissions depends on the baseline state of the atmosphere under pristine preindustrial conditions. Measurements show that particle formation in atmospheric conditions can occur solely from biogenic vapors. Here, we evaluate the potential effect of this source of particles on preindustrial cloud condensation nuclei (CCN) concentrations and aerosol-cloud radiative forcing over the industrial period. Model simulations show that the pure biogenic particle formation mechanism has a much larger relative effect on CCN concentrations in the preindustrial atmosphere than in the present atmosphere because of the lower aerosol concentrations. Consequently, preindustrial cloud albedo is increased more than under present day conditions, and therefore the cooling forcing of anthropogenic aerosols is reduced. The mechanism increases CCN concentrations by 20-100% over a large fraction of the preindustrial lower atmosphere, and the magnitude of annual global mean radiative forcing caused by changes of cloud albedo since 1750 is reduced by [Formula: see text] (27%) to [Formula: see text] Model uncertainties, relatively slow formation rates, and limited available ambient measurements make it difficult to establish the significance of a mechanism that has its dominant effect under preindustrial conditions. Our simulations predict more particle formation in the Amazon than is observed. However, the first observation of pure organic nucleation has now been reported for the free troposphere. Given the potentially significant effect on anthropogenic forcing, effort should be made to better understand such naturally driven aerosol processes.

  20. Properties of aerosols and formation mechanisms over southern China during the monsoon season

    Directory of Open Access Journals (Sweden)

    W. Chen

    2016-10-01

    Full Text Available Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May–June in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (< 2.5 µm. Sulfate was found to be strongly correlated with aerosol water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.

  1. Secondary Organic Aerosol Coating Formation and Evaporation: Chamber Studies Using Black Carbon Seed Aerosol and the Single-Particle Soot Photometer

    OpenAIRE

    Metcalf, Andrew R.; Loza, Christine L.; Coggon, Matthew M.; Craven, Jill S; Haflidi H. Jonsson; Flagan, Richard C; Seinfeld, John H.

    2013-01-01

    The article of record as published may be found at http://dx.doi.org/10.1080/02786826.2012.750712 We report a protocol for using black carbon (BC) aerosol as the seed for secondary organic aerosol (SOA) formation in an environmental chamber. We employ a single-particle soot photometer (SP2) to probe single-particle SOA coating growth dynamics and find that SOA growth on nonspherical BC aerosol is diffusion- limited. Aerosol composition measurements with an Aerodyne high resolution time-of-...

  2. Characterization of ambient aerosol composition and formation mechanisms and development of quantification methodologies utilizing ATOFMS

    Science.gov (United States)

    Qin, Xueying

    Aerosols are solid or liquid particles suspended in the air. They are generated from a range of natural and anthropogenic sources. Aerosols also experience various reactions such as photo-oxidation and aqueous-phase processing, which constantly change their physical and chemical properties. Therefore, in order to determine the emission inventory, it is important to study aerosol reactions and transformation mechanisms in ambient atmosphere. The research described in this dissertation aimed to characterize temporal, spatial, and seasonal variations on ambient aerosol chemical compositions and formation mechanisms. The results contribute to the understanding of air pollution, climate change, and human health problems, and to devising necessary strategies and policies to resolve these problems. The main experimental technique utilized in the current work is Aerosol time-of-flight mass spectrometry (ATOFMS). It measures the size and chemical composition of individual particles in real-time, and can thus provide high time resolution information on aerosol mixing states, reaction mechanisms, and sources. Continuous ATOFMS measurements have been conducted to study the ambient aerosol properties in several highly polluted regions of California, including the Fresno and Angiola area and the Riverside area. The results provide important insights on the characteristics, distinct diurnal temporal trends, and seasonal variations of aerosols in both urban and rural locations. The second focus of this dissertation is on the quantification capability of ATOFMS, which had been limited by several factors including the size-dependant particle transmission loss and shot-to-shot variability of the desorption/ionization laser. It is demonstrated that, by scaling the ATOFMS measurements using the results from an aerodynamic particle sizer (APS) or a micro-orifice uniform deposit impactor (MOUDI) measurements, it is possible to obtain high temporal resolution mass concentrations from

  3. The formation of aerosol particles during combustion of biomass and waste. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Hjerrild Zeuthen, J.

    2007-05-15

    This thesis describes the formation of aerosol particles during combustion of biomass and waste. The formation of aerosol particles is investigated by studying condensation of alkali salts from synthetic flue gasses in a laboratory tubular furnace. In this so-called laminar flow aerosol condenser-furnace gaseous alkali chlorides are mixed with sulphur dioxide, water vapour and oxygen. At high temperatures the alkali chloride reacts with sulphur dioxide to form alkali sulphate. During subsequent cooling of the synthetic flue gas the chlorides and sulphates condense either as deposits on walls or on other particles or directly from the gas phase by homogenous nucleation. A previously developed computer code for simulation of one-component nucleation of particles in a cylindrical laminar flow is extended to include a homogeneous gas phase reaction to produce gaseous alkali sulphate. The formation of aerosol particles during full-scale combustion of wheat straw is investigated in a 100 MW grate-fired boiler. Finally, aerosols from incineration of waste are investigated during full-scale combustion of municipal waste in a 22 MW grate-fired unit. (BA)

  4. Secondary organic aerosol formation through fog processing of VOCs

    Science.gov (United States)

    Herckes, P.; Hutchings, J. W.

    2010-07-01

    Volatile Organic Compounds (VOCs) including benzene, toluene, ethylbenzene and xylenes (BTEX) have been determined in highly concentrated amounts (>1 ug/L) in intercepted clouds in northern Arizona (USA). These VOCs are found in concentrations much higher than predicted by partitioning alone. The reactivity of BTEX in the fog/cloud aqueous phase was investigated through laboratory studies. BTEX species showed fast degradation in the aqueous phase in the presence of peroxides and light. Observed half-lives ranged from three and six hours, substantially shorter than the respective gas phase half-lives (several days). The observed reaction rates were on the order of 1 ppb/min but decreased substantially with increasing concentrations of organic matter (TOC). The products of BTEX oxidation reactions were analyzed using HPLC-UV and LCMS. The first generation of products identified included phenol and cresols which correspond to the hydroxyl-addition reaction to benzene and toluene. Upon investigating of multi-generational products, smaller, less volatile species are predominant although a large variety of products is found. Most reaction products have substantially lower vapor pressure and will remain in the particle phase upon droplet evaporation. The SOA generation potential of cloud and fog processing of BTEX was evaluated using simple calculations and showed that in ideal situations these reactions could add up to 9% of the ambient aerosol mass. In more conservative scenarios, the contribution of the processing of BTEX was around 1% of ambient aerosol concentrations. Overall, cloud processing of VOC has the potential to contribute to the atmospheric aerosol mass. However, the contribution will depend upon many factors such as the irradiation, organic matter content in the droplets and droplet lifetime.

  5. Thresholds of secondary organic aerosol formation by ozonolysis of monoterpenes measured in a laminar flow aerosol reactor

    OpenAIRE

    Bernard, François; Fedioun, Ivan; Peyroux, Fabrice; Quilgars, Alain; Daële, Véronique; Mellouki, Abdelwahid

    2012-01-01

    International audience; The reactions of ozone with a series of monoterpenes (α-pinene, sabinene, limonene and myrcene) were investigated in a novel flow reactor dedicated to the investigation of secondary organic aerosol (SOA) formation. Rate constants for the gas phase reactions and nucleation thresholds were determined at T∼296 K, P∼764 Torr under dry conditions (dew point ≤−33 °C) and in absence of OH radicals scavenger and seed particles. Comparison with the literature as well as data fr...

  6. Formation of aerosols in and after the flame

    DEFF Research Database (Denmark)

    Dederichs, Anne

    Bildning av aerosoler har en stor betydelse i brandsammanhang. Aerosoler, härtill räknas partiklar och vätskedroppar, bildas i bränder, de påverkar flamspridning och minskar siktbarheten. Därmed är de avgörande för evakuering. De är ofta toxiska och ställer till problem för människa och miljö. Ae...... fasta partiklar bör och kan överföras till droppar och inkluderas i CFD modeller. Eftersom sådan forskning leder till ökat behov av CPU tid, rekommenderas en satsning på hardware programmering, en forskningsdisciplin som redan används för tunga beräkningar....... områden anses vara viktiga: o Aerosolernas bildningsprocess. o Heterogena reaktioner och partiklarnas sammansättning. o Aerosolernas ändring med tiden. Processen kallas för åldring och hänvisar till olika tidsintervall för de tre forskningsgrenarna. Men alla anses vara viktiga. Kunskap och modeller från...

  7. The role of HO_x in super- and subsonic aircraft exhaust plumes

    OpenAIRE

    Hanisco, T. F.; Wennberg, P. O.; R. C. Cohen; J. G. Anderson; D. W. Fahey; Keim, E. R; Gao, R. S.; Wamsley, R. C.; Donnelly, S. G.; Del Negro, L. A.; R. J. Salawitch; Kelly, K. K.; Proffitt, M.H.

    1997-01-01

    The generation of sulfuric acid aerosols in aircraft exhaust has emerged as a critical issue in determining the impact of supersonic aircraft on stratospheric ozone. It has long been held that the first step in the mechanism of aerosol formation is the oxidation of SO_(2) emitted from the engine by OH in the exhaust plume. We report in situ measurements of OH and HO_(2) in the exhaust plumes of a supersonic (Air France Concorde) and a subsonic (NASA ER-2) aircraft in the lower stratosphere. T...

  8. Missing ozone-induced potential aerosol formation in a suburban deciduous forest

    Science.gov (United States)

    Nakayama, T.; Kuruma, Y.; Matsumi, Y.; Morino, Y.; Sato, K.; Tsurumaru, H.; Ramasamy, S.; Sakamoto, Y.; Kato, S.; Miyazaki, Y.; Mochizuki, T.; Kawamura, K.; Sadanaga, Y.; Nakashima, Y.; Matsuda, K.; Kajii, Y.

    2017-12-01

    As a new approach to investigating formation processes of secondary organic aerosol (SOA) in the atmosphere, ozone-induced potential aerosol formation was measured in summer at a suburban forest site surrounded by deciduous trees, near Tokyo, Japan. After passage through a reactor containing high concentrations of ozone, increases in total particle volume (average of 1.4 × 109 nm3/cm3, which corresponds to 17% that of pre-existing particles) were observed, especially during daytime. The observed aerosol formations were compared with the results of box model simulations using simultaneously measured concentrations of gaseous and particulate species. According to the model, the relative contributions of isoprene, monoterpene, and aromatic hydrocarbon oxidation to SOA formation in the reactor were 24, 21, and 55%, respectively. However, the model could explain, on average, only ∼40% of the observed particle formation, and large discrepancies between the observations and model were found, especially around noon and in the afternoon when the concentrations of isoprene and oxygenated volatile organic compounds were high. The results suggest a significant contribution of missing (unaccounted-for) SOA formation processes from identified and/or unidentified volatile organic compounds, especially those emitted during daytime. Further efforts should be made to explore and parameterize this missing SOA formation to assist in the improvement of atmospheric chemistry and climate models.

  9. Properties of aerosols and formation mechanisms over southern China during the monsoon season

    Science.gov (United States)

    Chen, Weihua; Wang, Xuemei; Blake Cohen, Jason; Zhou, Shengzhen; Zhang, Zhisheng; Chang, Ming; Chan, Chuen-Yu

    2016-10-01

    Measurements of size-resolved aerosols from 0.25 to 18 µm were conducted at three sites (urban, suburban and background sites) and used in tandem with an atmospheric transport model to study the size distribution and formation of atmospheric aerosols in southern China during the monsoon season (May-June) in 2010. The mass distribution showed the majority of chemical components were found in the smaller size bins (water and anticorrelated with atmospheric SO2, hinting at aqueous-phase reactions being the main formation pathway. Nitrate was the only major species that showed a bimodal distribution at the urban site and was dominated by the coarse mode in the other two sites, suggesting that an important component of nitrate formation is chloride depletion of sea salt transported from the South China Sea. In addition to these aqueous-phase reactions and interactions with sea salt aerosols, new particle formation, chemical aging, and long-range transport from upwind urban or biomass burning regions was also found to be important in at least some of the sites on some of the days. This work therefore summarizes the different mechanisms that significantly impact the aerosol chemical composition during the monsoon over southern China.

  10. Sub 2 nm Particle Characterization in Systems with Aerosol Formation and Growth

    Science.gov (United States)

    Wang, Yang

    Aerosol science and technology enable continual advances in material synthesis and atmospheric pollutant control. Among these advances, one important frontier is characterizing the initial stages of particle formation by real time measurement of particles below 2 nm in size. Sub 2 nm particles play important roles by acting as seeds for particle growth, ultimately determining the final properties of the generated particles. Tailoring nanoparticle properties requires a thorough understanding and precise control of the particle formation processes, which in turn requires characterizing nanoparticle formation from the initial stages. The knowledge on particle formation in early stages can also be applied in quantum dot synthesis and material doping. This dissertation pursued two approaches in investigating incipient particle characterization in systems with aerosol formation and growth: (1) using a high-resolution differential mobility analyzer (DMA) to measure the size distributions of sub 2 nm particles generated from high-temperature aerosol reactors, and (2) analyzing the physical and chemical pathways of aerosol formation during combustion. Part. 1. Particle size distributions reveal important information about particle formation dynamics. DMAs are widely utilized to measure particle size distributions. However, our knowledge of the initial stages of particle formation is incomplete, due to the Brownian broadening effects in conventional DMAs. The first part of this dissertation studied the applicability of high-resolution DMAs in characterizing sub 2 nm particles generated from high-temperature aerosol reactors, including a flame aerosol reactor (FLAR) and a furnace aerosol reactor (FUAR). Comparison against a conventional DMA (Nano DMA, Model 3085, TSI Inc.) demonstrated that the increased sheath flow rates and shortened residence time indeed greatly suppressed the diffusion broadening effect in a high-resolution DMA (half mini type). The incipient particle

  11. Halogen-induced organic aerosol (XOA): a study on ultra-fine particle formation and time-resolved chemical characterization.

    Science.gov (United States)

    Ofner, Johannes; Kamilli, Katharina A; Held, Andreas; Lendl, Bernhard; Zetzsch, Cornelius

    2013-01-01

    The concurrent presence of high values of organic SOA precursors and reactive halogen species (RHS) at very low ozone concentrations allows the formation of halogen-induced organic aerosol, so-called XOA, in maritime areas where high concentrations of RHS are present, especially at sunrise. The present study combines aerosol smog-chamber and aerosol flow-reactor experiments for the characterization of XOA. XOA formation yields from alpha-pinene at low and high concentrations of chlorine as reactive halogen species (RHS) were determined using a 700 L aerosol smog-chamber with a solar simulator. The chemical transformation of the organic precursor during the aerosol formation process and chemical aging was studied using an aerosol flow-reactor coupled to an FTIR spectrometer. The FTIR dataset was analysed using 2D correlation spectroscopy. Chlorine induced homogeneous XOA formation takes place at even 2.5 ppb of molecular chlorine, which was photolysed by the solar simulator. The chemical pathway of XOA formation is characterized by the addition of chlorine and abstraction of hydrogen atoms, causing simultaneous carbon-chlorine bond formation. During further steps of the formation process, carboxylic acids are formed, which cause a SOA-like appearance of XOA. During the ozone-free formation of secondary organic aerosol with RHS a special kind of particulate matter (XOA) is formed, which is afterwards transformed to SOA by atmospheric aging or degradation pathways.

  12. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

    Science.gov (United States)

    Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

    2013-07-16

    Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

  13. Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

    Science.gov (United States)

    Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

    2013-12-01

    The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles cloud formation and potential

  14. Formation of Oxidized Organic Aerosol (OOA) through Fog Processing in the Po Valley

    Science.gov (United States)

    Gilardoni, S.; Paglione, M.; Rinaldi, M.; Giulianelli, L.; Massoli, P.; Hillamo, R. E.; Carbone, S.; Lanconelli, C.; Laaksonen, A. J.; Russell, L. M.; Poluzzi, V.; Fuzzi, S.; Facchini, C.

    2014-12-01

    Aqueous phase chemistry might be responsible for the formation of a significant fraction of the organic aerosol (OA) observed in the atmosphere, and could explain some of the discrepancies between OA concentration and properties predicted by models and observed in the environment. Aerosol - fog interaction and its effect on submicron aerosol properties were investigated in the Po Valley (northern Italy) during fall 2011, in the framework of the Supersite project (ARPA Emilia Romagna). Composition and physical properties of submicron aerosol were measured online by a High Resolution- Time of Flight - Aerosol Mass Spectrometer (HR-TOF-AMS), a Soot Photometer - Aerosol Mass Spectrometer (SP-AMS), and a Tandem Differential Mobility Particle Sizer (TDMPS). Organic functional group analysis was performed off-line by Hydrogen - Nuclear Magnetic Resonance (H-NMR) spectrometry and by Fourier Transform Infrared (FTIR) spectrometry. Aerosol absorption, scattering, and total extinction were measured simultaneously with a Particle Soot Absorption Photometer (PSAP), a Nephelometer, and a Cavity Attenuated Phase Shift Spectrometer particle extinction monitor (CAPS PMex), respectively. Water-soluble organic carbon in fog-water was characterized off-line by HR-TOF-AMS. Fourteen distinct fog events were observed. Fog dissipation left behind an aerosol enriched in particles larger than 400 nm, typical of fog and cloud processing, and dominated by secondary species, including ammonium nitrate, ammonium sulfate and oxidized OA (OOA). Source apportionment of OA allowed us to identify OOA as the difference between total OA and primary OA (hydrocarbon like OA and biomass burning OA). The formation of OOA through fog processing is proved by the correlation of OOA concentration with hydroxyl methyl sulfonate signal and by the similarity of OOA spectra with organic mass spectra obtained by re-aerosolization of fog water samples. The oxygen to carbon ratio and the hydrogen to carbon ratio of

  15. Aerosol Formation during the Combustion of Straw with Addition of Sorbents

    DEFF Research Database (Denmark)

    Zeuthen, Frederik Jacob; Jensen, Peter Arendt; Jensen, Jørgen P.

    2007-01-01

    The influence of six sorbents on aerosol formation during the combustion of straw in a 100 MW boiler on a Danish power plant has been studied in full-scale. The following sorbents were studied: ammonium sulfate, monocalcium phosphate, Bentonite, ICA5000, clay, and chalk. Bentonite and ICA5000......, calcium phosphate, Bentonite, ICA5000, and clay. The addition of chalk increased the aerosol mass concentration by 24%. Experiments in a laminar flow aerosol condenser with the six sorbents were carried out in the laboratory using a synthetic flue gas to avoid fluctuations in the alkali feeding...... are mixtures of clay minerals and consist mainly of the oxides from Fe, Al, and Si. The straw used was Danish wheat and seed grass. Measurements were also made with increased flow of primary air. The experiments showed between 46% and 70% reduction in particle mass concentrations when adding ammonium sulfate...

  16. Formation characteristics of aerosol particles from pulverized coal pyrolysis in high-temperature environments.

    Science.gov (United States)

    Chen, Wei-Hsin; Du, Shan-Wen; Yang, Hsi-Hsien; Wu, Jheng-Syun

    2008-05-01

    The formation characteristics of aerosol particles from pulverized coal pyrolysis in high temperatures are studied experimentally. By conducting a drop-tube furnace, fuel pyrolysis processes in industrial furnaces are simulated in which three different reaction temperatures of 1000, 1200, and 1400 degrees C are considered. Experimental observations indicate that when the reaction temperature is 1000 degrees C, submicron particles are produced, whereas the particle size is dominated by nanoscale for the temperature of 1400 degrees C. Thermogravimetric analysis of the aerosol particles stemming from the pyrolysis temperature of 1000 degrees C reveals that the thermal behavior of the aerosol is characterized by a three-stage reaction with increasing heating temperature: (1) a volatile-reaction stage, (2) a weak-reaction stage, and (3) a soot-reaction stage. However, with the pyrolysis temperature of 1400 degrees C, the volatile- and weak-reaction stages almost merge together and evolve into a chemical-frozen stage. The submicron particles (i.e., 1000 degrees C) are mainly composed of volatiles, tar, and soot, with the main component of the nanoscale particles (i.e., 1400 degrees C) being soot. The polycyclic aromatic hydrocarbons (PAHs) contained in the aerosols are also analyzed. It is found that the PAH content in generated aerosols decreases dramatically as the pyrolysis temperature increases.

  17. Atmospheric aerosol formation and its growth during the cold ...

    Indian Academy of Sciences (India)

    mid-point diameter 13 nm and it is due to photo-chemical nucleation, coagulation and coalescence among nucleated clusters. The ratios of real to ... Atmospheric new particle formation processes contribute significantly to the global ..... It is desirable to quantify the influence of mole- cular mass and diffusivity of vapours of ...

  18. Measurements of organic gases during aerosol formation events in the boreal forest atmosphere during QUEST

    Directory of Open Access Journals (Sweden)

    K. Sellegri

    2005-01-01

    Full Text Available Biogenic VOCs are important in the growth and possibly also in the early stages of formation of atmospheric aerosol particles. In this work, we present 10 min-time resolution measurements of organic trace gases at Hyytiälä, Finland during March 2002. The measurements were part of the project QUEST (Quantification of Aerosol Nucleation in the European Boundary Layer and took place during a two-week period when nucleation events occurred with various intensities nearly every day. Using a ground-based Chemical Ionization Mass Spectrometer (CIMS instrument, the following trace gases were detected: acetone, TMA, DMA, mass 68amu (candidate=isoprene, monoterpenes, methyl vinyl ketone (MVK and methacrolein (MaCR and monoterpene oxidation products (MTOP. For all of them except for the amines, we present daily variations during different classes of nucleation events, and non-event days. BVOC oxidation products (MVK, MaCR and MTOP show a higher ratio to the CS on event days compared to non-event days, indicating that their abundance relative to the surface of aerosol available is higher on nucleation days. Moreover, BVOC oxidation products are found to show significant correlations with the condensational sink (CS on nucleation event days, which indicates that they are representative of less volatile organic compounds that contribute to the growth of the nucleated particles and generally secondary organic aerosol formation. Behaviors of BVOC on event and non event days are compared to the behavior of CO.

  19. Aqueous chemistry and its role in secondary organic aerosol (SOA formation

    Directory of Open Access Journals (Sweden)

    Y. B. Lim

    2010-11-01

    Full Text Available There is a growing understanding that secondary organic aerosol (SOA can form through reactions in atmospheric waters (i.e., clouds, fogs, and aerosol water. In clouds and wet aerosols, water-soluble organic products of gas-phase photochemistry dissolve into the aqueous phase where they can react further (e.g., with OH radicals to form low volatility products that are largely retained in the particle phase. Organic acids, oligomers and other products form via radical and non-radical reactions, including hemiacetal formation during droplet evaporation, acid/base catalysis, and reaction of organics with other constituents (e.g., NH4+.

    This paper provides an overview of SOA formation through aqueous chemistry, including atmospheric evidence for this process and a review of radical and non-radical chemistry, using glyoxal as a model precursor. Previously unreported analyses and new kinetic modeling are reported herein to support the discussion of radical chemistry. Results suggest that reactions with OH radicals tend to be faster and form more SOA than non-radical reactions. In clouds these reactions yield organic acids, whereas in wet aerosols they yield large multifunctional humic-like substances formed via radical-radical reactions and their O/C ratios are near 1.

  20. High formation of secondary organic aerosol from the photo-oxidation of toluene

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2009-05-01

    Full Text Available Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental conditions: yields are higher under higher UV intensity, under low-NOx conditions and at lower temperatures. The extent of oxidation of the aerosol also varies with experimental conditions, consistent with ongoing, progressive photochemical aging of the toluene SOA. Measurements using a thermodenuder system suggest that the aerosol formed under high- and low-NOx conditions is semi-volatile. These results suggest that SOA formation from toluene depends strongly on ambient conditions. An approximate parameterization is proposed for use in air-quality models until a more thorough treatment accounting for the dynamic nature of this system becomes available.

  1. Carbonyl emissions from heavy-duty diesel vehicle exhaust in China and the contribution to ozone formation potential.

    Science.gov (United States)

    Dong, Dong; Shao, Min; Li, Yue; Lu, Sihua; Wang, Yanjun; Ji, Zhe; Tang, Dagang

    2014-01-01

    Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4-dinitrophenyhydrazine cartridge and 23 carbonyl compounds were analyzed by high performance liquid chromatography. The average emission factor of carbonyls was 97.2 mg/km, higher than that of light-duty diesel vehicles and gasoline-powered vehicles. Formaldehyde, acetaldehyde, acetone and propionaldehyde were the species with the highest emission factors. Main influencing factors for carbonyl emissions were vehicle type, average speed and regulated emission standard, and the impact of vehicle loading was not evident in this study. National emission of carbonyls from diesel vehicles exhaust was calculated for China, 2011, based on both vehicle miles traveled and fuel consumption. Carbonyl emission of diesel vehicle was estimated to be 45.8 Gg, and was comparable to gasoline-powered vehicles (58.4 Gg). The emissions of formaldehyde, acetaldehyde and acetone were 12.6, 6.9, 3.8 Gg, respectively. The ozone formation potential of carbonyls from diesel vehicles exhaust was 537 mg O3/km, higher than 497 mg O3/km of none-methane hydrocarbons emitted from diesel vehicles.

  2. Rapid Formation of Molecular Bromine from Deliquesced NaBr Aerosol in the Presence of Ozone and UV Light

    Science.gov (United States)

    The formation of gas-phase bromine from aqueous sodium bromide aerosols is investigated through a combination of chamber experiments and chemical kinetics modeling. Experiments show that Br2(g) is produced rapidly from deliquesced NaBr aerosols in the presence of OH radicals prod...

  3. The formation, properties and impact of secondary organic aerosol: current and emerging issues

    Directory of Open Access Journals (Sweden)

    J. Wildt

    2009-07-01

    Full Text Available Secondary organic aerosol (SOA accounts for a significant fraction of ambient tropospheric aerosol and a detailed knowledge of the formation, properties and transformation of SOA is therefore required to evaluate its impact on atmospheric processes, climate and human health. The chemical and physical processes associated with SOA formation are complex and varied, and, despite considerable progress in recent years, a quantitative and predictive understanding of SOA formation does not exist and therefore represents a major research challenge in atmospheric science. This review begins with an update on the current state of knowledge on the global SOA budget and is followed by an overview of the atmospheric degradation mechanisms for SOA precursors, gas-particle partitioning theory and the analytical techniques used to determine the chemical composition of SOA. A survey of recent laboratory, field and modeling studies is also presented. The following topical and emerging issues are highlighted and discussed in detail: molecular characterization of biogenic SOA constituents, condensed phase reactions and oligomerization, the interaction of atmospheric organic components with sulfuric acid, the chemical and photochemical processing of organics in the atmospheric aqueous phase, aerosol formation from real plant emissions, interaction of atmospheric organic components with water, thermodynamics and mixtures in atmospheric models. Finally, the major challenges ahead in laboratory, field and modeling studies of SOA are discussed and recommendations for future research directions are proposed.

  4. Simulating SAL formation and aerosol size distribution during SAMUM-I

    KAUST Repository

    Khan, Basit Ali

    2015-04-01

    To understand the formation mechanisms of Saharan Air Layer (SAL), we combine model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM-I), which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. We employed the Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF-Chem) to reproduce the meteorological environment and spatial and size distributions of dust. The experimental domain covers northwest Africa including the southern Sahara, Morocco and part of the Atlantic Ocean with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of most intensive dust outbreaks. Comparisons of model results with available airborne and ground-based observations show that WRF-Chem reproduces observed meteorological fields as well as aerosol spatial distribution across the entire region and along the airplane\\'s tracks. We evaluated several aerosol uplift processes and found that orographic lifting, aerosol transport through the land/sea interface with steep gradients of meteorological characteristics, and interaction of sea breezes with the continental outflow are key mechanisms that form a surface-detached aerosol plume over the ocean. Comparisons of simulated dust size distributions with airplane and ground-based observations are generally good, but suggest that more detailed treatment of microphysics in the model is required to capture the full-scale effect of large aerosol particles.

  5. Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

    Directory of Open Access Journals (Sweden)

    T. Liu

    2017-06-01

    Full Text Available Cooking emissions can potentially contribute to secondary organic aerosol (SOA but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils was investigated in a potential aerosol mass (PAM chamber. Experiments were conducted at 19–20 °C and 65–70 % relative humidity (RH. The characterization instruments included a scanning mobility particle sizer (SMPS and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS. The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm−3 s, was 1. 35 ± 0. 30 µg min−1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5 from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc of SOA was −1.51 to −0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA and semi-volatile oxygenated organic aerosol (SV-OOA, indicating that SOA in these experiments was lightly oxidized.

  6. Formation of secondary organic aerosols from gas-phase emissions of heated cooking oils

    Science.gov (United States)

    Liu, Tengyu; Li, Zijun; Chan, ManNin; Chan, Chak K.

    2017-06-01

    Cooking emissions can potentially contribute to secondary organic aerosol (SOA) but remain poorly understood. In this study, formation of SOA from gas-phase emissions of five heated vegetable oils (i.e., corn, canola, sunflower, peanut and olive oils) was investigated in a potential aerosol mass (PAM) chamber. Experiments were conducted at 19-20 °C and 65-70 % relative humidity (RH). The characterization instruments included a scanning mobility particle sizer (SMPS) and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS). The efficiency of SOA production, in ascending order, was peanut oil, olive oil, canola oil, corn oil and sunflower oil. The major SOA precursors from heated cooking oils were related to the content of monounsaturated fat and omega-6 fatty acids in cooking oils. The average production rate of SOA, after aging at an OH exposure of 1. 7 × 1011 molecules cm-3 s, was 1. 35 ± 0. 30 µg min-1, 3 orders of magnitude lower compared with emission rates of fine particulate matter (PM2. 5) from heated cooking oils in previous studies. The mass spectra of cooking SOA highly resemble field-derived COA (cooking-related organic aerosol) in ambient air, with R2 ranging from 0.74 to 0.88. The average carbon oxidation state (OSc) of SOA was -1.51 to -0.81, falling in the range between ambient hydrocarbon-like organic aerosol (HOA) and semi-volatile oxygenated organic aerosol (SV-OOA), indicating that SOA in these experiments was lightly oxidized.

  7. Formation and occurrence of dimer esters of pinene oxidation products in atmospheric aerosols

    DEFF Research Database (Denmark)

    Kristensen, Kasper; Enggrob, Kirsten L.; King, S. M.

    2013-01-01

    products cis-pinic and terpenylic acids, but similar to the second-generation oxidation products 3-methyl-1,2,3-butane tricarboxylic acid (MBTCA) and diaterpenylic acid acetate (DTAA). Dimer esters were observed within the first 30 min, indicating rapid production simultaneous to their structural......The formation of carboxylic acids and dimer esters from alpha-pinene oxidation was investigated in a smog chamber and in ambient aerosol samples collected during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX). Chamber experiments of alpha-pinene ozonolysis in dry air...... times higher during the warmer 2009 campaign relative to 2007, while the concentration of cis-pinic acid was approximately the same during both periods, and lack of correlation with levels of cis-pinic and terpenylic acids for both campaigns indicate that the formation of the pinyl-diaterpenyl ester...

  8. Nano-Sized Secondary Organic Aerosol of Diesel Engine Exhaust Origin Impairs Olfactory-Based Spatial Learning Performance in Preweaning Mice.

    Science.gov (United States)

    Win-Shwe, Tin-Tin; Kyi-Tha-Thu, Chaw; Moe, Yadanar; Maekawa, Fumihiko; Yanagisawa, Rie; Furuyama, Akiko; Tsukahara, Shinji; Fujitani, Yuji; Hirano, Seishiro

    2015-06-30

    The aims of our present study were to establish a novel olfactory-based spatial learning test and to examine the effects of exposure to nano-sized diesel exhaust-origin secondary organic aerosol (SOA), a model environmental pollutant, on the learning performance in preweaning mice. Pregnant BALB/c mice were exposed to clean air, diesel exhaust (DE), or DE-origin SOA (DE-SOA) from gestational day 14 to postnatal day (PND) 10 in exposure chambers. On PND 11, the preweaning mice were examined by the olfactory-based spatial learning test. After completion of the spatial learning test, the hippocampus from each mouse was removed and examined for the expressions of neurological and immunological markers using real-time RT-PCR. In the test phase of the study, the mice exposed to DE or DE-SOA took a longer time to reach the target as compared to the control mice. The expression levels of neurological markers such as the N -methyl-d-aspartate (NMDA) receptor subunits NR1 and NR2B, and of immunological markers such as TNF-α, COX2, and Iba1 were significantly increased in the hippocampi of the DE-SOA-exposed preweaning mice as compared to the control mice. Our results indicate that DE-SOA exposure in utero and in the neonatal period may affect the olfactory-based spatial learning behavior in preweaning mice by modulating the expressions of memory function-related pathway genes and inflammatory markers in the hippocampus.

  9. Identifying precursors and aqueous organic aerosol formation pathways during the SOAS campaign

    Science.gov (United States)

    Sareen, Neha; Carlton, Annmarie G.; Surratt, Jason D.; Gold, Avram; Lee, Ben; Lopez-Hilfiker, Felipe D.; Mohr, Claudia; Thornton, Joel A.; Zhang, Zhenfa; Lim, Yong B.; Turpin, Barbara J.

    2016-11-01

    Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized, low-volatility organic aerosol and, in some cases, light-absorbing (brown) carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, and health. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented, forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols), leading to the formation of secondary organic aerosol (SOAAQ). Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify additional precursors and products that may be atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere into water at Brent, Alabama, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Hydroxyl (OH⚫) radical oxidation experiments were conducted with the aqueous mixtures collected from SOAS to better understand the formation of SOA through gas-phase followed by aqueous-phase chemistry. Total aqueous-phase organic carbon concentrations for these mixtures ranged from 92 to 179 µM-C, relevant for cloud and fog waters. Aqueous OH-reactive compounds were primarily observed as odd ions in the positive ion mode by electrospray ionization mass spectrometry (ESI-MS). Ultra high-resolution Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) spectra and tandem MS (MS-MS) fragmentation of these ions were consistent with the presence of carbonyls and tetrols. Products were observed in the negative ion mode and included pyruvate and oxalate, which were confirmed by ion chromatography. Pyruvate and oxalate have been found in the particle phase in many locations (as salts and complexes). Thus

  10. Identifying precursors and aqueous organic aerosol formation pathways during the SOAS campaign

    Directory of Open Access Journals (Sweden)

    N. Sareen

    2016-11-01

    Full Text Available Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized, low-volatility organic aerosol and, in some cases, light-absorbing (brown carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, and health. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented, forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols, leading to the formation of secondary organic aerosol (SOAAQ. Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify additional precursors and products that may be atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere into water at Brent, Alabama, during the 2013 Southern Oxidant and Aerosol Study (SOAS. Hydroxyl (OH⚫ radical oxidation experiments were conducted with the aqueous mixtures collected from SOAS to better understand the formation of SOA through gas-phase followed by aqueous-phase chemistry. Total aqueous-phase organic carbon concentrations for these mixtures ranged from 92 to 179 µM-C, relevant for cloud and fog waters. Aqueous OH-reactive compounds were primarily observed as odd ions in the positive ion mode by electrospray ionization mass spectrometry (ESI-MS. Ultra high-resolution Fourier-transform ion cyclotron resonance mass spectrometry (FT-ICR-MS spectra and tandem MS (MS–MS fragmentation of these ions were consistent with the presence of carbonyls and tetrols. Products were observed in the negative ion mode and included pyruvate and oxalate, which were confirmed by ion chromatography. Pyruvate and oxalate have been found in the particle phase in many locations (as salts and

  11. Secondary organic aerosol formation from gasoline vehicle emissions in a new mobile environmental reaction chamber

    Directory of Open Access Journals (Sweden)

    S. M. Platt

    2013-09-01

    Full Text Available We present a new mobile environmental reaction chamber for the simulation of the atmospheric aging of different emission sources without limitation from the instruments or facilities available at any single site. Photochemistry is simulated using a set of 40 UV lights (total power 4 KW. Characterisation of the emission spectrum of these lights shows that atmospheric aging of emissions may be simulated over a range of temperatures (−7 to 25 °C. A photolysis rate of NO2, JNO2, of (8.0 ± 0.7 × 10−3 s−1 was determined at 25 °C. We demonstrate the utility of this new system by presenting results on the aging (OH = 12 × 106 cm−3 h of emissions from a modern (Euro 5 gasoline car operated during a driving cycle (New European Driving Cycle, NEDC on a chassis dynamometer in a vehicle test cell. Emissions from the entire NEDC were sampled and aged in the chamber. Total organic aerosol (OA; primary organic aerosol (POA emission + secondary organic aerosol (SOA formation was (369.8–397.510−3 g kg−1 fuel, or (13.2–15.4 × 10−3 g km−1, after aging, with aged OA/POA in the range 9–15. A thorough investigation of the composition of the gas phase emissions suggests that the observed SOA is from previously unconsidered precursors and processes. This large enhancement in particulate matter mass from gasoline vehicle aerosol emissions due to SOA formation, if it occurs across a wider range of gasoline vehicles, would have significant implications for our understanding of the contribution of on-road gasoline vehicles to ambient aerosols.

  12. A Computational Approach to Understanding Aerosol Formation and Oxidant Chemistry in the Troposphere

    Energy Technology Data Exchange (ETDEWEB)

    Francisco, Joseph S.; Kathmann, Shawn M.; Schenter, Gregory K.; Dang, Liem X.; Xantheas, Sotiris S.; Garrett, Bruce C.; Du, Shiyu; Dixon, David A.; Bianco, Roberto; Wang, Shuzhi; Hynes, James T.; Morita, Akihiro; Peterson, Kirk A.

    2006-04-18

    An understanding of the mechanisms and kinetics of aerosol formation and ozone production in the troposphere is currently a high priority because these phenomena are recognized as two major effects of energy-related air pollution. Atmospheric aerosols are of concern because of their effect on visibility, climate, and human health. Equally important, aerosols can change the chemistry of the atmosphere, in dramatic fashion, by providing new chemical pathways (in the condensed phase) unavailable in the gas phase. The oxidation of volatile organic compounds (VOCs) and inorganic compounds (e.g., sulfuric acid, ammonia, nitric acid, ions, and mineral) can produce precursor molecules that act as nucleation seeds. The U.S. Department of Energy (DOE) Atmospheric Chemistry Program (ACP) has identified the need to evaluate the causes of variations in tropospheric aerosol chemical composition and concentrations, including determining the sources of aerosol particles and the fraction of such that are of primary and secondary origin. In particular, the ACP has called for a deeper understanding into aerosol formation because nucleation creates substantial concentrations of fresh particles that, via growth and coagulation, influence the Earth's radiation budget. Tropospheric ozone is also of concern primarily because of its impact on human health. Ozone levels are controlled by NOx and by VOCs in the lower troposphere. The VOCs can be either from natural emissions from such sources as vegetation and phytoplankton or from anthropogenic sources such as automobiles and oil-fueled power production plants. The major oxidant for VOCs in the atmosphere is the OH radical. With the increase in VOC emissions, there is rising concern regarding the available abundance of HOx species needed to initiate oxidation. Over the last five years, there have been four field studies aimed at initial measurements of HOx species (OH and HO? radicals). These measurements revealed HOx levels that are

  13. New Parameterizations for Understanding Secondary Organic Aerosol Formation from Isoprene under Anthropogenic Influence

    Science.gov (United States)

    Yee, L.; Isaacman-VanWertz, G. A.; Wernis, R. A.; Kreisberg, N. M.; de Sá, S. S.; Martin, S. T.; Alexander, L.; Palm, B. B.; Hu, W.; Campuzano Jost, P.; Day, D. A.; Jimenez, J. L.; Artaxo, P.; Manzi, A. O.; Souza, R. A. F. D.; Hering, S. V.; Goldstein, A. H.

    2015-12-01

    Several studies have focused on elucidating the chemical mechanisms responsible for isoprene photochemistry leading to secondary organic aerosol (SOA) formation. While isoprene oxidation is the source of a large fraction of the organic mass in biogenic SOA formation over forested regions, few ambient measurements of the isoprene-derived products exist at sufficient time-resolution to fully parameterize the dynamic reactions in the particle phase. We deployed the Semi-Volatile Thermal desorption Aerosol Gas chromatograph (SV-TAG) during the Southern Oxidant and Aerosol Study (SOAS) in the Southeastern U.S. in summer 2013 and during the wet and dry seasons of the Green Ocean Amazon experiment (GoAmazon 2014/5) in central Amazonia. Both field campaigns were located in isoprene-rich forested regions under the varying influence of anthropogenic pollution. We measured oxidation products at the molecular level, including 2-methyl tetrols, C5-alkene triols, and 2-methyl glyceric acid in the gas and particle phases at hourly time resolution. Using supporting measurements of particle composition (e.g. sulfate) and modelled liquid water content, we compare the relative contribution of these tracers to the particle-phase across these regions and explore possible parameterizations that can be used for modeling SOA formation from isoprene.

  14. Long term model studies of aerosol formation and growth in borea forest

    Science.gov (United States)

    Zhou, L.; Boy, M.; Vuollekoski, H.; Watcharapaskorn, C.; Mogensen, D.; Smolander, S.; Sogachev, A.; Kulmala, M. T.

    2012-12-01

    Natural and anthropogenic aerosols may have a great impact on climate as they can directly interact with solar radiation and indirectly affect the Earth's radiation balance and precipitation by modifying clouds. In order to quantify the direct and indirect effect, it is essential to understand the complex processes that connect an aerosol particle to a cloud droplet. However, while modern measurement techniques are able to detect particle sizes down to nanometer all the way from ground up to the stratosphere, the data does not serve for all of our needs for understanding the processes. Hence we will demonstrate a modeling approach to investigate the complex processes of aerosols in the atmospheric boundary layer (ABL). SOSAA (model to Simulate the concentration of Organic vapors, Sulphuric Acid, and Aerosols) is a 1D chemical-transport model with detailed aerosol dynamics. It was constructed to study the emissions, transport, chemistry, as well as aerosols in the ABL in and above a vegetation canopy [Boy et al., 2011]. As a first application of the model, we tested different nucleation theories by simulating the new particle formation events in year 2010 at a boreal forest site in Finland. Since condensible organic vapors are the dominant contributors to the aerosol particle growth, particularly in regions where biogenic volatile organic compound emissions are high, we also simulated the concentrations of a set of organic compounds and their first reaction products from oxidation [e.g. Kerminen et al. (2000); Sellegri et al. (2005); Boy et al. (2005); Allan et al. (2006); Laaksonen et al. (2008)]. The results have showed the ability of SOSAA to reconstruct the general behavior of atmospheric trace gases and new particle formation in a boreal forest environment with reasonable uncertainties. The underestimation in sulfuric acid concentration during nighttime supports the view that other production mechanisms of sulfuric acid exist. It also suggests that the missing

  15. Evaluation of the atmospheric significance of multiphase reactions in atmospheric secondary organic aerosol formation

    Directory of Open Access Journals (Sweden)

    Gelencsér

    2005-01-01

    Full Text Available In a simple conceptual cloud-aerosol model the mass of secondary organic aerosol (SOA that may be formed in multiphase reaction in an idealized scenario involving two cloud cycles separated with a cloud-free period is evaluated. The conditions are set to those typical of continental clouds, and each parameter used in the model calculations is selected as a mean of available observational data of individual species for which the multiphase SOA formation route has been established. In the idealized setting gas and aqueous-phase reactions are both considered, but only the latter is expected to yield products of sufficiently low volatility to be retained by aerosol particles after the cloud dissipates. The key variable of the model is the Henry-constant which primarily determines how important multiphase reactions are relative to gas-phase photooxidation processes. The precursor considered in the model is assumed to already have some affinity to water, i.e. it is a compound having oxygen-containing functional group(s. As a principal model output an aerosol yield parameter is calculated for the multiphase SOA formation route as a function of the Henry-constant, and has been found to be significant already above H~103 M atm-1. Among the potential precursors that may be eligible for this mechanism based on their Henry constants, there are a suite of oxygenated compounds such as primary oxidation products of biogenic and anthropogenic hydrocarbons, including, for example, pinonaldehyde. Finally, the analogy of multiphase SOA formation to in-cloud sulfate production is exploited.

  16. Heterogeneous photochemistry of imidazole-2-carboxaldehyde: HO2 radical formation and aerosol growth

    Directory of Open Access Journals (Sweden)

    L. González Palacios

    2016-09-01

    Full Text Available The multiphase chemistry of glyoxal is a source of secondary organic aerosol (SOA, including its light-absorbing product imidazole-2-carboxaldehyde (IC. IC is a photosensitizer that can contribute to additional aerosol ageing and growth when its excited triplet state oxidizes hydrocarbons (reactive uptake via H-transfer chemistry. We have conducted a series of photochemical coated-wall flow tube (CWFT experiments using films of IC and citric acid (CA, an organic proxy and H donor in the condensed phase. The formation rate of gas-phase HO2 radicals (PHO2 was measured indirectly by converting gas-phase NO into NO2. We report on experiments that relied on measurements of NO2 formation, NO loss and HONO formation. PHO2 was found to be a linear function of (1 the [IC]  ×  [CA] concentration product and (2 the photon actinic flux. Additionally, (3 a more complex function of relative humidity (25 %  <  RH  <  63 % and of (4 the O2 ∕ N2 ratio (15 %  <  O2 ∕ N2  <  56 % was observed, most likely indicating competing effects of dilution, HO2 mobility and losses in the film. The maximum PHO2 was observed at 25–55 % RH and at ambient O2 ∕ N2. The HO2 radicals form in the condensed phase when excited IC triplet states are reduced by H transfer from a donor, CA in our system, and subsequently react with O2 to regenerate IC, leading to a catalytic cycle. OH does not appear to be formed as a primary product but is produced from the reaction of NO with HO2 in the gas phase. Further, seed aerosols containing IC and ammonium sulfate were exposed to gas-phase limonene and NOx in aerosol flow tube experiments, confirming significant PHO2 from aerosol surfaces. Our results indicate a potentially relevant contribution of triplet state photochemistry for gas-phase HO2 production, aerosol growth and ageing in the atmosphere.

  17. Aerosol formation and effect in biomass combustion and gasification

    Energy Technology Data Exchange (ETDEWEB)

    Strand, Michael; Lillieblad, Lena; Sanati, Mehri [Vaexjoe Univ. (Sweden). Bioenergy Technology; Pagels, Joakim; Szpila, Aneta; Boghard, Mats [Lund Univ. (Sweden). Div. of Ergonomics and Aerosol Technology; Rissler, Jenny; Swietlicki, Erik [Lund Univ. (Sweden). Div. of Nuclear Physics

    2005-09-01

    The fine particle composition as analysed with PIXE and IC, was dominated by potassium, sulphur and chlorine. In some cases there was also a substantial concentration of zinc in the fine mode particles. The proposed mechanism for formation of the fine mode is homogenous chemical reactions to form potassium sulphate, which nucleates to form a fine particle mode at high temperatures The concentration profile of zinc indicates that zinc-containing species may form particles by gas-to-particle conversion prior to the nucleation of potassium sulphate. As the flue gas temperature decrease below 650 deg C potassium chloride will condense on the surfaces of the previously formed particles. As the temperature descends further, other more volatile components such as Pb and heavy hydrocarbons will condense. The coarse particle number concentration varied between 100-10,000 particles/cm{sup 3}, and the mass concentration varied between 4-87 mg/cm{sup 3}, with the highest concentrations for the high load cases. The coarse mode particles were mainly composed of calcium and manganese in addition to potassium, sulphur and chlorine. The proposed mechanism for inception of the coarse particle mode was fragmentation/dispersion of refractory material from the burning char or from the residual ash in the bed. The ratios of the potentially volatile elements potassium, sulphur and chlorine, were similar in the fine and the coarse mode, indicating the material had the same origin in both modes. The presence of the volatile components may be explained by non-complete vaporisation, chemical surface reactions, and re-entrainment of deposited particles or by coagulation of fine particles. However, neither of the proposed mechanisms can give a conclusive explanation to the composition of the coarse mode, i.e. the high concentration potentially volatile elements.

  18. Aerosol and CCN properties at Princess Elisabeth station, East Antarctica: seasonality, new particle formation events and properties around precipitation events

    Science.gov (United States)

    Mangold, Alexander; Laffineur, Quentin; De Backer, Hugo; Herenz, Paul; Wex, Heike; Gossart, Alexandra; Souverijns, Niels; Gorodetskaya, Irina; Van Lipzig, Nicole

    2016-04-01

    Since 2010, several complementary ground-based instruments for measuring the aerosol composition of the Antarctic atmosphere have been operated at the Belgian Antarctic research station Princess Elisabeth, in Dronning Maud Land, East Antarctica (71.95° S, 23.35° E, 1390 m asl.). In addition, three ground-based remote sensing instruments for cloud and precipitation observations have been installed for continuous operation, including a ceilometer (cloud base height, type, vertical extent), a 24 Ghz micro-rain radar (vertical profiles of radar effective reflectivity and Doppler velocity), and a pyrometer (cloud base temperature). The station is inhabited from November to end of February and operates under remote control during the other months. In this contribution, the general aerosol and cloud condensation nuclei (CCN) properties will be described with a special focus on new particle formation events and around precipitation events. New particle formation events are important for the atmospheric aerosol budget and they also show that aerosols are not only transported to Antarctica but are also produced there, also inland. Aerosols are essential for cloud formation and therefore also for precipitation, which is the only source for mass gain of the Antarctic ice sheet. Measured aerosol properties comprise size distribution, total number, total mass concentration, mass concentration of light-absorbing aerosol and absorption coefficient and total scattering coefficient. In addition, a CCN counter has been operated during austral summers 2013/14, 2014/15 and 2015/16. The baseline total number concentration N-total was around some hundreds of particles/cm3. During new particle formation events N-total increased to some thousands of particles/cm3. Simultaneous measurements of N-total, size distribution and CCN number revealed that mostly the number of particles smaller than 100 nm increased and that the concentration of cloud condensation nuclei increased only very

  19. Calculating Equilibrium Phase Distribution during the Formation of Secondary Organic Aerosol Using COSMOtherm.

    Science.gov (United States)

    Wang, Chen; Goss, Kai-Uwe; Lei, Ying Duan; Abbatt, Jonathan P D; Wania, Frank

    2015-07-21

    Challenges in the parametrization of compound distribution between the gas and particle phase contribute significantly to the uncertainty in the prediction of secondary organic aerosol (SOA) formation and are rooted in the complexity and variability of atmospheric condensed matter, which includes water, salts, and a multitude of organic oxidation products, often in two separated phases. Here, we explore the use of the commercial quantum-chemistry-based software COSMOtherm to predict equilibrium partitioning and Setchenow coefficients of a suite of oxidation products of α-pinene ozonolysis in an aerosol that is assumed to separate into an organic-enriched phase and an electrolyte-enriched aqueous phase. The predicted coefficients are used to estimate the phase distribution of the organic compounds, water and ammonium sulfate, the resulting phase composition, and the SOA yield. Four scenarios that differ in terms of organic loading, liquid water content, and chemical aging are compared. The organic compounds partition preferentially to the organic phase rather than the aqueous phase for the studied aerosol scenarios, partially due to the salting-out effect. Extremely low volatile organic compounds are predicted to be the dominant species in the organic aerosols at low loadings and an important component at higher loadings. The highest concentration of oxidation products in the condensed phase is predicted for a scenario assuming the presence of non-phase-separated cloud droplets. Partitioning into an organic aerosol phase composed of the oxidation products is predicted to be similar to partitioning into a phase composed of a single organic surrogate molecule, suggesting that the calculation procedure can be simplified without major loss of accuracy. COSMOtherm is shown to produce results that are comparable to those obtained using group contribution methods. COSMOtherm is likely to have a much larger application domain than those group contribution methods because

  20. Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

    Science.gov (United States)

    Zhang, Y. M.; Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Gong, S. L.; Shen, X. J.; Yang, S.

    2011-07-01

    Size-resolved aerosol number and mass concentrations and the mixing ratios of O3 and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM1) and sulphate; nitrate and ammonium were more minor contributors.

  1. Secondary organic aerosol formation from ozone-initiated reactions with nicotine and secondhand tobacco smoke

    Science.gov (United States)

    Sleiman, Mohamad; Destaillats, Hugo; Smith, Jared D.; Liu, Chen-Lin; Ahmed, Musahid; Wilson, Kevin R.; Gundel, Lara A.

    2010-11-01

    We used controlled laboratory experiments to evaluate the aerosol-forming potential of ozone reactions with nicotine and secondhand smoke. Special attention was devoted to real-time monitoring of the particle size distribution and chemical composition of SOA as they are believed to be key factors determining the toxicity of SOA. The experimental approach was based on using a vacuum ultraviolet photon ionization time-of-flight aerosol mass spectrometer (VUV-AMS), a scanning mobility particle sizer (SMPS) and off-line thermal desorption coupled to mass spectrometry (TD-GC-MS) for gas-phase byproducts analysis. Results showed that exposure of SHS to ozone induced the formation of ultrafine particles (health effects is highlighted.

  2. Secondary Organic Aerosol Formation by Reactive Condensation of Glyoxal and Water Vapor

    Science.gov (United States)

    Hastings, W. P.; Koehler, C. A.; de Haan, D. O.

    2004-05-01

    The formation of secondary organic aerosol particles by particle-phase reactions is currently of great interest. Glyoxal has been identified as a significant component in the particle phase in recent smog chamber aromatic oxidation studies. This is surprising because glyoxal has a high vapor pressure and phase partitioning theory would predict that it remain almost entirely in the gas phase. Growth of inorganic seed aerosol in a particle chamber was monitored by scanning mobility particle sizing during addition of gas-phase glyoxal and small amounts of water vapor. Glyoxal was observed to condense on inorganic seed aerosol at concentrations that are at least 100 times below its vapor pressure. This behavior can be explained by a chemical reaction: glyoxal is known to polymerize when exposed to water vapor. This polymerization may be a general mechanism for secondary aerosol formation by alpha-dicarbonyl compounds. The reactivity of hydrated and polymerized forms of glyoxal during analysis by gas chromatography was assessed. Hydrated glyoxal was found to convert to glyoxal at even slightly elevated temperatures in GC injection ports. We then showed that breakdown of solid-phase glyoxal trimer dihydrate, forming gas phase glyoxal and water vapor, occurs at temperatures just above 50 *C, the boiling point of glyoxal. These observations suggest that reports of particle-phase glyoxal are likely caused by GC sampling artifacts, and that the actual particulate species are instead polymerized forms of glyoxal. It does not appear that chemical derivatization protects glyoxal polymers from thermal breakdown during GC analysis. The existence in the particle phase of glyoxal polymers with negligable vapor pressures, rather than volatile glyoxal, is consistent with phase partitioning theory.

  3. Concentration Effects and Ion Properties Controlling the Fractionation of Halides during Aerosol Formation

    Science.gov (United States)

    Guzman, Marcelo I.; Athalye, Richa R.; Rodriguez, Jose M.

    2012-01-01

    During the aerosolization process at the sea surface, halides are incorporated into aerosol droplets, where they may play an important role in tropospheric ozone chemistry. Although this process may significantly contribute to the formation of reactive gas phase molecular halogens, little is known about the environmental factors that control how halides selectively accumulate at the air-water interface. In this study, the production of sea spray aerosol is simulated using electrospray ionization (ESI) of 100 nM equimolar solutions of NaCl, NaBr, NaI, NaNO2, NaNO3, NaClO4, and NaIO4. The microdroplets generated are analyzed by mass spectrometry to study the comparative enrichment of anions (f (Isub x-)) and their correlation with ion properties. Although no correlation exists between f (sub x-) and the limiting equivalent ionic conductivity, the correlation coefficient of the linear fit with the size of the anions R(sub x-), dehydration free-energy ?Gdehyd, and polarizability alpha, follows the order: (R(sub x-)(exp -2)) > (R(sub x-)(exp -1)) >(R(sub x-) > delta G(sub dehyd) > alpha. The same pure physical process is observed in H2O and D2O. The factor f (sub x-) does not change with pH (6.8-8.6), counterion (Li+, Na+, K+, and Cs+) substitution effects, or solvent polarity changes in methanol - and ethanol-water mixtures (0 water interface of equimolar solutions, our results of seawater mimic samples agree with a model in which the interfacial composition is increasingly enriched in I- < Br- < Cl- over the oceanic boundary layer due to concentration effects in sea spray aerosol formation.

  4. Salting Constants of Small Organic Molecules in Aerosol-Relevant Salts and Application to Aerosol Formation in the Southeastern United States

    Science.gov (United States)

    Waxman, E.; Carlton, A. M. G.; Ziemann, P. J.; Volkamer, R. M.

    2014-12-01

    Secondary organic aerosol (SOA) formation from small water-soluble molecules such as glyoxal and methyl glyoxal is a topic of emerging interest. Results from recent field campaigns, e.g. Waxman et al. (2013, GRL) and Knote et al. (2014, ACP), show that these molecules can form significant SOA mass as a result of 'salting-in'. Salting-in happens when a molecule's solubility increases with salt concentration and salting-out is the reverse. Salting effects modify the solubility exponentially with increasing salt concentration, and thus the effective Henry's law constant can strongly modify partitioning, and multiphase chemical reaction rates in aerosol water. Moreover, the solubility in aerosol water cannot easily inferred based on the solubility in cloud water, as the salting effects could change the solubility by a factor of 104 or more. In this work, we have devised and applied a novel experimental setup to measure salting constants using an ion trap mass spectrometer. We focus on small, water soluble molecules like methyl glyoxal and similar compounds and measure salting constants for aerosol-relevant salts including ammonium sulfate, ammonium nitrate, and sodium chloride. The Setschenow salting-constant values are then used to parameterize the effects of salting in CMAQ. We present a series of sensitivity studies of the effects that inorganic aerosols have on the SOA formation from small soluble molecules in the southeastern United States.

  5. Secondary organic aerosol formation from a large number of reactive man-made organic compounds

    Energy Technology Data Exchange (ETDEWEB)

    Derwent, Richard G., E-mail: r.derwent@btopenworld.com [rdscientific, Newbury, Berkshire (United Kingdom); Jenkin, Michael E. [Atmospheric Chemistry Services, Okehampton, Devon (United Kingdom); Utembe, Steven R.; Shallcross, Dudley E. [School of Chemistry, University of Bristol, Bristol (United Kingdom); Murrells, Tim P.; Passant, Neil R. [AEA Environment and Energy, Harwell International Business Centre, Oxon (United Kingdom)

    2010-07-15

    A photochemical trajectory model has been used to examine the relative propensities of a wide variety of volatile organic compounds (VOCs) emitted by human activities to form secondary organic aerosol (SOA) under one set of highly idealised conditions representing northwest Europe. This study applied a detailed speciated VOC emission inventory and the Master Chemical Mechanism version 3.1 (MCM v3.1) gas phase chemistry, coupled with an optimised representation of gas-aerosol absorptive partitioning of 365 oxygenated chemical reaction product species. In all, SOA formation was estimated from the atmospheric oxidation of 113 emitted VOCs. A number of aromatic compounds, together with some alkanes and terpenes, showed significant propensities to form SOA. When these propensities were folded into a detailed speciated emission inventory, 15 organic compounds together accounted for 97% of the SOA formation potential of UK man made VOC emissions and 30 emission source categories accounted for 87% of this potential. After road transport and the chemical industry, SOA formation was dominated by the solvents sector which accounted for 28% of the SOA formation potential.

  6. Reactive oxidation products promote secondary organic aerosol formation from green leaf volatiles

    Directory of Open Access Journals (Sweden)

    J. F. Hamilton

    2009-06-01

    Full Text Available Green leaf volatiles (GLVs are an important group of chemicals released by vegetation which have emission fluxes that can be significantly increased when plants are damaged or stressed. A series of simulation chamber experiments has been conducted at the European Photoreactor in Valencia, Spain, to investigate secondary organic aerosol (SOA formation from the atmospheric oxidation of the major GLVs cis-3-hexenylacetate and cis-3-hexen-1-ol. Liquid chromatography-ion trap mass spectrometry was used to identify chemical species present in the SOA. Cis-3-hexen-1-ol proved to be a more efficient SOA precursor due to the high reactivity of its first generation oxidation product, 3-hydroxypropanal, which can hydrate and undergo further reactions with other aldehydes resulting in SOA dominated by higher molecular weight oligomers. The lower SOA yields produced from cis-3-hexenylacetate are attributed to the acetate functionality, which inhibits oligomer formation in the particle phase. Based on observed SOA yields and best estimates of global emissions, these compounds may be calculated to be a substantial unidentified global source of SOA, contributing 1–5 TgC yr−1, equivalent to around a third of that predicted from isoprene. Molecular characterization of the SOA, combined with organic mechanistic information, has provided evidence that the formation of organic aerosols from GLVs is closely related to the reactivity of their first generation atmospheric oxidation products, and indicates that this may be a simple parameter that could be used in assessing the aerosol formation potential for other unstudied organic compounds in the atmosphere.

  7. Chemical composition, source, and process of urban aerosols during winter haze formation in Northeast China.

    Science.gov (United States)

    Zhang, Jian; Liu, Lei; Wang, Yuanyuan; Ren, Yong; Wang, Xin; Shi, Zongbo; Zhang, Daizhou; Che, Huizheng; Zhao, Hujia; Liu, Yanfei; Niu, Hongya; Chen, Jianmin; Zhang, Xiaoye; Lingaswamy, A P; Wang, Zifa; Li, Weijun

    2017-12-01

    The characteristics of aerosol particles have been poorly evaluated even though haze episodes frequently occur in winter in Northeast China. OC/EC analysis, ion chromatography, and transmission electron microscopy (TEM) were used to investigate the organic carbon (OC) and elemental carbon (EC), and soluble ions in PM 2.5 and the mixing state of individual particles during a severe wintertime haze episode in Northeast China. The organic matter (OM), NH 4 + , SO 4 2- , and NO 3 - concentrations in PM 2.5 were 89.5 μg/m 3 , 24.2 μg/m 3 , 28.1 μg/m 3 , and 32.8 μg/m 3 on the haze days, respectively. TEM observations further showed that over 80% of the haze particles contained primary organic aerosols (POAs). Based on a comparison of the data obtained during the haze formation, we generate the following synthetic model of the process: (1) Stable synoptic meteorological conditions drove the haze formation. (2) The early stage of haze formation (light or moderate haze) was mainly caused by the enrichment of POAs from coal burning for household heating and cooking. (3) High levels of secondary organic aerosols (SOAs), sulfates, and nitrates formation via heterogeneous reactions together with POAs accumulation promoted to the evolution from light or moderate to severe haze. Compared to the severe haze episodes over the North China Plain, the PM 2.5 in Northeast China analyzed in the present study contained similar sulfate, higher SOA, and lower nitrate contents. Our results suggest that most of the POAs and secondary particles were likely related to emissions from coal-burning residential stoves in rural outskirts and small boilers in urban areas. The inefficient burning of coal for household heating and cooking should be monitored during wintertime in Northeast China. Copyright © 2017 Elsevier Ltd. All rights reserved.

  8. Study of particle size distribution and formation mechanism of radioactive aerosols generated in high-energy neutron fields

    CERN Document Server

    Endo, A; Noguchi, H; Tanaka, S; Iida, T; Furuichi, S; Kanda, Y; Oki, Y

    2003-01-01

    The size distributions of sup 3 sup 8 Cl, sup 3 sup 9 Cl, sup 8 sup 2 Br and sup 8 sup 4 Br aerosols generated by irradiations of argon and krypton gases containing di-octyl phthalate (DOP) aerosols with 45 MeV and 65 MeV quasi-monoenergetic neutrons were measured in order to study the formation mechanism of radioactive particles in high energy radiation fields. The effects of the size distribution of the radioactive aerosols on the size of the added DOP aerosols, the energy of the neutrons and the kinds of nuclides were studied. The observed size distributions of the radioactive particles were explained by attachment of the radioactive atoms generated by the neutron-induced reactions to the DOP aerosols. (author)

  9. Organic Aerosol Formation in the Humid, Photochemically-Active Southeastern US: SOAS Experiments and Simulations

    Science.gov (United States)

    Sareen, N.; Lim, Y. B.; Carlton, A. G.; Turpin, B. J.

    2013-12-01

    Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized low volatility organic aerosol and, in some cases, light absorbing (brown) carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, health, and the environment. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols) leading to the formation of secondary organic aerosol (SOAAQ). Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify other precursors that are atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere at Brent, Alabama during the Southern Oxidant and Aerosol Study (SOAS). Four mist chambers in parallel collected ambient gases in a DI water medium at 20-25 LPM with a 4 hr collection time. Total organic carbon (TOC) values in daily composited samples were 64-180 μM. Aqueous OH radical oxidation experiments were conducted with these mixtures in a newly designed cuvette chamber to understand the formation of SOA through gas followed by aqueous chemistry. OH radicals (3.5E-2 μM [OH] s-1) were formed in-situ in the chamber, continuously by H2O2 photolysis. Precursors and products of these aqueous OH experiments were characterized using ion chromatography (IC), electrospray ionization mass spectrometry (ESI-MS), and IC-ESI-MS. ESI-MS results from a June 12th, 2013 sample showed precursors to be primarily odd, positive mode ions, indicative of the presence of non-nitrogen containing alcohols, aldehydes, organic peroxides, or epoxides. Products were seen in the negative mode and included organic acid ions like pyruvate

  10. FORMATION OF POLYKETONES IN IRRADIATED TOLUENE/PROPYLENE/NOX/AIR MIXTURES

    Science.gov (United States)

    A laboratory study was carried out to investigate the formation of polyketones in secondary organic aerosol from photooxidation of the aromatic hydrocarbon toluene, a major constituent of automobile exhaust. The laboratory experiments consisted of irradiating toluene/propylene...

  11. Effect of organic compounds on nanoparticle formation in diluted diesel exhaust

    Directory of Open Access Journals (Sweden)

    U. Mathis

    2004-01-01

    Full Text Available The nucleation of nanoparticles in the exhaust of a modern light-duty diesel vehicle was investigated on a chassis dynamometer. This laboratory study is focused on the influence of volatile organic compounds (VOCs on nucleation of volatile nanoparticles. Different organic compounds were added to the dilution air of the particle sampling under different sampling conditions. Sample temperature and relative sample humidity were varied in a wide range. The number size distribution of the particles was measured with a scanning mobility particle sizer (SMPS and showed significant differences in response to the added organic compounds. While the nucleation mode particles showed a large variation in concentration, the accumulation mode particles remained unchanged for all compounds. Depending on the functional group, organic compounds were capable of initiating and increasing (alcohols and toluene or decreasing (acetone, aniline, and methyl tert-butyl ether (MTBE nucleation mode particles. Short volatile aliphatic hydrocarbons (hexane and cyclohexane turned out to be without effect on nucleation of nanoparticles. Possible reasons for the differences are discussed.

  12. Role of TLR4 in olfactory-based spatial learning activity of neonatal mice after developmental exposure to diesel exhaust origin secondary organic aerosol.

    Science.gov (United States)

    Nway, Nay Chi; Fujitani, Yuji; Hirano, Seishiro; Mar, Ohn; Win-Shwe, Tin-Tin

    2017-12-01

    Exposure to ambient air pollutants has been reported to have various adverse health impacts. Ambient particulate matter comprises primary particles released directly via engine exhaust and secondary organic aerosols (SOAs) formed from oxidative reactions of the ultrafine particle fraction of diesel exhaust (DE). Toll-like receptor 4 (TLR4) is well known to initiate the inflammatory cascade in the central nervous system. However, whether and how DE and DE-SOA exposure influences TLR4 signaling in the immature brain remains unclear. We attempted to evaluate the roles of TLR-4, inflammatory mediators and microglial markers in the impaired spatial learning ability of neonatal mice exposed to DE and DE-SOAs. Pregnant C3H/HeN (TLR4-intact) and C3H/HeJ (TLR4- mutated) mice were exposed to clean air, DE or DE-SOA from gestational day 14 to postnatal day (PND) 10 (5h/day for 5days) in exposure chambers. PND11 neonatal mice were examined for their performance in the olfactory-based spatial learning test. After the spatial learning test, the hippocampi of the mice were removed and real-time RT-PCR analysis was performed to examine the neurological and immunological markers. Both male and female C3H/HeN and C3H/HeJ neonatal mice exposed to DE and DE-SOAs showed poor performance in the test phase of spatial learning as compared to the mice exposed to clean air. However, this spatial learning deficit was prominent in C3H/HeJ neonatal mice. In the neonatal C3H/HeN male mice exposed to DE and DE-SOAs, the mRNA expression levels of the NMDA receptor subunits (NR1, NR2B), proinflammatory cytokines, tumor necrosis factor-α and cyclooxygenase-2, oxidative stress marker, heme oxygenase-1, and microglial marker, Iba1, in the hippocampus were significantly increased, but these changes were not observed in female mice. Our findings indicate that activation of the neuroimmune system and TLR4 signaling may possibly be involved in environmental pollutant-induced spatial learning impairment

  13. Modeling the formation of secondary organic aerosol during 2014 over China using NAQPMS

    Science.gov (United States)

    Yang, Wenyi

    2017-04-01

    The Nested Air Quality Prediction Modeling System (NAQPMS) with the updated Volatility Basis Set (VBS) approach instead of the two-product approach was used to investigate the formation of secondary organic aerosol (SOA) over China in 2014. This model considers the multi-generation oxidation process of volatile organic compounds (VOCs) and intermediate VOC (IVOCs), and the chemical aging of semi-volatile primary organic aerosol (POA). The model capability of reproducing the spatial and temporal distribution of fine particulate matter was confirmed by the comparison with the observation. Overall, the SOA accounted for approximately 60% of total organic aerosol in winter, 50-60% in spring and autumn, and in summer even more than 70% due to the strong photochemical reaction. In winter, more than 60% of the predicted SOA was contributed by the oxidation of IVOCs in central and eastern China. The SOA production from IVOCs is dominant compared to the production from traditional VOCs and the IVOCs oxidation mechanism is expected to improve the SOA model performance in China. However, the emission sources and reactions rates of IVOCs still remained large uncertainties and are needed for further identification and quantification.

  14. submitter On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

    CERN Document Server

    Schobesberger, S; Bianchi, F; Rondo, L; Duplissy, J; Kürten, A; Ortega, I K; Metzger, A; Schnitzhofer, R; Almeida, J; Amorim, A; Dommen, J; Dunne, E M; Ehn, M; Gagné, S; Ickes, L; Junninen, H; Hansel, A; Kerminen, V -M; Kirkby, J; Kupc, A; Laaksonen, A; Lehtipalo, K; Mathot, S; Onnela, A; Petäjä, T; Riccobono, F; Santos, F D; Sipilä, M; Tomé, A; Tsagkogeorgas, G; Viisanen, Y; Wagner, P E; Wimmer, D; Curtius, J; Donahue, N M; Baltensperger, U; Kulmala, M; Worsnop, D R

    2015-01-01

    The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia $(NH_3)$ and sulfuric acid $(H-2SO_4)$. Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small $NH_3–H_2SO_4$ clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm/Δn = 1.05 and were only observed at sufficiently high $[NH_3]$ / $[H_2SO_4]$. The $H_2SO_4$ molecules of these clusters are partially neutralized by $NH_3$, in close resemblance...

  15. Variations in Aerosol Chemical Composition during New Particle Formation and Growth Events Downwind of Seoul, Korea

    Science.gov (United States)

    Park, J.; Choi, Y.; Ghim, Y. S.

    2016-12-01

    New particle formation and growth has been characterized through various field studies using scanning mobility particle sizer (SMPS). However, there is insufficient knowledge of the variation of aerosol chemical compositions during those events. We investigated the variation of aerosol chemical composition during new particle formation and growth events downwind of Seoul. New particle formation and growth events were identified based on the evolution of the number size distribution measured by SMPS. The concentrations of inorganic ions and black carbon were measured using a particle-into-liquid sampler (PILS) coupled with an ion chromatograph (IC) and multi-angle absorption photometer (MAAP), respectively. We also measured concentrations of gaseous precursors (SO2, NO2) along with meteorological parameters using an automatic weather station. The measurements were conducted on the rooftop of a five-story building on a hill (37.34°N, 127.27°E, 167 m above sea level) at the Global Campus of Hankuk University of Foreign Studies, located about 35 km southeast of downtown Seoul. The measurement periods were from February 12 to April 1, 2015 and from April 13 to June 12, 2016. We investigated the difference in chemical compositions between event and non-event days and its association with the variations in precursor concentrations and meteorological parameters.

  16. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

    CERN Document Server

    Schobesberger, S; Bianchi, F; Rondo, L; Duplissy, J; Kürten, A; Ortega, I K; Metzger, A; Schnitzhofer, R; Almeida, J; Amorim, A; Dommen, J; Dunne, E M; Ehn, M; Gagné, S; Ickes, L; Junninen, H; Hansel, A; Kerminen, V-M; Kirkby, J; Kupc, A; Laaksonen, A; Lehtipalo, K; Mathot, S; Onnela, A; Petäjä, T; Riccobono, F; Santos, F D; Sipilä, M; Tomé, A; Tsagkogeorgas, G; Viisanen, Y; Wagner, P E; Wimmer, D; Curtius, J; Donahue, N M; Baltensperger, U; Kulmala, M; Worsnop, D R

    2014-01-01

    The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm / Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid-base bindings ...

  17. Ozone and secondary organic aerosol formation potential from anthropogenic volatile organic compounds emissions in China.

    Science.gov (United States)

    Wu, Wenjing; Zhao, Bin; Wang, Shuxiao; Hao, Jiming

    2017-03-01

    Volatile organic compounds (VOCs) are major precursors for ozone and secondary organic aerosol (SOA), both of which greatly harm human health and significantly affect the Earth's climate. We simultaneously estimated ozone and SOA formation from anthropogenic VOCs emissions in China by employing photochemical ozone creation potential (POCP) values and SOA yields. We gave special attention to large molecular species and adopted the SOA yield curves from latest smog chamber experiments. The estimation shows that alkylbenzenes are greatest contributors to both ozone and SOA formation (36.0% and 51.6%, respectively), while toluene and xylenes are largest contributing individual VOCs. Industry solvent use, industry process and domestic combustion are three sectors with the largest contributions to both ozone (24.7%, 23.0% and 17.8%, respectively) and SOA (22.9%, 34.6% and 19.6%, respectively) formation. In terms of the formation potential per unit VOCs emission, ozone is sensitive to open biomass burning, transportation, and domestic solvent use, and SOA is sensitive to industry process, domestic solvent use, and domestic combustion. Biomass stoves, paint application in industrial protection and buildings, adhesives application are key individual sources to ozone and SOA formation, whether measured by total contribution or contribution per unit VOCs emission. The results imply that current VOCs control policies should be extended to cover most important industrial sources, and the control measures for biomass stoves should be tightened. Finally, discrepant VOCs control policies should be implemented in different regions based on their ozone/aerosol concentration levels and dominant emission sources for ozone and SOA formation potential. Copyright © 2016. Published by Elsevier B.V.

  18. Seasonality of New Particle Formation in Vienna, Austria - Influence of Air Mass Origin and Aerosol Chemical Composition

    Czech Academy of Sciences Publication Activity Database

    Wonaschütz, A.; Demattio, A.; Wagner, R.; Burkart, J.; Zíková, Naděžda; Vodička, Petr; Ludwig, W.; Steiner, G.; Schwarz, Jaroslav; Hitzenberger, R.

    2015-01-01

    Roč. 118, OCT 2015 (2015), s. 118-126 ISSN 1352-2310 R&D Projects: GA MŠk 7AMB12AT021; GA ČR(CZ) GBP503/12/G147 Grant - others:FWF(AT) P19515-N20 Institutional support: RVO:67985858 Keywords : urban aerosol * aerosol chemical composition * new particle formation Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.459, year: 2015

  19. Formation and occurrence of dimer esters of pinene oxidation products in atmospheric aerosols

    Directory of Open Access Journals (Sweden)

    K. Kristensen

    2013-04-01

    Full Text Available The formation of carboxylic acids and dimer esters from α-pinene oxidation was investigated in a smog chamber and in ambient aerosol samples collected during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX. Chamber experiments of α-pinene ozonolysis in dry air and at low NOx concentrations demonstrated formation of two dimer esters, pinyl-diaterpenyl (MW 358 and pinonyl-pinyl dimer ester (MW 368, under both low- and high-temperature conditions. Concentration levels of the pinyl-diaterpenyl dimer ester were lower than the assumed first-generation oxidation products cis-pinic and terpenylic acids, but similar to the second-generation oxidation products 3-methyl-1,2,3-butane tricarboxylic acid (MBTCA and diaterpenylic acid acetate (DTAA. Dimer esters were observed within the first 30 min, indicating rapid production simultaneous to their structural precursors. However, the sampling time resolution precluded conclusive evidence regarding formation from gas- or particle-phase processes. CCN activities of the particles formed in the smog chamber displayed a modest variation during the course of experiments, with κ values in the range 0.06–0.09 (derived at a supersaturation of 0.19%. The pinyl-diaterpenyl dimer ester was also observed in ambient aerosol samples collected above a ponderosa pine forest in the Sierra Nevada Mountains of California during two seasonally distinct field campaigns in September 2007 and July 2009. The pinonyl-pinyl ester was observed for the first time in ambient air during the 2009 campaign, and although present at much lower concentrations, it was correlated with the abundance of the pinyl-diaterpenyl ester, suggesting similarities in their formation. The maximum concentration of the pinyl-diaterpenyl ester was almost 10 times higher during the warmer 2009 campaign relative to 2007, while the concentration of cis-pinic acid was approximately the same during both periods, and lack of correlation

  20. Key parameters controlling OH-initiated formation of secondary organic aerosol in the aqueous phase (aqSOA)

    Science.gov (United States)

    Ervens, Barbara; Sorooshian, Armin; Lim, Yong B.; Turpin, Barbara J.

    2014-04-01

    Secondary organic aerosol formation in the aqueous phase of cloud droplets and aerosol particles (aqSOA) might contribute substantially to the total SOA burden and help to explain discrepancies between observed and predicted SOA properties. In order to implement aqSOA formation in models, key processes controlling formation within the multiphase system have to be identified. We explore parameters affecting phase transfer and OH(aq)-initiated aqSOA formation as a function of OH(aq) availability. Box model results suggest OH(aq)-limited photochemical aqSOA formation in cloud water even if aqueous OH(aq) sources are present. This limitation manifests itself as an apparent surface dependence of aqSOA formation. We estimate chemical OH(aq) production fluxes, necessary to establish thermodynamic equilibrium between the phases (based on Henry's law constants) for both cloud and aqueous particles. Estimates show that no (currently known) OH(aq) source in cloud water can remove this limitation, whereas in aerosol water, it might be feasible. Ambient organic mass (oxalate) measurements in stratocumulus clouds as a function of cloud drop surface area and liquid water content exhibit trends similar to model results. These findings support the use of parameterizations of cloud-aqSOA using effective droplet radius rather than liquid water volume or drop surface area. Sensitivity studies suggest that future laboratory studies should explore aqSOA yields in multiphase systems as a function of these parameters and at atmospherically relevant OH(aq) levels. Since aerosol-aqSOA formation significantly depends on OH(aq) availability, parameterizations might be less straightforward, and oxidant (OH) sources within aerosol water emerge as one of the major uncertainties in aerosol-aqSOA formation.

  1. Importance of Physico-Chemical Properties of Aerosols in the Formation of Arctic Ice Clouds

    Science.gov (United States)

    Keita, S. A.; Girard, E.

    2014-12-01

    Ice clouds play an important role in the Arctic weather and climate system but interactions between aerosols, clouds and radiation are poorly understood. Consequently, it is essential to fully understand their properties and especially their formation process. Extensive measurements from ground-based sites and satellite remote sensing reveal the existence of two Types of Ice Clouds (TICs) in the Arctic during the polar night and early spring. TIC-1 are composed by non-precipitating very small (radar-unseen) ice crystals whereas TIC-2 are detected by both sensors and are characterized by a low concentration of large precipitating ice crystals. It is hypothesized that TIC-2 formation is linked to the acidification of aerosols, which inhibit the ice nucleating properties of ice nuclei (IN). As a result, the IN concentration is reduced in these regions, resulting to a smaller concentration of larger ice crystals. Over the past 10 years, several parameterizations of homogeneous and heterogeneous ice nucleation have been developed to reflect the various physical and chemical properties of aerosols. These parameterizations are derived from laboratory studies on aerosols of different chemical compositions. The parameterizations are also developed according to two main approaches: stochastic (that nucleation is a probabilistic process, which is time dependent) and singular (that nucleation occurs at fixed conditions of temperature and humidity and time-independent). This research aims to better understand the formation process of TICs using a newly-developed ice nucleation parameterizations. For this purpose, we implement some parameterizations (2 approaches) into the Limited Area version of the Global Multiscale Environmental Model (GEM-LAM) and use them to simulate ice clouds observed during the Indirect and Semi-Direct Arctic Cloud (ISDAC) in Alaska. We use both approaches but special attention is focused on the new parameterizations of the singular approach. Simulation

  2. Limited effect of anthropogenic nitrogen oxides on secondary organic aerosol formation

    Science.gov (United States)

    Zheng, Y.; Unger, N.; Hodzic, A.; Emmons, L.; Knote, C.; Tilmes, S.; Lamarque, J.-F.; Yu, P.

    2015-12-01

    Globally, secondary organic aerosol (SOA) is mostly formed from emissions of biogenic volatile organic compounds (VOCs) by vegetation, but it can be modified by human activities as demonstrated in recent research. Specifically, nitrogen oxides (NOx = NO + NO2) have been shown to play a critical role in the chemical formation of low volatility compounds. We have updated the SOA scheme in the global NCAR (National Center for Atmospheric Research) Community Atmospheric Model version 4 with chemistry (CAM4-chem) by implementing a 4-product volatility basis set (VBS) scheme, including NOx-dependent SOA yields and aging parameterizations. Small differences are found for the no-aging VBS and 2-product schemes; large increases in SOA production and the SOA-to-OA ratio are found for the aging scheme. The predicted organic aerosol amounts capture both the magnitude and distribution of US surface annual mean measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network by 50 %, and the simulated vertical profiles are within a factor of 2 compared to aerosol mass spectrometer (AMS) measurements from 13 aircraft-based field campaigns across different regions and seasons. We then perform sensitivity experiments to examine how the SOA loading responds to a 50 % reduction in anthropogenic nitric oxide (NO) emissions in different regions. We find limited SOA reductions of 0.9-5.6, 6.4-12.0 and 0.9-2.8 % for global, southeast US and Amazon NOx perturbations, respectively. The fact that SOA formation is almost unaffected by changes in NOx can be largely attributed to a limited shift in chemical regime, to buffering in chemical pathways (low- and high-NOx pathways, O3 versus NO3-initiated oxidation) and to offsetting tendencies in the biogenic versus anthropogenic SOA responses.

  3. Halogen-induced organic aerosol (XOA) formation and decarboxylation of carboxylic acids by reactive halogen species - a time-resolved aerosol flow-reactor study

    Science.gov (United States)

    Ofner, Johannes; Zetzsch, Cornelius

    2013-04-01

    Reactive halogen species (RHS) are released to the atmosphere from various sources like photo-activated sea-salt aerosol and salt lakes. Recent studies (Cai et al., 2006 and 2008, Ofner et al., 2012) indicate that RHS are able to interact with SOA precursors similarly to common atmospheric oxidizing gases like OH radicals and ozone. The reaction of RHS with SOA precursors like terpenes forms so-called halogen-induced organic aerosol (XOA). On the other hand, RHS are also able to change the composition of functional groups, e.g. to initiate the decarboxylation of carboxylic acids (Ofner et al., 2012). The present study uses a 50 cm aerosol flow-reactor, equipped with a solar simulator to investigate the time-resolved evolution and transformation of vibrational features in the mid-infrared region. The aerosol flow-reactor is coupled to a home-made multi-reflection cell (Ofner et al., 2010), integrated into a Bruker IFS 113v FTIR spectrometer. The reactor is operated with an inlet feed (organic compound) and a surrounding feed (reactive halogen species). The moveable inlet of the flow reactor allows us to vary reaction times between a few seconds and up to about 3 minutes. Saturated vapours of different SOA precursors and carboxylic acids were fed into the flow reactor using the moveable inlet. The surrounding feed inside the flow reactor was a mixture of zero air with molecular chlorine as the precursor for the formation of reactive halogen species. Using this setup, the formation of halogen-induced organic aerosol could be monitored with a high time resolution using FTIR spectroscopy. XOA formation is characterized by hydrogen-atom abstraction, carbon-chlorine bond formation and later, even formation of carboxylic acids. Several changes of the entire structure of the organic precursor, caused by the reaction of RHS, are visible. While XOA formation is a very fast process, the decarboxylation of carboxylic acids, induced by RHS is rather slow. However, XOA formation

  4. The Role of HO(x) in Super- and Subsonic Aircraft Exhaust Plumes

    Science.gov (United States)

    Hanisco, T. F.; Wennberg, P. O.; Cohen, R. C.; Anderson, J. G.; Fahey, D. W.; Keim, E. R.; Gao, R. S.; Wamsley, R. C.; Donnelly, S. G.; DelNegro, L. A.; hide

    1997-01-01

    The generation of sulfuric acid aerosols in aircraft exhaust has emerged as a critical issue in determining the impact of supersonic aircraft on stratospheric ozone. It has long been held that the first step in the mechanism of aerosol formation is the oxidation of SO2 emitted from the engine by OH in the exhaust plume. We report in situ measurements of OH and HO2 in the exhaust plumes of a supersonic (Air France Concorde) and a subsonic (NASA ER-2) aircraft in the lower stratosphere. These measurements imply that reactions with OH are responsible for oxidizing only a small fraction of SO2 (2%), and thus cannot explain the large number of particles observed in the exhaust wake of the Concorde.

  5. The role of HOx in super- and subsonic aircraft exhaust plumes

    Science.gov (United States)

    Hanisco, T. F.; Wennberg, P. O.; Cohen, R. C.; Anderson, J. G.; Fahey, D. W.; Keim, E. R.; Gao, R. S.; Wamsley, R. C.; Donnelly, S. G.; Del Negro, L. A.; Salawitch, R. J.; Kelly, K. K.; Proffitt, M. H.

    The generation of sulfuric acid aerosols in aircraft exhaust has emerged as a critical issue in determining the impact of supersonic aircraft on stratospheric ozone. It has long been held that the first step in the mechanism of aerosol formation is the oxidation of SO2 emitted from the engine by OH in the exhaust plume. We report in situ measurements of OH and HO2 in the exhaust plumes of a supersonic (Air France Concorde) and a subsonic (NASA ER-2) aircraft in the lower stratosphere. These measurements imply that reactions with OH are responsible for oxidizing only a small fraction of SO2 (2%), and thus cannot explain the large number of particles observed in the exhaust wake of the Concorde.

  6. Efficient Isoprene Secondary Organic Aerosol Formation from a Non-IEPOX Pathway

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Jiumeng; D’Ambro, Emma L.; Lee, Ben H.; Lopez-Hilfiker, Felipe D.; Zaveri, Rahul A.; Rivera-Rios, Jean C.; Keutsch, Frank N.; Iyer, Siddharth; Kurten, Theo; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.; Shilling, John E.; Thornton, Joel A.

    2016-09-20

    With a large global emission rate and high reactivity, isoprene has a profound effect upon atmospheric chemistry and composition. The atmospheric pathways by which isoprene converts to secondary organic aerosol (SOA) and how anthropogenic pollutants such as nitrogen oxides and sulfur affect this process are a subject of intense research because particles affect Earth’s climate and local air quality. In the absence of both nitrogen oxides and reactive aqueous seed particles, we measure SOA mass yields from isoprene photochemical oxidation of up to 15%, which are factors of 2, or more, higher than those typically used in coupled chemistry-climate models. SOA yield is initially constant with the addition of increasing amounts of nitric oxide (NO) but then sharply decreases for input concentrations above 10 ppbv. Online measurements of aerosol molecular composition show that the fate of second-generation RO2 radicals is key to understanding the efficient SOA formation and the NOx dependent yields described here and in the literature. These insights allow for improved quantitative estimates of SOA formation in the pre-industrial atmosphere and in biogenic-rich regions with limited anthropogenic impacts and suggest a more complex representation of NOx dependent SOA yields may be important in models.

  7. Formation of secondary aerosols from biomass burning plumes: chamber simulation study

    Science.gov (United States)

    Wang, X.; Hu, Q.; Fang, Z.; Deng, W.

    2015-12-01

    Biomass burning contributed substantially to carbonaceous aerosols in China's ambient air, even in its highly industrialized megacities, based on recent source attributions by receptor modeling or by molecular and isotopic tracers. Although chemical evolution of biomass burning plumes in the ambient is a vital issue for the study of climatic and health effects, the understanding of secondary pollutants formation during the aging of biomass burning plumes is far from complete. Here we collected typical agriculture residues and forest plant branches in the Pearl River Delta in south China, and got them burned in laboratory-controlled conditions and introduced the plumes from burning these biomass directly into the GIGCAS indoor smog chamber with a reactor of 30 m3 to investigate the photochemical aging of the plumes. The inorganic trace gases, including SO2, NOx, NH3 and O3, were monitored online with chemiluminescence gas analyzers, precursor volatile organic compounds (VOCs) were monitor online with a PTR-ToF-MS and offline by a preconcentrator coupled with a gas chromatography-mass selective detector/flame ionization detector/electron capture detector (GC-MSD/FID/ECD), particle number concentrations and size distributions were obtained using a scanning mobility particle sizer (SMPS), and a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) was used to measure the chemical compositions and evolutions of submicron aerosols and to trace the change in the average element ratios of organics, like H/C, O/C, and N/C. The results from the study were summarized in the following aspects: 1) primary emission factors of gaseous and particulate pollutants from burning of typical biomass including agricultural remains and forest wood plants; 2) yields of secondary pollutants, including secondary inorganic and organic aerosols and gaseous products (like O3) during photochemical aging of biomass burning plumes; 3) relationship between the formed secondary

  8. Secondary organic aerosol formation from the ozonolysis of 2-carene and 3-carene

    Science.gov (United States)

    Mellouki, A.; Chen, H.; Bernard, F.; Cazaunau, M.; Grosselin, B.; Daele, V.; Chen, J.

    2013-12-01

    The atmospheric degradation of terpenes in the remote areas such as those with coniferous forests is known to lead to the formation and growth of atmospheric new particles. 2-carene and 3-carene have been reported to be present in number of such areas. Hence, their oxidation may represent an important source of secondary organic aerosols in some specific regions. 2-carene and 3-carene possess a structure of endocyclic double bonds which make them reactive toward ozone under atmospheric conditions. We have conducted a study on the reactions of ozone with 2-carene and 3-carene using a flow reactor dedicated to the investigation of secondary organic aerosol (SOA) formation. The reactor is equipped with an ozone generator and a movable injector which allows the reaction to occur within a short time range (typically 17 - 48 seconds). This enables us to investigate the initial steps of the SOA formation. In a first series of experiments, we have determined the rate constant for the reaction of ozone with 3-carene under pseudo-first-order conditions. The rate constant value measured was 3.8 x 10-17 molecule-1s-1, at 298 K, in agreement with the literatures and simulation chamber experiments. We have then investigated the SOA formation from the ozonolysis of 2-carene and 3-carene. By adjusting the residence time and initial concentration of carenes and ozone, number concentration of SOA have been measured for short reactions times and low concentrations of reactants. Nucleation thresholds of 2-carene and 3-carene were extracted from the plots of log N = f(Δ[Carenes]).

  9. Secondary Organic Aerosol Formation from Acetylene (C2H2: seed effect on SOA yields due to organic photochemistry in the aerosol aqueous phase

    Directory of Open Access Journals (Sweden)

    P. J. Ziemann

    2009-03-01

    Full Text Available The lightest Non Methane HydroCarbon (NMHC, i.e., acetylene (C2H2 is found to form secondary organic aerosol (SOA. Contrary to current belief, the number of carbon atoms, n, for a NMHC to act as SOA precursor is lowered to n=2 here. The OH-radical initiated oxidation of C2H2 forms glyoxal (CHOCHO as the highest yield product, and >99% of the SOA from C2H2 is attributed to CHOCHO. SOA formation from C2H2 and CHOCHO was studied in a photochemical and a dark simulation chamber. Further, the experimental conditions were varied with respect to the chemical composition of the seed aerosols, mild acidification with sulphuric acid (SA, 3aerosols is found responsible for this seed effect. WSOC photochemistry enhances the SOA source from CHOCHO, while seeds containing amino acids (AA and/or SA showed among the lowest of all YSOA values, and largely suppress the photochemical enhancement on the rate of CHOCHO uptake. Our results give first evidence for the importance of heterogeneous photochemistry of CHOCHO in SOA formation, and identify a potential bias in the currently available YSOA data for other SOA precursor NMHCs. We demonstrate that SOA formation via the aqueous phase is not limited to cloud droplets, but proceeds also in the absence of clouds, i.e., does not stop once a cloud droplet evaporates. Atmospheric models need to be expanded to include SOA formation from WSOC photochemistry of CHOCHO, and possibly other α-dicarbonyls, in aqueous aerosols.

  10. Role of secondary aerosols in haze formation in summer in the Megacity Beijing.

    Science.gov (United States)

    Han, Tingting; Liu, Xingang; Zhang, Yuanhang; Qu, Yu; Zeng, Limin; Hu, Min; Zhu, Tong

    2015-05-01

    A field experiment from 18 August to 8 September 2006 in Beijing, China, was carried out. A hazy day was defined as visibilityaerosol) concentrations. The average values with standard deviation of SO4(2-), NO3-, NH4+ and SOA were 49.8 (±31.6), 31.4 (±22.3), 25.8 (±16.6) and 8.9 (±4.1)μg/m3, respectively, during the haze episodes, which were 4.3, 3.4, 4.1, and 1.7 times those in the non-haze days. The SO4(2-), NO3-, NH4+, and SOA accounted for 15.8%, 8.8%, 7.3%, and 6.0% of the total mass concentration of PM10 during the non-haze days. The respective contributions of SNA species to PM10 rose to about 27.2%, 15.9%, and 13.9% during the haze days, while the contributions of SOA maintained the same level with a slight decrease to about 4.9%. The observed mass concentrations of SNA and SOA increased with the increase of PM10 mass concentration, however, the rate of increase of SNA was much faster than that of the SOA. The SOR (sulfur oxidation ratio) and NOR (nitrogen oxidation ratio) increased from non-haze days to hazy days, and increased with the increase of RH. High concentrations of aerosols and water vapor favored the conversion of SO2 to SO4(2-) and NO2 to NO3-, which accelerated the accumulation of the aerosols and resulted in the formation of haze in Beijing. Copyright © 2015. Published by Elsevier B.V.

  11. Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms

    Directory of Open Access Journals (Sweden)

    S.-L. Sihto

    2006-01-01

    Full Text Available We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland. During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.

  12. Formation of secondary organic aerosol and oligomers from the ozonolysis of enol ethers

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    A. Sadezky

    2006-01-01

    Full Text Available Formation of secondary organic aerosol has been observed in the gas phase ozonolysis of a series of enol ethers, among them several alkyl vinyl ethers (AVE, ROCH=CH2, such as ethyl, propyl, n-butyl, iso-butyl, t-butyl vinyl ether, and ethyl propenyl ether (EPE, C2H5OCH=CHCH3. The ozonolysis has been studied in a 570 l spherical glass reactor at ambient pressure (730 Torr and room temperature (296 K. Gas phase reaction products were investigated by in-situ FTIR spectroscopy, and secondary organic aerosol (SOA formation was monitored by a scanning mobility particle sizer (SMPS. The chemical composition of the formed SOA was analysed by a hybrid mass spectrometer using electrospray ionization (ESI. The main stable gas phase reaction product is the respective alkyl formate ROC(OH, formed with yields of 60 to 80%, implying that similar yields of the corresponding excited Criegee Intermediates (CI CH2O2 for the AVE and CH3CHO2 for EPE are generated. Measured SOA yields are between 2 to 4% for all enol ethers. Furthermore, SOA formation is strongly reduced or suppressed by the presence of an excess of formic acid, which acts as an efficient CI scavenger. Chemical analysis of the formed SOA by ESI(+/MS-TOF allows to identify oligomeric compounds in the mass range 200 to 800 u as its major constituents. Repetitive chain units are identified as CH2O2 (mass 46 for the AVE and C2H4O2 (mass 60 for EPE and thus have the same chemical compositions as the respective major Criegee Intermediates formed during ozonolysis of these ethers. The oligomeric structure and chain unit identity are confirmed by HPLC/ESI(+/MS-TOF and ESI(+/MS/MS-TOF experiments, whereby successive and systematic loss of a fragment with mass 46 for the AVE (and mass 60 for EPE is observed. It is proposed that the oligomer has the following basic structure of an oligoperoxide, -[CH(R-O-O]n-, where R=H for the AVE and R=CH3 for the EPE. Oligoperoxide formation is thus suggested to be another

  13. The critical assessment of vapour pressure estimation methods for use in modelling the formation of atmospheric organic aerosol

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    M. H. Barley

    2010-01-01

    Full Text Available A selection of models for estimating vapour pressures have been tested against experimental data for a set of compounds selected for their particular relevance to the formation of atmospheric aerosol by gas-liquid partitioning. The experimental vapour pressure data (all <100 Pa of 45 multifunctional compounds provide a stringent test of the estimation techniques, with a recent complex group contribution method providing the best overall results. The effect of errors in vapour pressures upon the formation of organic aerosol by gas-liquid partitioning in an atmospherically relevant example is also investigated. The mass of organic aerosol formed under typical atmospheric conditions was found to be very sensitive to the variation in vapour pressure values typically present when comparing estimation methods.

  14. Formation of semivolatile inorganic aerosols in the Mexico City Metropolitan Area during the MILAGRO campaign

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    V. A. Karydis

    2011-12-01

    Full Text Available One of the most challenging tasks for chemical transport models (CTMs is the prediction of the formation and partitioning of the major semi-volatile inorganic aerosol components (nitrate, chloride, ammonium between the gas and particulate phases. In this work the PMCAMx-2008 CTM, which includes the recently developed aerosol thermodynamic model ISORROPIA-II, is applied in the Mexico City Metropolitan Area in order to simulate the formation of the major inorganic aerosol components. The main sources of SO2 (such as the Miguel Hidalgo Refinery and the Francisco Perez Rios Power Plant in the Mexico City Metropolitan Area (MCMA are located in Tula, resulting in high predicted PM1 (particulate matter with diameter less than 1 μm sulfate concentrations (over 25 μg m-3 in that area. The average predicted PM1 nitrate concentrations are up to 3 μg m−3 (with maxima up to 11 μg m−3 in and around the urban center, mostly produced from local photochemistry. The presence of calcium coming from the Tolteca area (7 μg m−3 as well as the rest of the mineral cations (1 μg m−3 potassium, 1 μg m−3 magnesium, 2 μg m−3 sodium, and 3 μg m−3 calcium from the Texcoco Lake resulted in the formation of a significant amount of aerosol nitrate in the coarse mode with concentrations up to 3 μg m−3 over these areas. PM1−10 (particulate matter with diameter between 1 and 10 μm chloride is also high and its concentration exceeds 2 μg m−3 in Texcoco Lake. PM1 ammonium concentrations peak at the center of Mexico City (2 μg m−3 and the Tula vicinity (2.5 μg m−3. The performance of the model for the major inorganic PM components (sulfate, ammonium, nitrate, chloride, sodium, calcium, and magnesium is encouraging. At the T0 measurement site, located in the

  15. Formation of semivolatile inorganic aerosols in the Mexico City Metropolitan Area during the MILAGRO campaign

    Science.gov (United States)

    Karydis, V. A.; Tsimpidi, A. P.; Lei, W.; Molina, L. T.; Pandis, S. N.

    2011-12-01

    One of the most challenging tasks for chemical transport models (CTMs) is the prediction of the formation and partitioning of the major semi-volatile inorganic aerosol components (nitrate, chloride, ammonium) between the gas and particulate phases. In this work the PMCAMx-2008 CTM, which includes the recently developed aerosol thermodynamic model ISORROPIA-II, is applied in the Mexico City Metropolitan Area in order to simulate the formation of the major inorganic aerosol components. The main sources of SO2 (such as the Miguel Hidalgo Refinery and the Francisco Perez Rios Power Plant) in the Mexico City Metropolitan Area (MCMA) are located in Tula, resulting in high predicted PM1 (particulate matter with diameter less than 1 μm) sulfate concentrations (over 25 μg m-3) in that area. The average predicted PM1 nitrate concentrations are up to 3 μg m-3 (with maxima up to 11 μg m-3) in and around the urban center, mostly produced from local photochemistry. The presence of calcium coming from the Tolteca area (7 μg m-3) as well as the rest of the mineral cations (1 μg m-3 potassium, 1 μg m-3 magnesium, 2 μg m-3 sodium, and 3 μg m-3 calcium) from the Texcoco Lake resulted in the formation of a significant amount of aerosol nitrate in the coarse mode with concentrations up to 3 μg m-3 over these areas. PM1-10 (particulate matter with diameter between 1 and 10 μm) chloride is also high and its concentration exceeds 2 μg m-3 in Texcoco Lake. PM1 ammonium concentrations peak at the center of Mexico City (2 μg m-3) and the Tula vicinity (2.5 μg m-3). The performance of the model for the major inorganic PM components (sulfate, ammonium, nitrate, chloride, sodium, calcium, and magnesium) is encouraging. At the T0 measurement site, located in the Mexico City urban center, the average measured values of PM1 sulfate, nitrate, ammonium, and chloride are 3.5 μg m-3, 3.5 μg m-3, 2.1 μg m-3, and 0.36 μg m-3, respectively. The corresponding predicted values are 3.7

  16. Formation of secondary organic aerosol in the Paris pollution plume and its impact on surrounding regions

    Science.gov (United States)

    Zhang, Q. J.; Beekmann, M.; Freney, E.; Sellegri, K.; Pichon, J. M.; Schwarzenboeck, A.; Colomb, A.; Bourrianne, T.; Michoud, V.; Borbon, A.

    2015-12-01

    Secondary pollutants such as ozone, secondary inorganic aerosol, and secondary organic aerosol formed in the plumes of megacities can affect regional air quality. In the framework of the FP7/EU MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) project, an intensive campaign was launched in the greater Paris region in July 2009. The major objective was to quantify different sources of organic aerosol (OA) within a megacity and in its plume. In this study, we use airborne measurements aboard the French ATR-42 aircraft to evaluate the regional chemistry-transport model CHIMERE within and downwind of the Paris region. Two mechanisms of secondary OA (SOA) formation are used, both including SOA formation from oxidation and chemical aging of primary semivolatile and intermediate volatility organic compounds (SI-SOA) in the volatility basis set (VBS) framework. As for SOA formed from traditional VOC (volatile organic compound) precursors (traditional SOA), one applies chemical aging in the VBS framework adopting different SOA yields for high- and low-NOx environments, while another applies a single-step oxidation scheme without chemical aging. Two emission inventories are used for discussion of emission uncertainties. The slopes of the airborne OA levels versus Ox (i.e., O3 + NO2) show SOA formation normalized with respect to photochemical activity and are used for specific evaluation of the OA scheme in the model. The simulated slopes were overestimated slightly by factors of 1.1, 1.7 and 1.3 with respect to those observed for the three airborne measurements, when the most realistic "high-NOx" yields for traditional SOA formation in the VBS scheme are used in the model. In addition, these slopes are relatively stable from one day to another, which suggests that they are characteristic for the given megacity plume environment. The configuration with increased primary

  17. Lessons Learned About Organic Aerosol Formation in the Southeast U.S. Using Observations and Modeling

    Science.gov (United States)

    Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA). In this work, modeling of isoprene SOA via heterogeneous uptake is explored and compared to observations from the Southern Oxidant and Aerosol Study (SOAS).

  18. Simulating ultrafine particle formation in Europe using a regional CTM: Contribution of primary emissions versus secondary formation to aerosol number concentrations

    NARCIS (Netherlands)

    Fountoukis, C.; Riipinen, I.; Denier Van Der Gon, H.A.C.; Charalampidis, P.E.; Pilinis, C.; Wiedensohler, A.; O'Dowd, C.; Putaud, J.P.; Moerman, M.; Pandis, S.N.

    2012-01-01

    A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic

  19. Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the Megapoli summer and winter campaigns

    NARCIS (Netherlands)

    Fountoukis, C.; Megaritis, A.G.; Skyllakou, K.; Charalampidis, P.E.; Denier van der Gon, H.A.C.; Crippa, M.; Prevot, A.S.H.; Fachinger, F.; Wiedensohler, A.; Pilinis, C.; Pandis, S.N.

    2016-01-01

    We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 x 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol dur-ing a summer (July 2009) and a winter (January/February 2010) period as part of

  20. In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol

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    A. Monod

    2009-07-01

    Full Text Available The fate of methacrolein in cloud evapo-condensation cycles was experimentally investigated. To this end, aqueous-phase reactions of methacrolein with OH radicals were performed (as described in Liu et al., 2009, and the obtained solutions were then nebulized and dried into a mixing chamber. ESI-MS and ESI-MS/MS analyses of the aqueous phase composition denoted the formation of high molecular weight multifunctional products containing hydroxyl, carbonyl and carboxylic acid moieties. The time profiles of these products suggest that their formation can imply radical pathways. These high molecular weight organic products are certainly responsible for the formation of secondary organic aerosol (SOA observed during the nebulization experiments. The size, number and mass concentration of these particles increased significantly with the reaction time: after 22 h of reaction, the aerosol mass concentration was about three orders of magnitude higher than the initial aerosol quantity. The evaluated SOA yield ranged from 2 to 12%. These yields were confirmed by another estimation method based on the hygroscopic and volatility properties of the obtained SOA measured and reported by Michaud et al. (2009. These results provide, for the first time to our knowledge, strong experimental evidence that cloud processes can act, through photooxidation reactions, as important contributors to secondary organic aerosol formation in the troposphere.

  1. Secondary Organic Aerosol (SOA) formation from the β-pinene + NO3 system: effect of humidity and peroxy radical fate

    Science.gov (United States)

    Boyd, C. M.; Sanchez, J.; Xu, L.; Eugene, A. J.; Nah, T.; Tuet, W. Y.; Guzman, M. I.; Ng, N. L.

    2015-01-01

    The formation of secondary organic aerosol (SOA) from the oxidation of β-pinene via nitrate radicals is investigated in the Georgia Tech Environmental Chamber facility (GTEC). Aerosol yields are determined for experiments performed under both dry (RH organic nitrate species (with molecular weights of 215, 229, 231 and 245 amu) are detected by chemical ionization mass spectrometry and their formation mechanisms are proposed. The ions at m/z 30 (NO+) and m/z 46 (NO2+) contribute about 11% to the total organics signal in the typical aerosol mass spectrum, with NO+ : NO2+ ratio ranging from 6 to 9 in all experiments conducted. The SOA yields in the "RO2 + NO3 dominant" and "RO2 + HO2 dominant" experiments are comparable. For a wide range of organic mass loadings (5.1-216.1 μg m-3), the aerosol mass yield is calculated to be 27.0-104.1%. Although humidity does not appear to affect SOA yields, there is evidence of particle-phase hydrolysis of organic nitrates, which are estimated to compose 45-74% of the organic aerosol. The extent of organic nitrate hydrolysis is significantly lower than that observed in previous studies on photooxidation of volatile organic compounds in the presence of NOx. It is estimated that about 90 and 10% of the organic nitrates formed from the β-pinene + NO3 reaction are primary organic nitrates and tertiary organic nitrates, respectively. While the primary organic nitrates do not appear to hydrolyze, the tertiary organic nitrates undergo hydrolysis with a lifetime of 3-4.5 h. Results from this laboratory chamber study provide the fundamental data to evaluate the contributions of monoterpene + NO3 reaction to ambient organic aerosol measured in the southeastern United States, including the Southern Oxidant and Aerosol Study (SOAS) and the Southeastern Center for Air Pollution and Epidemiology (SCAPE) study.

  2. Size-resolved aerosol water-soluble ions during the summer and winter seasons in Beijing: Formation mechanisms of secondary inorganic aerosols.

    Science.gov (United States)

    Liu, Zirui; Xie, Yuzhu; Hu, Bo; Wen, Tianxue; Xin, Jinyuan; Li, Xingru; Wang, Yuesi

    2017-09-01

    Size-segregated water-soluble ionic species (WSIs) were measured using an Anderson cascade impactor from Jul. to Aug. 2008 and from Dec. 2009 to Feb. 2010 in urban Beijing. The results showed that fine particles (PM2.1, Dp aerosols (SIAs, the sum of SO42-, NO3- and NH4+) accounted for more than 30% of the fine particles, which were greatly elevated during particle pollution events (PM events), thereby leading to an alteration of the size distributions of SO42- and NO3- to nearly single fine-mode distributions peaking at 0.65-2.1 μm. This finding suggests that heterogeneous aqueous reactions were enhanced at high RH values. SIAs also increased during dust events, particularly for coarse mode SO42-, which indicated enhanced heterogeneous reactions on the dust surface. The positive matrix factorization (PMF) model was used to resolve the bulk mass size distributions into condensation, droplet, and coarse modes, representing the three major sources of the particles. The formation of SO42- was attributed primarily to in-cloud or aerosol droplet processes during summer (45%), and the heterogeneous reaction of SO2 on mineral dust surfaces was an important formation pathway during winter (45%). The formation pathways of NO3- in fine particles were similar to those of SO42-, where over 30% were formed by in-cloud processes. This work provides important field measurement-based evidence for understanding the formation pathway of secondary inorganic aerosols in the megacity of Beijing. Copyright © 2017 Elsevier Ltd. All rights reserved.

  3. Modeling secondary organic aerosol formation through cloud processing of organic compounds

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    J. Chen

    2007-10-01

    Full Text Available Interest in the potential formation of secondary organic aerosol (SOA through reactions of organic compounds in condensed aqueous phases is growing. In this study, the potential formation of SOA from irreversible aqueous-phase reactions of organic species in clouds was investigated. A new proposed aqueous-phase chemistry mechanism (AqChem is coupled with the existing gas-phase Caltech Atmospheric Chemistry Mechanism (CACM and the Model to Predict the Multiphase Partitioning of Organics (MPMPO that simulate SOA formation. AqChem treats irreversible organic reactions that lead mainly to the formation of carboxylic acids, which are usually less volatile than the corresponding aldehydic compounds. Zero-dimensional model simulations were performed for tropospheric conditions with clouds present for three consecutive hours per day. Zero-dimensional model simulations show that 48-h average SOA formation is increased by 27% for a rural scenario with strong monoterpene emissions and 7% for an urban scenario with strong emissions of aromatic compounds, respectively, when irreversible organic reactions in clouds are considered. AqChem was also incorporated into the Community Multiscale Air Quality Model (CMAQ version 4.4 with CACM/MPMPO and applied to a previously studied photochemical episode (3–4 August 2004 focusing on the eastern United States. The CMAQ study indicates that the maximum contribution of SOA formation from irreversible reactions of organics in clouds is 0.28 μg m−3 for 24-h average concentrations and 0.60 μg m−3 for one-hour average concentrations at certain locations. On average, domain-wide surface SOA predictions for the episode are increased by 9% when irreversible, in-cloud processing of organics is considered. Because aldehydes of carbon number greater than four are assumed to convert fully to the corresponding carboxylic acids upon reaction with OH in cloud droplets and this assumption may overestimate

  4. Emission of sunscreen salicylic esters from desert vegetation and their contribution to aerosol formation

    Science.gov (United States)

    Matsunaga, S. N.; Guenther, A. B.; Potosnak, M. J.; Apel, E. C.

    2008-12-01

    Biogenic volatile organic compounds (BVOC) produced by plants are known to have an important role in atmospheric chemistry. However, our knowledge of the range of BVOCs produced by different plant processes is still expanding, and there remain poorly understood categories of BVOCs. In this study, emissions of a novel class of BVOC emissions were investigated in a desert region. Our study considered 8 species of common desert plants: blackbrush (Coleogyne ramosissima), desert willow (Chilopsis linearis), mesquite (Prosopis glandulosa), mondel pine (Pinus eldarica), pinyon pine (Pinus monophylla), cottonwood (Populus deltoides), saguaro cactus (Carnegiea gigantea) and yucca (Yucca baccata). The measurements focused on BVOCs with relatively high molecular weight (>C15) and/or an oxygenated functional group. Significantly high emission rates of two salicylic esters were found for blackbrush, desert willow and mesquite with emission rates of 3.1, 1.0 and 4.8μgC dwg-1 h-1, respectively (dwg; dry weight of the leaves in gram). The salicylic esters were identified as 2-ethylhexenyl salicylate (2-EHS) and 3,3,5-trimethylcyclohexenyl salicylate (homosalate) and are known as effective ultraviolet (UV) absorbers. We propose that the plants derive a protective benefit against UV radiation from the salicylic esters and that the emission process is driven by the physical evaporation of the salicylic esters due to the high ambient temperatures. In addition, the salicylic esters are predicted to be an effective precursor of secondary organic aerosol (SOA) because they probably produce oxidation products that can condense onto the aerosol phase. We estimated the contribution of the sunscreen esters themselves and their oxidation products on the SOA formation for the Las Vegas area using a BVOC emission model. The contribution was estimated to reach 50% of the biogenic terpenoid emission in the landscapes dominated by desert willow and mesquite and 13% in the Las Vegas area. The

  5. Kinetics of oxygenated product formation during the heterogeneous oxidation of organic aerosol

    Science.gov (United States)

    Kolesar, K. R.; Cappa, C. D.; Wilson, K. R.

    2014-12-01

    Oxidation of organic aerosols can lead to changes in their atmospheric lifetime, optical properties and health effects. Whereas much is known about the rates of reaction and subsequent branching ratios of gas-phase organic species, much less is known about their condensed phase counterparts. The determination of the kinetics and abundances of the oxidation products associated with condensed phase reactions is needed to understand the oxidation reaction pathways and their branching ratios. The Vacuum Ultraviolet Aerosol Mass Spectrometer (VUV-AMS) at the Chemical Dynamics Beamline at Lawrence Berkeley National Laboratory has been useful in determining the reaction rate constants for a number of condensed phase organic compounds with oxidants such as OH and O3. The relatively soft ionization in the VUV-AMS leads to substantially less fragmentation than other AMS instruments that use electron impact ionization, and therefore preserves a greater amount of molecular information about parent molecules. Previously, ketones formed from the heterogenous oxidation of model organic compounds have been identified and their formation kinetics quantified. However, other possible products, such as alcohols and organic peroxides, have not previously been identified in the VUV-AMS mass spectra or characterized as these are subject to greater fragmentation. Here, we present a method in which the fragmentation pattern is specified for each alcohol isomer formed from the oxidation of two model organic compounds, bis-2-ethylhexl sebacate and squalane. From this we are able to define unique m/z fragments for each isomer from which we derive information about alcohol and abundances. This study demonstrates additional methods for the analysis of mass spectra obtained with the VUV-AMS as well as provides insights into condensed phase oxidation kinetics.

  6. Model analysis of secondary organic aerosol formation by glyoxal in laboratory studies: the case for photoenhanced chemistry.

    Science.gov (United States)

    Sumner, Andrew J; Woo, Joseph L; McNeill, V Faye

    2014-10-21

    The reactive uptake of glyoxal by atmospheric aerosols is believed to be a significant source of secondary organic aerosol (SOA). Several recent laboratory studies have been performed with the goal of characterizing this process, but questions remain regarding the effects of photochemistry on SOA growth. We applied GAMMA (McNeill et al. Environ. Sci. Technol. 2012, 46, 8075-8081), a photochemical box model with coupled gas-phase and detailed aqueous aerosol-phase chemistry, to simulate aerosol chamber studies of SOA formation by the uptake of glyoxal by wet aerosol under dark and irradiated conditions (Kroll et al. J. Geophys. Res. 2005, 110 (D23), 1-10; Volkamer et al. Atmos. Chem. Phys. 2009, 9, 1907-1928; Galloway et al. Atmos. Chem. Phys. 2009, 9, 3331- 306 3345 and Geophys. Res. Lett. 2011, 38, L17811). We find close agreement between simulated SOA growth and the results of experiments conducted under dark conditions using values of the effective Henry's Law constant of 1.3-5.5 × 10(7) M atm(-1). While irradiated conditions led to the production of some organic acids, organosulfates, and other oxidation products via well-established photochemical mechanisms, these additional product species contribute negligible aerosol mass compared to the dark uptake of glyoxal. Simulated results for irradiated experiments therefore fell short of the reported SOA mass yield by up to 92%. This suggests a significant light-dependent SOA formation mechanism that is not currently accounted for by known bulk photochemistry, consistent with recent laboratory observations of SOA production via photosensitizer chemistry.

  7. Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements

    Directory of Open Access Journals (Sweden)

    A. T. Lambe

    2011-03-01

    Full Text Available Motivated by the need to develop instrumental techniques for characterizing organic aerosol aging, we report on the performance of the Toronto Photo-Oxidation Tube (TPOT and Potential Aerosol Mass (PAM flow tube reactors under a variety of experimental conditions. The PAM system was designed with lower surface-area-to-volume (SA/V ratio to minimize wall effects; the TPOT reactor was designed to study heterogeneous aerosol chemistry where wall loss can be independently measured. The following studies were performed: (1 transmission efficiency measurements for CO2, SO2, and bis(2-ethylhexyl sebacate (BES particles, (2 H2SO4 yield measurements from the oxidation of SO2, (3 residence time distribution (RTD measurements for CO2, SO2, and BES particles, (4 aerosol mass spectra, O/C and H/C ratios, and cloud condensation nuclei (CCN activity measurements of BES particles exposed to OH radicals, and (5 aerosol mass spectra, O/C and H/C ratios, CCN activity, and yield measurements of secondary organic aerosol (SOA generated from gas-phase OH oxidation of m-xylene and α-pinene. OH exposures ranged from (2.0 ± 1.0 × 1010 to (1.8 ± 0.3 × 1012 molec cm−3 s. Where applicable, data from the flow tube reactors are compared with published results from the Caltech smog chamber. The TPOT yielded narrower RTDs. However, its transmission efficiency for SO2 was lower than that for the PAM. Transmission efficiency for BES and H2SO4 particles was size-dependent and was similar for the two flow tube designs. Oxidized BES particles had similar O/C and H/C ratios and CCN activity at OH exposures greater than 1011 molec cm−3 s, but different CCN activity at lower OH exposures. The O/C ratio, H/C ratio, and yield of m-xylene and α-pinene SOA was strongly affected by reactor design and

  8. Hydrochloric acid aerosol formation by the interaction of hydrogen chloride with humid air

    Science.gov (United States)

    Rhein, R. A.

    1973-01-01

    The conditions in which hydrochloric acid aerosol is predicted by the interaction of hydrogen chloride gas with the water vapor in humid air are analyzed. The liquid gas phase equilibrium for the HCL-H2O system is expressed in terms of relative humidity and hydrogen chloride concentration as parts per million, units commonly used in pollution studies. Presented are the concentration (wt %) of HC1 in the aerosol and the concentration of aerosol (ppm) predicted.

  9. 3rd hand smoking; heterogeneous oxidation of nicotine and secondary aerosol formation in the indoor environment

    Science.gov (United States)

    Petrick, Lauren; Dubowski, Yael

    2010-05-01

    Tobacco smoking is well known as a significant source of primary indoor air pollutants. However, only recently has it been recognized that the impact of Tobacco smoking may continue even after the cigarette has been extinguished (i.e., third hand smoke) due to the effect of indoor surfaces. These surfaces may affect the fate of tobacco smoke in the form of secondary reactions and pollutants, including secondary organic aerosol (SOA) formation. Fourier Transform Infrared spectrometry with Attenuated Total Reflection (FTIR-ATR) in tandem with a Scanning Mobility Particle Sizing (SMPS) system was used to monitor the ozonation of cellulose sorbed nicotine and resulting SOA formation. SOA formation began at onset of ozone introduction ([O3] = 60 ± 5 ppb) with a size distribution of dp ≤ 25 nm, and was determined to be a result of heterogeneous reaction (opposed to homogeneous). SOA yield from reacted surface nicotine was on the order of 10 %. Simultaneous to SOA monitoring, FTIR-ATR spectra showed surface changes in the nicotine film as the reaction progressed, revealing a pseudo first-order surface reaction rate of 0.0026 ± 0.0008 min-1. Identified surface oxidation products included: cotinine, myosmine, methylnicotinamide and nicotyrine. Surface reaction rate was found to be partially inhibited at high relative humidity. Given the toxicity of some of the identified products (e.g., cotinine has shown potential mutagenicity and teratogenicity) and that small particles may contribute to adverse health effects, the present study indicates that exposure to 3rd hand smoke ozonation products may pose additional health risks.

  10. Secondary organic aerosol formation from ozone reactions with single terpenoids and terpenoid mixtures

    Science.gov (United States)

    Waring, Michael S.; Wells, J. Raymond; Siegel, Jeffrey A.

    2011-08-01

    Ozone reacts with indoor-emitted terpenoids to form secondary organic aerosol (SOA). Most SOA research has focused on ozone reactions with single terpenoids or with consumer products, and this paper reports the results from an investigation of SOA formation from ozone reactions with both single terpenoids and mixtures of D-limonene, α-pinene, and α-terpineol. Transient experiments were conducted at low (25 ppb) and high (100 ppb) initial concentrations of ozone. The three terpenoids were tested singly and in combinations in a manner that controlled for their different reaction rates with ozone. The SOA formation was assessed by examining the evolution in time of the resulting number size-distributions and estimates of the mass concentrations. The results suggest that at higher ozone and terpenoid concentrations, SOA number formation follows a linear trend as a function of the initial rate of reaction. This finding was valid for both single terpenoids and mixtures. Generally speaking, higher ozone and terpenoid concentrations also led to larger geometric mean diameters and smaller geometric standard deviations of fitted lognormal distributions of the formed SOA. By assuming a density, mass concentrations were also assessed and did not follow as consistent of a trend. At low ozone concentration conditions, reactions with only D-limonene yielded the largest number concentrations of any experiment, even more than experiments with mixtures containing D-limonene and much higher overall terpenoid concentrations. This finding was not seen for high ozone concentrations. These experiments demonstrate quantifiable trends for SOA forming reactions of ozone and mixtures, and this work provides a framework for expanding these results to more complex mixtures and consumer products.

  11. Insight into winter haze formation mechanisms based on aerosol hygroscopicity and effective density measurements

    Science.gov (United States)

    Xie, Yuanyuan; Ye, Xingnan; Ma, Zhen; Tao, Ye; Wang, Ruyu; Zhang, Ci; Yang, Xin; Chen, Jianmin; Chen, Hong

    2017-06-01

    We characterize a representative particulate matter (PM) episode that occurred in Shanghai during winter 2014. Particle size distribution, hygroscopicity, effective density, and single particle mass spectrometry were determined online, along with offline analysis of water-soluble inorganic ions. The mass ratio of SNA / PM1. 0 (sulfate, nitrate, and ammonium) fluctuated slightly around 0.28, suggesting that both secondary inorganic compounds and carbonaceous aerosols contributed substantially to the haze formation, regardless of pollution level. Nitrate was the most abundant ionic species during hazy periods, indicating that NOx contributed more to haze formation in Shanghai than did SO2. During the representative PM episode, the calculated PM was always consistent with the measured PM1. 0, indicating that the enhanced pollution level was attributable to the elevated number of larger particles. The number fraction of the near-hydrophobic group increased as the PM episode developed, indicating the accumulation of local emissions. Three banana-shaped particle evolutions were consistent with the rapid increase of PM1. 0 mass loading, indicating that the rapid size growth by the condensation of condensable materials was responsible for the severe haze formation. Both hygroscopicity and effective density of the particles increased considerably with growing particle size during the banana-shaped evolutions, indicating that the secondary transformation of NOx and SO2 was one of the most important contributors to the particle growth. Our results suggest that the accumulation of gas-phase and particulate pollutants under stagnant meteorological conditions and subsequent rapid particle growth by secondary processes were primarily responsible for the haze pollution in Shanghai during wintertime.

  12. Aerosol surface area concentration: a governing factor in new particle formation in Beijing

    Directory of Open Access Journals (Sweden)

    R. Cai

    2017-10-01

    Full Text Available The predominating role of aerosol Fuchs surface area, AFuchs, in determining the occurrence of new particle formation (NPF events in Beijing was elucidated in this study. The analysis was based on a field campaign from 12 March to 6 April 2016 in Beijing, during which aerosol size distributions down to  ∼  1 nm and sulfuric acid concentrations were simultaneously monitored. The 26 days were classified into 11 typical NPF days, 2 undefined days, and 13 non-event days. A dimensionless factor, LΓ, characterized by the relative ratio of the coagulation scavenging rate over the condensational growth rate (Kuang et al., 2010, was applied in this work to reveal the governing factors for NPF events in Beijing. The three parameters determining LΓ are sulfuric acid concentration, the growth enhancement factor characterized by contribution of other gaseous precursors to particle growth, Γ, and AFuchs. Different from other atmospheric environments, such as in Boulder and Hyytiälä, the daily-maximum sulfuric acid concentration and Γ in Beijing varied in a narrow range with geometric standard deviations of 1.40 and 1.31, respectively. A positive correlation between the estimated new particle formation rate, J1.5, and sulfuric acid concentration was found with a mean fitted exponent of 2.4. However, the maximum sulfuric acid concentrations on NPF days were not significantly higher (even lower, sometimes than those on non-event days, indicating that the abundance of sulfuric acid in Beijing was high enough to initiate nucleation, but may not necessarily lead to NPF events. Instead, AFuchs in Beijing varied greatly among days with a geometric standard deviation of 2.56, whereas the variabilities of AFuchs in Tecamac, Atlanta, and Boulder were reported to be much smaller. In addition, there was a good correlation between AFuchs and LΓ in Beijing (R2 = 0.88. Therefore, it was AFuchs that fundamentally determined the occurrence of NPF events

  13. Aerosol surface area concentration: a governing factor in new particle formation in Beijing

    Science.gov (United States)

    Cai, Runlong; Yang, Dongsen; Fu, Yueyun; Wang, Xing; Li, Xiaoxiao; Ma, Yan; Hao, Jiming; Zheng, Jun; Jiang, Jingkun

    2017-10-01

    The predominating role of aerosol Fuchs surface area, AFuchs, in determining the occurrence of new particle formation (NPF) events in Beijing was elucidated in this study. The analysis was based on a field campaign from 12 March to 6 April 2016 in Beijing, during which aerosol size distributions down to ˜ 1 nm and sulfuric acid concentrations were simultaneously monitored. The 26 days were classified into 11 typical NPF days, 2 undefined days, and 13 non-event days. A dimensionless factor, LΓ, characterized by the relative ratio of the coagulation scavenging rate over the condensational growth rate (Kuang et al., 2010), was applied in this work to reveal the governing factors for NPF events in Beijing. The three parameters determining LΓ are sulfuric acid concentration, the growth enhancement factor characterized by contribution of other gaseous precursors to particle growth, Γ, and AFuchs. Different from other atmospheric environments, such as in Boulder and Hyytiälä, the daily-maximum sulfuric acid concentration and Γ in Beijing varied in a narrow range with geometric standard deviations of 1.40 and 1.31, respectively. A positive correlation between the estimated new particle formation rate, J1.5, and sulfuric acid concentration was found with a mean fitted exponent of 2.4. However, the maximum sulfuric acid concentrations on NPF days were not significantly higher (even lower, sometimes) than those on non-event days, indicating that the abundance of sulfuric acid in Beijing was high enough to initiate nucleation, but may not necessarily lead to NPF events. Instead, AFuchs in Beijing varied greatly among days with a geometric standard deviation of 2.56, whereas the variabilities of AFuchs in Tecamac, Atlanta, and Boulder were reported to be much smaller. In addition, there was a good correlation between AFuchs and LΓ in Beijing (R2 = 0.88). Therefore, it was AFuchs that fundamentally determined the occurrence of NPF events. Among 11 observed NPF events, 10

  14. Possible role of electric forces in bromine activation during polar boundary layer ozone depletion and aerosol formation events

    Science.gov (United States)

    Tkachenko, Ekaterina

    2017-11-01

    This work presents a hypothesis about the mechanism of bromine activation during polar boundary layer ozone depletion events (ODEs) as well as the mechanism of aerosol formation from the frost flowers. The author suggests that ODEs may be initiated by the electric-field gradients created at the sharp tips of ice formations as a result of the combined effect of various environmental conditions. According to the author's estimates, these electric-field gradients may be sufficient for the onset of point or corona discharges followed by generation of high local concentrations of the reactive oxygen species and initiation of free-radical and redox reactions. This process may be responsible for the formation of seed bromine which then undergoes further amplification by HOBr-driven bromine explosion. The proposed hypothesis may explain a variety of environmental conditions and substrates as well as poor reproducibility of ODE initiation observed by researchers in the field. According to the author's estimates, high wind can generate sufficient conditions for overcoming the Rayleigh limit and thus can initiate ;spraying; of charged aerosol nanoparticles. These charged aerosol nanoparticles can provoke formation of free radicals, turning the ODE on. One can also envision a possible emission of halogen ion as a result of the ;electrospray; process analogous to that of electrospray ionization mass-spectrometry.

  15. Seasonal variations of ultra-fine and submicron aerosols in Taipei, Taiwan: implications for particle formation processes in a subtropical urban area

    Directory of Open Access Journals (Sweden)

    H. C. Cheung

    2016-02-01

    , which was characterized by average particle growth and formation rates of 4.0 ± 1.1 nm h−1 and 1.4 ± 0.8 cm−3 s−1, respectively. The prevalence of new particle formation (NPF in summer was suggested as a result of seasonally enhanced photochemical oxidation of SO2 that contributed to the production of H2SO4, and a low level of PM10 (d ≤ 10 µm that served as the condensation sink. Regarding the sources of aerosol particles, correlation analysis of the PNCs against NOx revealed that the local vehicular exhaust was the dominant contributor of the UFPs throughout the year. Conversely, the Asian pollution outbreaks had significant influence in the PNC of accumulation-mode particles during the seasons of winter monsoons. The results of this study implied the significance of secondary organic aerosols in the seasonal variations of UFPs and the influences of continental pollution outbreaks in the downwind areas of Asian outflows.

  16. Resolving detailed molecular structures in complex organic mixtures and modeling their secondary organic aerosol formation

    Science.gov (United States)

    Goodman-Rendall, Kevin A. S.; Zhuang, Yang R.; Amirav, Aviv; Chan, Arthur W. H.

    2016-03-01

    Characterization of unresolved complex mixtures (UCMs) remains an ongoing challenge towards developing detailed and accurate inputs for modeling secondary organic aerosol (SOA) formation. Traditional techniques based on gas chromatography/electron impact-mass spectrometry induce excessive fragmentation, making it difficult to speciate and quantify isomers precisely. The goal of this study is to identify individual organic isomers by gas chromatography/mass spectrometry with supersonic molecular beam (SMB-GC/MS, also known as GC/MS with Cold EI) and to incorporate speciated isomers into an SOA model that accounts for the specific structures elucidated. Two samples containing atmospherically relevant UCMs are analyzed. The relative isomer distributions exhibit remarkably consistent trends across a wide range of carbon numbers. Constitutional isomers of different alkanes are speciated and individually quantified as linear, branched - for the first time by position of branching - multiply branched, or unsaturated - by degree of ring substitution and number of rings. Relative amounts of exact molecular structures are used as input parameters in an SOA box model to study the effects of molecular structures on SOA yields and volatility evolution. Highly substituted cyclic, mono-substituted cyclic, and linear species have the highest SOA yields while branched alkanes formed the least SOA. The rate of functionalization of a representative UCM is found to be in agreement with current volatility basis set (VBS) parameterizations based on detailed knowledge of composition and known oxidation mechanisms, confirming the validity of VBS parameters currently used in air quality models.

  17. Simulating Marine New Particle Formation and Growth Using the M7 Modal Aerosol Dynamics Modal

    Directory of Open Access Journals (Sweden)

    Ciaran Monahan

    2010-01-01

    Full Text Available A modal atmospheric aerosol model (M7 is evaluated in terms of predicting marine new particle formation and growth. Simulations were carried out for three different nucleation schemes involving (1 kinetic self-nucleation of OIO (2 nucleation via OIO activation by H2SO4 and (3 nucleation via OIO activation by H2SO4 plus condensation of a low-volatility organic vapour. Peak OIO and H2SO4 vapour concentrations were both limited to 6×106 molecules cm-3 at noontime while the peak organic vapour concentration was limited to 12×106 molecules cm-3. All simulations produced significant concentrations of new particles in the Aitken mode. From a base case particle concentration of 222 cm-3 at radii >15 nm, increases in concentrations to 366 cm-3 were predicted from the OIO-OIO case, 722 cm-3 for the OIO-H2SO4 case, and 1584 cm-3 for the OIO-H2SO4 case with additional condensing organic vapours. The results indicate that open ocean new particle production is feasible for clean conditions; however, new particle production becomes most significant when an additional condensable organic vapour is available to grow the newly formed particles to larger sizes. Comparison to sectional model for a typical case study demonstrated good agreement and the validity of using the modal model.

  18. Heterogeneous chemistry of glyoxal on acidic solutions. An oligomerization pathway for secondary organic aerosol formation.

    Science.gov (United States)

    Gomez, Mario E; Lin, Yun; Guo, Song; Zhang, Renyi

    2015-05-14

    The heterogeneous chemistry of glyoxal on sulfuric acid surfaces has been investigated at various acid concentrations and temperatures, utilizing a low-pressure fast flow laminar reactor coupled to an ion drift-chemical ionization mass spectrometer (ID-CIMS). The uptake coefficient (γ) of glyoxal ranges from (1.2 ± 0.06) × 10(-2) to (2.5 ± 0.01) × 10(-3) for 60-93 wt % H2SO4 at 253-273 K. The effective Henry's Law constant (H*) ranges from (98.9 ± 4.9) × 10(5) to (1.6 ± 0.1) × 10(5) M atm(-1) for 60-93 wt % at 263-273 K. Both the uptake coefficient and Henry's Law constant increase with decreasing acid concentration and temperature. Our results reveal a reaction mechanism of hydration followed by oligomerization for glyoxal on acidic media, indicating an efficient aqueous reaction of glyoxal on hygroscopic particles leading to secondary organic aerosol formation.

  19. Atmospheric aerosol characterization with the Dutch-Chinese FAST formation flying mission

    NARCIS (Netherlands)

    Gill, E.; Maessen, D.; Laan, E.C.; Kraft, S.; Zheng, G.

    2010-01-01

    Large current uncertainties in the characteristics of aerosols in the Earth's atmosphere preclude meaningful climate model evaluation. The FAST mission will contribute to the characterization of aerosols and their relation to climate change through a synoptic evaluation of local, regional and global

  20. Quantifying dust plume formation and aerosol size distribution during the Saharan Mineral Dust Experiment in North Africa

    KAUST Repository

    Khan, Basit Ali

    2015-01-01

    Dust particles mixed in the free troposphere have longer lifetimes than airborne particles near the surface. Their cumulative radiative impact on earth’s meteorological processes and climate might be significant despite their relatively small contribution to total dust abundance. One example is the elevated dust--laden Saharan Air Layer (SAL) over the equatorial North Atlantic, which cools the sea surface and likely suppresses hurricane activity. To understand the formation mechanisms of SAL, we combine model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM--I), which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. We employed the Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF--Chem) to reproduce the meteorological environment and spatial and size distributions of dust. The experimental domain covers northwest Africa including the southern Sahara, Morocco and part of the Atlantic Ocean with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of most intensive dust outbreaks. Comparisons of model results with available airborne and ground--based observations show that WRF--Chem reproduces observed meteorological fields as well as aerosol distribution across the entire region and along the airplane’s tracks. We evaluated several aerosol uplift processes and found that orographic lifting, aerosol transport through the land/sea interface with steep gradients of meteorological characteristics, and interaction of sea breezes with the continental outflow are key mechanisms that form a surface--detached aerosol plume over the ocean. Comparisons of simulated dust size distributions with airplane and ground--based observations are generally good, but suggest

  1. Secondary organic aerosol formation in biomass-burning plumes: Theoretical analysis of lab studies and ambient plumes

    OpenAIRE

    Bian, Qijing; Jathar, Shantanu H.; Kodros, John K.; Barsanti, Kelley C.; Hatch, Lindsay E.; May, Andrew A.; Kreidenweis, Sonia M.; Pierce, Jeffrey R.

    2016-01-01

    Secondary organic aerosol (SOA) has been shown to form in biomass-burning emissions in laboratory and field studies. However, there is significant variability among studies in mass enhancement, which could be due to differences in fuels, fire conditions, dilution, and/or limitations of laboratory experiments and observations. This study focuses on understanding processes affecting biomass-burning SOA formation in laboratory smog-chamber experiments and in ambient plumes. Vapor wall losses hav...

  2. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

    Directory of Open Access Journals (Sweden)

    E. Asmi

    2010-05-01

    Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

  3. Emission of sunscreen salicylic esters from desert vegetation and their contribution to aerosol formation

    Directory of Open Access Journals (Sweden)

    S. N. Matsunaga

    2008-12-01

    Full Text Available Biogenic volatile organic compounds (BVOC produced by plants are known to have an important role in atmospheric chemistry. However, our knowledge of the range of BVOCs produced by different plant processes is still expanding, and there remain poorly understood categories of BVOCs. In this study, emissions of a novel class of BVOC emissions were investigated in a desert region. Our study considered 8 species of common desert plants: blackbrush (Coleogyne ramosissima, desert willow (Chilopsis linearis, mesquite (Prosopis glandulosa, mondel pine (Pinus eldarica, pinyon pine (Pinus monophylla, cottonwood (Populus deltoides, saguaro cactus (Carnegiea gigantea and yucca (Yucca baccata. The measurements focused on BVOCs with relatively high molecular weight (>C15 and/or an oxygenated functional group. Significantly high emission rates of two salicylic esters were found for blackbrush, desert willow and mesquite with emission rates of 3.1, 1.0 and 4.8μgC dwg−1 h−1, respectively (dwg; dry weight of the leaves in gram. The salicylic esters were identified as 2-ethylhexenyl salicylate (2-EHS and 3,3,5-trimethylcyclohexenyl salicylate (homosalate and are known as effective ultraviolet (UV absorbers. We propose that the plants derive a protective benefit against UV radiation from the salicylic esters and that the emission process is driven by the physical evaporation of the salicylic esters due to the high ambient temperatures. In addition, the salicylic esters are predicted to be an effective precursor of secondary organic aerosol (SOA because they probably produce oxidation products that can condense onto the aerosol phase. We estimated the contribution of the sunscreen esters themselves and their oxidation products on the SOA formation for the Las Vegas area using a BVOC emission model. The contribution was estimated to reach 50% of the biogenic terpenoid

  4. Formation of secondary aerosols from the ozonolysis of styrene: Effect of SO2 and H2O

    Science.gov (United States)

    Díaz-de-Mera, Yolanda; Aranda, Alfonso; Martínez, Ernesto; Rodríguez, Ana Angustias; Rodríguez, Diana; Rodríguez, Ana

    2017-12-01

    In this work we report the study of the ozonolysis of styrene and the reaction conditions leading to the formation of secondary aerosols. The reactions have been carried out in a Teflon chamber filled with synthetic air mixtures at atmospheric pressure and room temperature. We have found that the ozonolysis of styrene in the presence of low concentrations of SO2 readily produces new particles under concentrations of reactants lower than those required in experiments in the absence of SO2. Thus, nucleation events occur at concentrations around (5.6 ± 1.7) × 108molecule cm-3 (errors are 2σ±20%) and SO2 is consumed during the experiments. The reaction of the Criegee intermediates with SO2 to produce SO3 and then H2SO4 may explain (together with OH reactions' contribution) the high capacity of styrene to produce particulate matter in polluted atmospheres. The formation of secondary aerosols in the smog chamber is inhibited under high H2O concentrations. So, the potential formation of secondary aerosols under atmospheric conditions depends on the concentration of SO2 and relative humidity, with a water to SO2 rate constants ratio kH2O/kSO2 = (2.8 ± 0.7) × 10-5 (errors are 2σ±20%).

  5. Secondary organic aerosol formation from photo-oxidation of toluene with NOx and SO2: Chamber simulation with purified air versus urban ambient air as matrix

    National Research Council Canada - National Science Library

    Deng, Wei; Liu, Tengyu; Zhang, Yanli; Situ, Shuping; Hu, Qihou; He, Quanfu; Zhang, Zhou; Lü, Sujun; Bi, Xinhui; Wang, Xuemei; Boreave, Antoinette; George, Christian; Ding, Xiang; Wang, Xinming

    2017-01-01

    Chamber studies on the formation of secondary aerosols are mostly performed with purified air as matrix, it is of wide concern in what extent they might be different from the situations in ambient air...

  6. Secondary organic aerosol formation from the β-pinene+NO3 system: effect of humidity and peroxy radical fate

    Science.gov (United States)

    Boyd, C. M.; Sanchez, J.; Xu, L.; Eugene, A. J.; Nah, T.; Tuet, W. Y.; Guzman, M. I.; Ng, N. L.

    2015-07-01

    The formation of secondary organic aerosol (SOA) from the oxidation of β-pinene via nitrate radicals is investigated in the Georgia Tech Environmental Chamber (GTEC) facility. Aerosol yields are determined for experiments performed under both dry (relative humidity (RH) organic nitrate species (with molecular weights of 215, 229, 231, and 245 amu, which likely correspond to molecular formulas of C10H17NO4, C10H15NO5, C10H17NO5, and C10H15NO6, respectively) are detected by chemical ionization mass spectrometry (CIMS) and their formation mechanisms are proposed. The NO+ (at m/z 30) and NO2+ (at m/z 46) ions contribute about 11 % to the combined organics and nitrate signals in the typical aerosol mass spectrum, with the NO+ : NO2+ ratio ranging from 4.8 to 10.2 in all experiments conducted. The SOA yields in the "RO2 + NO3 dominant" and "RO2 + HO2 dominant" experiments are comparable. For a wide range of organic mass loadings (5.1-216.1 μg m-3), the aerosol mass yield is calculated to be 27.0-104.1 %. Although humidity does not appear to affect SOA yields, there is evidence of particle-phase hydrolysis of organic nitrates, which are estimated to compose 45-74 % of the organic aerosol. The extent of organic nitrate hydrolysis is significantly lower than that observed in previous studies on photooxidation of volatile organic compounds in the presence of NOx. It is estimated that about 90 and 10 % of the organic nitrates formed from the β-pinene+NO3 reaction are primary organic nitrates and tertiary organic nitrates, respectively. While the primary organic nitrates do not appear to hydrolyze, the tertiary organic nitrates undergo hydrolysis with a lifetime of 3-4.5 h. Results from this laboratory chamber study provide the fundamental data to evaluate the contributions of monoterpene + NO3 reaction to ambient organic aerosol measured in the southeastern United States, including the Southern Oxidant and Aerosol Study (SOAS) and the Southeastern Center for Air Pollution

  7. Modelling the formation and composition of secondary organic aerosol from α- and β-pinene ozonolysis using MCM v3

    Directory of Open Access Journals (Sweden)

    M. E. Jenkin

    2004-01-01

    Full Text Available The formation and detailed composition of secondary organic aerosol (SOA from the gas phase ozonolysis of α- and β-pinene has been simulated using the Master Chemical Mechanism version 3 (MCM v3, coupled with a representation of gas-to-aerosol transfer of semivolatile and involatile oxygenated products. A kinetics representation, based on equilibrium absorptive partitioning of ca. 200 semivolatile products, was found to provide an acceptable description of the final mass concentrations observed in a number of reported laboratory and chamber experiments, provided partitioning coefficients were increased by about two orders of magnitude over those defined on the basis of estimated vapour pressures. This adjustment is believed to be due, at least partially, to the effect of condensed phase association reactions of the partitioning products. Even with this adjustment, the simulated initial formation of SOA was delayed relative to that observed, implying the requirement for the formation of species of much lower volatility to initiate SOA formation. The inclusion of a simplified representation of the formation and gas-to-aerosol transfer of involatile dimers of 22 bi- and multifunctional carboxylic acids (in addition to the absorptive partitioning mechanism allowed a much improved description of SOA formation for a wide range of conditions. The simulated SOA composition recreates certain features of the product distributions observed in a number of experimental studies, but implies an important role for multifunctional products containing hydroperoxy groups (i.e. hydroperoxides. This is particularly the case for experiments in which 2-butanol is used to scavenge OH radicals, because [HO2]/[RO2] ratios are elevated in such systems. The optimized mechanism is used to calculate SOA yields from α- and β-pinene ozonolysis in the presence and absence of OH scavengers, and as a function of temperature.

  8. Aqueous-Phase Reactions of Isoprene with Sulfoxy Radical Anions as a way of Wet Aerosol Formation in the Atmosphere

    Science.gov (United States)

    Kuznietsova, I.; Rudzinski, K. J.; Szmigielski, R.; Laboratory of the Environmental Chemistry

    2011-12-01

    Atmospheric aerosols exhibit an important role in the environment. They have implications on human health and life, and - in the larger scale - on climate, the Earth's radiative balance and the cloud's formation. Organic matter makes up a significant fraction of atmospheric aerosols (~35% to ~90%) and may originate from direct emissions (primary organic aerosol, POA) or result from complex physico-chemical processes of volatile organic compounds (secondary organic aerosol, SOA). Isoprene (2-methyl-buta-1,3-diene) is one of the relevant volatile precursor of ambient SOA in the atmosphere. It is the most abundant non-methane hydrocarbon emitted to the atmosphere as a result of living vegetation. According to the recent data, the isoprene emission rate is estimated to be at the level of 500 TgC per year. While heterogeneous transformations of isoprene have been well documented, aqueous-phase reactions of this hydrocarbon with radical species that lead to the production of new class of wet SOA components such as polyols and their sulfate esters (organosulfates), are still poorly recognized. The chain reactions of isoprene with sulfoxy radical-anions (SRA) are one of the recently researched route leading to the formation of organosulfates in the aqueous phase. The letter radical species originate from the auto-oxidation of sulfur dioxide in the aqueous phase and are behind the phenomenon of atmospheric acid rain formation. This is a complicated chain reaction that is catalyzed by transition metal ions, such as manganese(II), iron(III) and propagated by sulfoxy radical anions . The presented work addresses the chemical interaction of isoprene with sulfoxy radical-anions in the water solution in the presence of nitrite ions and nitrous acid, which are important trace components of the atmosphere. We showed that nitrite ions and nitrous acid significantly altered the kinetics of the auto-oxidation of SO2 in the presence of isoprene at different solution acidity from 2 to 8

  9. SAFARI 2000 MODIS MOD04_L2 Aerosol Data, GRANT Format, for Southern Africa

    Data.gov (United States)

    National Aeronautics and Space Administration — The subset of the MODIS MOD04_L2 aerosol product provided in this data set represents the swaths that coincide with known times of the South African Weather...

  10. SAFARI 2000 MODIS MOD04_L2 Aerosol Data, GRANT Format, for Southern Africa

    Data.gov (United States)

    National Aeronautics and Space Administration — ABSTRACT: The subset of the MODIS MOD04_L2 aerosol product provided in this data set represents the swaths that coincide with known times of the South African...

  11. The kinetics of aerosol particle formation and removal in NPP severe accidents

    Science.gov (United States)

    Zatevakhin, Mikhail A.; Arefiev, Valentin K.; Semashko, Sergey E.; Dolganov, Rostislav A.

    2016-06-01

    Severe Nuclear Power Plant (NPP) accidents are accompanied by release of a massive amount of energy, radioactive products and hydrogen into the atmosphere of the NPP containment. A valid estimation of consequences of such accidents can only be carried out through the use of the integrated codes comprising a description of the basic processes which determine the consequences. A brief description of a coupled aerosol and thermal-hydraulic code to be used for the calculation of the aerosol kinetics within the NPP containment in case of a severe accident is given. The code comprises a KIN aerosol unit integrated into the KUPOL-M thermal-hydraulic code. Some features of aerosol behavior in severe NPP accidents are briefly described.

  12. Formation and evolution of aerosols in filtered air and in natural air. Effect of radioactivity; Formation et evolution des aerosols dans l'air filtre et dans l'air naturel action de la radioactivite

    Energy Technology Data Exchange (ETDEWEB)

    Madelaine, G.J. [Commissariat a l' Energie Atomique, 92 - Fontenay-aux-Roses (France). Centre d' Etudes Nucleaires

    1968-06-01

    Results are presented concerning the formation, the evolution, the coagulation and the electrical charge of aerosols which form in natural filtered air containing only gaseous impurities, under the influence of solar light (photolysis) and of radioactive disintegrations (radiolysis). The modifications brought about in the aerosol by an increase in the sulphur dioxide content and in the natural radioactive gas content are studied. The work is then repeated with non-filtered natural atmospheric air. A comparison is also made of the behaviour of non-radioactive and radioactive particles (active thoron deposit). In conclusion, the possible consequences of these phenomena on the origin and the size distribution of particles occurring in the atmosphere is considered. (author) [French] On expose les resultats obtenus sur la formation, l'evolution, la coagulation et la charge electrique des aerosols qui se forment dans l'air naturel filtre, ne contenant que des impuretes gazeuses, sous l'influence de la lumiere solaire (photolyse) et des desintegrations radioactives (radiolyse). On examine les modifications apportees a l'aerosol forme par l'augmentation de la teneur de l'air en anhydride sulfureux et en gaz radioactif naturel. Cette etude est ensuite reprise mais avec de l'air naturel atmospherique non filtre. On compare egalement le comportement des particules non radioactives et radioactives (depot actif du thoron). En conclusion, on examine les consequences que peuvent avoir ces phenomenes sur l'origine et la granulometrie des particules contenues dans l'atmosphere. (auteur)

  13. Transformation of logwood combustion emissions in a smog chamber: formation of secondary organic aerosol and changes in the primary organic aerosol upon daytime and nighttime aging

    Science.gov (United States)

    Tiitta, Petri; Leskinen, Ari; Hao, Liqing; Yli-Pirilä, Pasi; Kortelainen, Miika; Grigonyte, Julija; Tissari, Jarkko; Lamberg, Heikki; Hartikainen, Anni; Kuuspalo, Kari; Kortelainen, Aki-Matti; Virtanen, Annele; Lehtinen, Kari E. J.; Komppula, Mika; Pieber, Simone; Prévôt, André S. H.; Onasch, Timothy B.; Worsnop, Douglas R.; Czech, Hendryk; Zimmermann, Ralf; Jokiniemi, Jorma; Sippula, Olli

    2016-10-01

    Organic aerosols (OA) derived from small-scale wood combustion emissions are not well represented by current emissions inventories and models, although they contribute substantially to the atmospheric particulate matter (PM) levels. In this work, a 29 m3 smog chamber in the ILMARI facility of the University of Eastern Finland was utilized to investigate the formation of secondary organic aerosol (SOA) from a small-scale modern masonry heater commonly used in northern Europe. Emissions were oxidatively aged in the smog chamber for a variety of dark (i.e., O3 and NO3) and UV (i.e., OH) conditions, with OH concentration levels of (0.5-5) × 106 molecules cm-3, achieving equivalent atmospheric aging of up to 18 h. An aerosol mass spectrometer characterized the direct OA emissions and the SOA formed from the combustion of three wood species (birch, beech and spruce) using two ignition processes (fast ignition with a VOC-to-NOx ratio of 3 and slow ignition with a ratio of 5).Dark and UV aging increased the SOA mass fraction with average SOA productions 2.0 times the initial OA mass loadings. SOA enhancement was found to be higher for the slow ignition compared with fast ignition conditions. Positive matrix factorization (PMF) was used to separate SOA, primary organic aerosol (POA) and their subgroups from the total OA mass spectra. PMF analysis identified two POA and three SOA factors that correlated with the three major oxidizers: ozone, the nitrate radical and the OH radical. Organonitrates (ONs) were observed to be emitted directly from the wood combustion and additionally formed during oxidation via NO3 radicals (dark aging), suggesting small-scale wood combustion may be a significant ON source. POA was oxidized after the ozone addition, forming aged POA, and after 7 h of aging more than 75 % of the original POA was transformed. This process may involve evaporation and homogeneous gas-phase oxidation as well as heterogeneous oxidation of particulate organic matter

  14. Aerosol impacts on radiative and microphysical properties of clouds and precipitation formation

    Science.gov (United States)

    Alizadeh-Choobari, O.; Gharaylou, M.

    2017-03-01

    Through modifying the number concentration and size of cloud droplets, aerosols have intricate impacts on radiative and microphysical properties of clouds, which together influence precipitation processes. Aerosol-cloud interactions for a mid-latitude convective cloud system are investigated using a two-moment aerosol-aware bulk microphysical scheme implemented into the Weather Research and Forecasting (WRF) model. Three sensitivity experiments with initial identical dynamic and thermodynamic conditions, but different cloud-nucleating aerosol concentrations were conducted. Increased aerosol number concentration has resulted in more numerous cloud droplets of overall smaller sizes, through which the optical properties of clouds have been changed. While the shortwave cloud forcing is significantly increased in more polluted experiments, changes in the aerosol number concentration have negligible impacts on the longwave cloud forcing. For the first time, it is found that polluted clouds have higher cloud base heights, the feature that is caused by more surface cooling due to a higher shortwave cloud forcing, as well as a drier boundary layer in the polluted experiment compared to the clean. The polluted experiment was also associated with a higher liquid water content (LWC), caused by an increase in the number of condensation of water vapor due to higher concentration of hygroscopic aerosols acting as condensation nuclei. The domain-averaged accumulated precipitation is little changed under both polluted and clean atmosphere. Nevertheless, changes in the rate of precipitation are identified, such that under polluted atmosphere light rain is reduced, while both moderate and heavy rain are intensified, confirming the fact that if an ample influx of water vapor exists, an increment of hygroscopic aerosols can increase the amount of precipitation.

  15. Time-resolved analysis of primary volatile emissions and secondary aerosol formation potential from a small-scale pellet boiler

    Science.gov (United States)

    Czech, Hendryk; Pieber, Simone M.; Tiitta, Petri; Sippula, Olli; Kortelainen, Miika; Lamberg, Heikki; Grigonyte, Julija; Streibel, Thorsten; Prévôt, André S. H.; Jokiniemi, Jorma; Zimmermann, Ralf

    2017-06-01

    Small-scale pellet boilers and stoves became popular as a wood combustion appliance for domestic heating in Europe, North America and Asia due to economic and environmental aspects. Therefore, an increasing contribution of pellet boilers to air pollution is expected despite their general high combustion efficiency. As emissions of primary organic aerosol (POA) and permanent gases of pellet boilers are well investigated, the scope of this study was to investigate the volatile organic emissions and the formation potential of secondary aerosols for this type of appliance. Fresh and aged emissions were analysed by a soot-particle aerosol time-of-flight mass spectrometry (SP-AMS) and the molecular composition of the volatile precursors with single-photon ionisation time-of-flight mass spectrometry (SPI-TOFMS) at different pellet boiler operation conditions. Organic emissions in the gas phase were dominated by unsaturated hydrocarbons while wood-specific VOCs, e.g. phenolic species or substituted furans, were only detected during the starting phase. Furthermore, organic emissions in the gas phase were found to correlate with fuel grade and combustion technology in terms of secondary air supply. Secondary organic aerosols of optimised pellet boiler conditions (OPT, state-of-the-art combustion appliance) and reduced secondary air supply (RSA, used as a proxy for pellet boilers of older type) were studied by simulating atmospheric ageing in a Potential Aerosol Mass (PAM) flow reactor. Different increases in OA mass (55% for OPT, 102% for RSA), associated with higher average carbon oxidation state and O:C, could be observed in a PAM chamber experiment. Finally, it was found that derived SOA yields and emission factors were distinctly lower than reported for log wood stoves.

  16. Laboratory Experiments and Modeling for Interpreting Field Studies of Secondary Organic Aerosol Formation Using an Oxidation Flow Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Jimenez, Jose-Luis [Univ. of Colorado, Boulder, CO (United States)

    2016-02-01

    This grant was originally funded for deployment of a suite of aerosol instrumentation by our group in collaboration with other research groups and DOE/ARM to the Ganges Valley in India (GVAX) to study aerosols sources and processing. Much of the first year of this grant was focused on preparations for GVAX. That campaign was cancelled due to political reasons and with the consultation with our program manager, the research of this grant was refocused to study the applications of oxidation flow reactors (OFRs) for investigating secondary organic aerosol (SOA) formation and organic aerosol (OA) processing in the field and laboratory through a series of laboratory and modeling studies. We developed a gas-phase photochemical model of an OFR which was used to 1) explore the sensitivities of key output variables (e.g., OH exposure, O3, HO2/OH) to controlling factors (e.g., water vapor, external reactivity, UV irradiation), 2) develop simplified OH exposure estimation equations, 3) investigate under what conditions non-OH chemistry may be important, and 4) help guide design of future experiments to avoid conditions with undesired chemistry for a wide range of conditions applicable to the ambient, laboratory, and source studies. Uncertainties in the model were quantified and modeled OH exposure was compared to tracer decay measurements of OH exposure in the lab and field. Laboratory studies using OFRs were conducted to explore aerosol yields and composition from anthropogenic and biogenic VOC as well as crude oil evaporates. Various aspects of the modeling and laboratory results and tools were applied to interpretation of ambient and source measurements using OFR. Additionally, novel measurement methods were used to study gas/particle partitioning. The research conducted was highly successful and details of the key results are summarized in this report through narrative text, figures, and a complete list of publications acknowledging this grant.

  17. Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

    Science.gov (United States)

    Roldin, P.; Eriksson, A. C.; Nordin, E. Z.; Hermansson, E.; Mogensen, D.; Rusanen, A.; Boy, M.; Swietlicki, E.; Svenningsson, B.; Zelenyuk, A.; Pagels, J.

    2014-08-01

    We have developed the novel Aerosol Dynamics, gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas-phase Master Chemical Mechanism version 3.2 (MCMv3.2), an aerosol dynamics and particle-phase chemistry module (which considers acid-catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion-limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study (1) the evaporation of liquid dioctyl phthalate (DOP) particles, (2) the slow and almost particle-size-independent evaporation of α-pinene ozonolysis secondary organic aerosol (SOA) particles, (3) the mass-transfer-limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), and (4) the influence of chamber wall effects on the observed SOA formation in smog chambers. ADCHAM is able to capture the observed α-pinene SOA mass increase in the presence of NH3(g). Organic salts of ammonium and carboxylic acids predominantly form during the early stage of SOA formation. In the smog chamber experiments, these salts contribute substantially to the initial growth of the homogeneously nucleated particles. The model simulations of evaporating α-pinene SOA particles support the recent experimental findings that these particles have a semi-solid tar-like amorphous-phase state. ADCHAM is able to reproduce the main features of the observed slow evaporation rates if the concentration of low-volatility and viscous oligomerized SOA material at the particle surface increases upon evaporation. The evaporation rate is mainly governed by the reversible decomposition of oligomers back to monomers. Finally, we demonstrate that the mass-transfer-limited uptake of condensable organic compounds

  18. Laboratory Simulation of Haze/Aerosol formation in warm and hot Jupiters

    Science.gov (United States)

    Gharib-Nezhad, Ehsan; Lyons, James R.; Wright, David P.

    2016-10-01

    During the transit of an exoplanet across its host star, transmitted starlight through exoplanet atmosphere is absorbed and scattered, and the recorded transit spectra reveal important chemical information. There are many detected exoplanets in which hazes/aerosols obscure the incident photons, and consequently, fewer photons are transmitted through the atmosphere, contributing to a flat/nearly flat transit spectrum. Here, we have carried out two complementary approaches to address haze formation. First, laboratory simulations of haze condensation in exoplanet atmospheres are carried out using an electric discharge tube. A mixture of likely gas species (i.e. H2, He, H2O, CH4, N2 and H2S) is inserted into a glass manifold on a vacuum line, at a pressure ~100-10 mbar, and depending on the exoplanet category (e.g., warm or hot Jupiters), the temperature is set. Applying a few kilovolts produces plasma in the discharge tube, and as a result, particles are formed. We use spectroscopic ellipsometry to measure the optical constants (complex refractive index) of the collected laboratory hazes. Then, chemical characterization is made using RBS (Rutherford Backscattering Spectroscopy) and XPS (X-ray Photoelectron Spectroscopy). Second, we developed a transit modeling code by which the transit spectra are generated using observational and laboratory data as an input. The model accounts for Mie scattering from haze particles in the vis-NIR spectral region, and Rayleigh scattering which comes from gases and particles (effective in UV-vis). The measured refractive indexes (real and imaginary part) describe the absorption and scattering in the vis-NIR transmission region, and, by generating transit spectra close to the observed ones from exoplanets, constraints on atmospheric chemical characterization can be revealed. Our laboratory results show that haze particles formed in the presence of water and with the solar C/O ratio = 0.5. The other outcome of our experiment is that

  19. Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

    Directory of Open Access Journals (Sweden)

    D. V. Spracklen

    2010-05-01

    Full Text Available We synthesised observations of total particle number (CN concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT and 1000–10 000 cm−3 in the continental boundary layer (BL. Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46 but fail to explain the observed seasonal cycle (R2=0.1. The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88% unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%. Simulated CN concentrations in the continental BL were also biased low (NMB=−74% unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one or kinetic-type mechanism (J proportional to sulfuric acid to the power two with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3 than by increasing the number emission from primary anthropogenic sources (R2=0.18. The nucleation constants that resulted in best overall match between model and observed CN concentrations were

  20. Secondary organic aerosol formation from propylene irradiations in a chamber study

    Science.gov (United States)

    Ge, Shuangshuang; Xu, Yongfu; Jia, Long

    2017-05-01

    Some studies have shown that low-molecular-weight VOCs such as ethylene and acetylene can form SOA. However, so far propylene (C3H6) has not been studied. The current work systematically investigates irradiations of propylene in the presence of NOx (x = 1, 2) in a self-made indoor chamber. Only a small amount of secondary organic aerosols (SOA) was formed under 5% and 80% RH conditions without sodium chloride (NaCl) seed particles or in the presence of solid NaCl. When NaCl was in the form of droplets, liquid water content (LWC) increased from 34.5 to 169.8 μg m-3 under different initial NaCl concentrations, and correspondingly the amount of SOA linearly increased from 5.9 to 29.8 μg m-3 (SOA = 0.0164 × LWC+1.137, R2 = 0.97) at the C3H6/NOx ratio of 32.2-44.9 (ppbC/ppb). The initial C3H6/NOx concentration ratio considerably impacted the formation of SOA, in which the amount of SOA increased from 12.1 to 47.9 μg m-3 exponentially as the ratio decreased from 46.5 to 6.3 with an important point of the ratio value of 11. At the ratio of less than 11 in the regime under the control of C3H6, SOA concentrations decreased considerably with increasing ratio, whereas at the ratio value of larger than 11 in the NOx controlled regime, SOA slightly decreased with increasing ratio. From combination of the analysis of different functional groups of particles by IR spectra and ESI-Exactive-Orbitrap mass spectrometer, the constituents of SOA were identified to be hydroperoxides (e.g. HOCH2CCl(CH3)OOH), esters (e.g. CH2ClC(O)OCHClCHO), organic nitrates (e.g. HO2CH(CH2Cl)C(O)OCCl(CH2Cl)C(O)OCHClCH2ONO2), etc. Furthermore, a liquid-phase mechanism of SOA formation has been proposed in this study.

  1. Simulating the formation of carbonaceous aerosol in a European Megacity (Paris during the MEGAPOLI summer and winter campaigns

    Directory of Open Access Journals (Sweden)

    C. Fountoukis

    2016-03-01

    Full Text Available We use a three-dimensional regional chemical transport model (PMCAMx with high grid resolution and high-resolution emissions (4 × 4 km2 over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009 and a winter (January/February 2010 period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 % of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA concentrations is also encouraging (mean bias = 0.1 µg m−3 during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m−3 mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d−1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00–14:00 LT and 20 % during dinner time (20:00–22:00 LT. Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias =  −2.3 µg m−3 pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.

  2. Insights into the molecular level composition, sources, and formation mechanisms of dissolved organic matter in aerosols and precipitation

    Science.gov (United States)

    Altieri, Katye Elisabeth

    Atmospheric aerosols scatter and absorb light influencing the global radiation budget and climate, and are associated with adverse effects on human health. Precipitation is an important removal mechanism for atmospheric dissolved organic matter (DOM), and a potentially important input for receiving ecosystems. However, the sources, formation, and composition of atmospheric DOM in aerosols and precipitation are not well understood. This dissertation investigates the composition and formation mechanisms of secondary organic aerosol (SOA) formed through cloud processing reactions, elucidates the composition and sources of DOM in rainwater, and provides links connecting the two. Photochemical batch aqueous-phase reactions of organics with both biogenic and anthropogenic sources (i.e., methylglyoxal, pyruvic acid) and OH radical were performed to simulate cloud processing. The composition of products formed through cloud processing experiments and rainwater collected in New Jersey, USA was investigated using a combination of electrospray ionization mass spectrometry techniques, including ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry. This dissertation has resulted in the first evidence that oligomers form through cloud processing reactions, the first detailed chemical mechanism of aqueous phase oligomerization, the first identification of oligomers, organosulfates, and nitrooxy organosulfates in precipitation, and the first molecular level chemical characterization of organic nitrogen in precipitation. The formation of oligomers in SOA helps to explain the presence of large multifunctional compounds and humic like substances (HULIS) that dominate particulate organic mass. Oligomers have low vapor pressures and remain in the particle phase after cloud evaporation, enhancing SOA. The chemical properties of the oligomers suggest that they are less hygroscopic than the monomeric reaction products (i.e., organic acids). Their elemental

  3. Aerosol characterization during project POLINAT

    Energy Technology Data Exchange (ETDEWEB)

    Hagen, D.E.; Hopkins, A.R.; Paladino, J.D.; Whitefield, P.D. [Missouri Univ., Rolla, MO (United States). Cloud and Aerosol Sciences Lab.; Lilenfeld, H.V. [McDonnell Douglas Aerospace-East, St. Louis, MO (United States)

    1997-12-31

    The objectives of the aerosol/particulate characterization measurements of project POLINAT (POLlution from aircraft emissions In the North ATlantic flight corridor) are: to search for aerosol/particulate signatures of air traffic emissions in the region of the North Atlantic Flight Corridor; to search for the aerosol/particulate component of large scale enhancement (`corridor effects`) of air traffic related species in the North Atlantic region; to determine the effective emission indices for the aerosol/particulate component of engine exhaust in both the near and far field of aircraft exhaust plumes; to measure the dispersion and transformation of the aerosol/particulate component of aircraft emissions as a function of ambient condition; to characterize background levels of aerosol/particulate concentrations in the North Atlantic Region; and to determine effective emission indices for engine exhaust particulates for regimes beyond the jet phase of plume expansion. (author) 10 refs.

  4. In-situ studies on volatile jet exhaust particle emissions - impacts of fuel sulfur content and environmental conditions on nuclei-mode aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Schroeder, F.; Baumann, R.; Petzold, A.; Busen, R.; Schulte, P.; Fiebig, M. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Brock, C.A. [Denver Univ., CO (United States). Dept. of Engineering

    2000-02-01

    In-situ measurements of ultrafine aerosol particle emissions were performed at cruise altitudes behind the DLR ATTAS research jet (RR M45H M501 engines) and a B737-300 aircraft (CFM56-3B1 engines). Measurements were made 0.15-20 seconds after emission as the source aircraft burned fuel with sulfur contents (FSC) of 2.6, 56 or 118 mg kg{sup -1}. Particle size distributions of from 3 to 60 nm diameter were determined using CN-counters with varying lower size detection limits. Volatile particle concentrations in the aircraft plumes strongly increased as diameter decreased toward the sizes of large molecular clusters, illustrating that apparent particle emissions are extremely sensitive to the smallest particle size detectable by the instrument used. Environmental conditions and plume age alone could influence the number of detected ultrafine (volatile) aerosols within an order of magnitude, as well. The observed volatile particle emissions decreased nonlinearly as FSC decreased to 60 mg kg{sup -1}, reaching minimum values of about 2 x 10{sup 17} kg{sup -1} and 2 x 10{sup 16} kg{sup -1} for particles >3 nm and >5 nm, respectively. Volatile particle emissions did not change significantly as FSCs were further reduced below 60 mg kg{sup -1}. Volatile particle emissions did not differ significantly between the two studied engine types. In contrast, soot particle emissions from the modern CFM56-3B1 engines were 4-5 times less (4 x 10{sup 14} kg{sup -1}) than from the older RR M45H M501 engines (1.8 x 10{sup 15} kg{sup -1}). Contrail processing has been identified as an efficient sink/quenching parameter for ultrafine particles and reduces the remaining interstitial aerosol by factors 2-10 depending on particle size.

  5. Quantification of Release of Critical Elements, Formation of Fly Ash and Aerosols: Status on Current Understanding and Research Needs

    DEFF Research Database (Denmark)

    Jappe Frandsen, Flemming

    2017-01-01

    ) shedding of deposits. Some of the steps may be repetitive, as the process is partly cyclic [Frandsen, 2011]. The inorganic fraction of solid fuels, may cause several problems during combustion, most importantly formation of particulate matter (aerosols and fly ashes). These may subsequently induce deposit...... of combustion units.Through several years, high quality research has been conducted on characterization of fuels, ashes and deposit formation in utility boilers fired with coal, biomass and waste fractions. Huge amounts of experimental data have been reported, from such work, but the fact...... is that there are still in 2017, a number of big gaps in our current understanding of these phenomena, and that we need focus on these points, in order to be able to describe, understand, and, quantify the processes of ash and deposit formation completely [Frandsen, 2009].This paper provide a brief outline of the current...

  6. Dust plume formation in the free troposphere and aerosol size distribution during the Saharan Mineral Dust Experiment in North Africa

    KAUST Repository

    Khan, Basit Ali

    2015-11-27

    Dust particles mixed in the free troposphere have longer lifetimes than airborne particles near the surface. Their cumulative radiative impact on earth’s meteorological processes and climate might be significant despite their relatively small contribution to total dust abundance. One example is the elevated dust-laden Saharan Air Layer (SAL) over the tropical and subtropical North Atlantic, which cools the sea surface. To understand the formation mechanisms of a dust layer in the free troposphere, this study combines model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM-I), which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. The Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF-Chem) is employed to reproduce the meteorological environment and spatial and size distributions of dust. The model domain covers northwest Africa and adjacent water with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of the most intensive dust outbreaks. Comparisons of model results with available airborne and ground-based observations show that WRF-Chem reproduces observed meteorological fields as well as aerosol distribution across the entire region and along the airplane’s tracks. Several mechanisms that cause aerosol entrainment into the free troposphere are evaluated and it is found that orographic lifting, and interaction of sea breeze with the continental outflow are key mechanisms that form a surface-detached aerosol plume over the ocean. The model dust emission scheme is tuned to simultaneously fit the observed total optical depth and the ratio of aerosol optical depths generated by fine and coarse dust modes. Comparisons of simulated dust size distributions with

  7. Dust plume formation in the free troposphere and aerosol size distribution during the Saharan Mineral Dust Experiment in North Africa

    Directory of Open Access Journals (Sweden)

    Basit Khan

    2015-11-01

    Full Text Available Dust particles mixed in the free troposphere have longer lifetimes than airborne particles near the surface. Their cumulative radiative impact on earth's meteorological processes and climate might be significant despite their relatively small contribution to total dust abundance. One example is the elevated dust-laden Saharan Air Layer (SAL over the tropical and subtropical North Atlantic, which cools the sea surface. To understand the formation mechanisms of a dust layer in the free troposphere, this study combines model simulations and dust observations collected during the first stage of the Saharan Mineral Dust Experiment (SAMUM-I, which sampled dust events that extended from Morocco to Portugal, and investigated the spatial distribution and the microphysical, optical, chemical, and radiative properties of Saharan mineral dust. The Weather Research Forecast model coupled with the Chemistry/Aerosol module (WRF-Chem is employed to reproduce the meteorological environment and spatial and size distributions of dust. The model domain covers northwest Africa and adjacent water with 5 km horizontal grid spacing and 51 vertical layers. The experiments were run from 20 May to 9 June 2006, covering the period of the most intensive dust outbreaks. Comparisons of model results with available airborne and ground-based observations show that WRF-Chem reproduces observed meteorological fields as well as aerosol distribution across the entire region and along the airplane's tracks. Several mechanisms that cause aerosol entrainment into the free troposphere are evaluated and it is found that orographic lifting, and interaction of sea breeze with the continental outflow are key mechanisms that form a surface-detached aerosol plume over the ocean. The model dust emission scheme is tuned to simultaneously fit the observed total optical depth and the ratio of aerosol optical depths generated by fine and coarse dust modes. Comparisons of simulated dust size

  8. Observation of aerosol number size distribution and new particle formation at a mountainous site in Southeast China.

    Science.gov (United States)

    Zhang, Xiaoru; Yin, Yan; Lin, Zhenyi; Han, Yongxiang; Hao, Jian; Yuan, Liang; Chen, Kui; Chen, Jinghua; Kong, Shaofei; Shan, Yunpeng; Xiao, Hui; Tan, Wen

    2017-01-01

    To quantify the physical/chemical properties, and the formation and growth processes of aerosol particles on mountainous regions in Southeast China, an intensive field campaign was conducted from April to July 2008 on the top of Mt. Huang (1840m above mean sea level). The average particle number concentration was 2.35×103cm-3, and the ultrafine particles (particle number concentration. Excluding the accumulation mode particles, the average daytime particle number concentrations were prominently higher than those measured at nighttime, suggesting there was a diurnal pattern of changes between planetary boundary layer and free troposphere air. The aerosol spectra were classified into two categories: the first category (FCS) exhibited a clear diurnal cycle, with relatively higher number concentration (3.19×103cm-3), smaller sizes and air masses from the inland; the second category (SCS) presented less obvious diurnal cycle, with lower number concentration (1.88×103cm-3), larger sizes and air masses from coastal regions. Air mass sources, weather conditions, and new particle formation (NPF) events were responsible for the differences of these two particle spectra. Six NPF events were identified, which usually began at 10:00-11:00 LT, with the estimated formation rate J10 in the range of 0.09-0.30cm-3s-1 and the growth rate at 1.42-4.53nmh-1. Wind speed, sulfur dioxide and ozone concentrations were higher on NPF days than those on non-NPF days, whereas temperature, relative humidity, concentrations of nitrogen oxide and carbonic oxide were lower on NPF days. Sulfur dioxide and ozone might be main potentially precursor gases for those NPF events. The NPF events at Mt. Huang corresponded closely to a southwest winds. These results are useful for improving our understanding of the main factors controlling the variation of aerosol size distribution and NPF events in this region. Copyright © 2016 Elsevier B.V. All rights reserved.

  9. Implications of ammonia emissions for fine aerosol formation and visibility impairment. A case study from the Lower Fraser Valley, British Columbia

    DEFF Research Database (Denmark)

    Barthelmie, R.J.; Pryor, S.C.

    1998-01-01

    of nitrogen and sulphur oxides over agricultural areas in the eastern and central valley with higher ammonia emissions favours subsequent ammonium nitrate and sulphate formation. This leads to higher fine mass concentrations and lowest visibility in the predominantly agricultural regions of the valley. (C......Ammonia enhances atmospheric aerosol formation and, once in the aerosol form, enhances the light extinction characteristics of those aerosols. In this paper, an ammonia emissions inventory is developed for the Lower Fraser Valley (LFV) of British Columbia and used in conjunction with ambient...... ammonia and ammonium measurements to explain: (i) the observed temporal and spatial variability of fine inorganic aerosol composition and concentrations in the valley, and (ii) the severity and spatial variability of visibility degradation in the LFV. It is proposed here that advection of urban emissions...

  10. Simulating ultrafine particle formation in Europe using a regional CTM: contribution of primary emissions versus secondary formation to aerosol number concentrations

    Directory of Open Access Journals (Sweden)

    C. Fountoukis

    2012-09-01

    Full Text Available A three-dimensional regional chemical transport model (CTM with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10 within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.

  11. Application of the characteristics-based sectional method to spatially varying aerosol formation and transport

    NARCIS (Netherlands)

    Frederix, E.M.A.; Kuczaj, Arkadiusz K.; Nordlund, M.; Veldman, A.E.P.; Geurts, Bernardus J.

    The characteristics-based ssolution. It is easy to verify thatectional method (CBSM) offers an Eulerian description of an internally mixed aerosol. It was shown to be robust and capable of exact preservation of lower order moments, allowing for highly skewed sectional droplet size distributions. In

  12. Characterization of Halyomorpha halys (brown marmorated stink bug) biogenic volatile organic compound emissions and their role in secondary organic aerosol formation.

    Science.gov (United States)

    Solomon, Danielle; Dutcher, Dabrina; Raymond, Timothy

    2013-11-01

    The formation of aerosols is a key component in understanding cloud formation in the context of radiative forcings and global climate modeling. Biogenic volatile organic compounds (BVOCs) are a significant source of aerosols, yet there is still much to be learned about their structures, sources, and interactions. The aims of this project were to identify the BVOCs found in the defense chemicals of the brown marmorated stink bug Halymorpha halys and quantify them using gas chromatography-mass spectrometry (GC/MS) and test whether oxidation of these compounds by ozone-promoted aerosol and cloud seed formation. The bugs were tested under two conditions: agitation by asphyxiation and direct glandular exposure. Tridecane, 2(5H)-furanone 5-ethyl, and (E)-2-decenal were identified as the three most abundant compounds. H. halys were also tested in the agitated condition in a smog chamber. It was found that in the presence of 100-180 ppm ozone, secondary aerosols do form. A scanning mobility particle sizer (SMPS) and a cloud condensation nuclei counter (CCNC) were used to characterize the secondary aerosols that formed. This reaction resulted in 0.23 microg/ bug of particulate mass. It was also found that these secondary organic aerosol particles could act as cloud condensation nuclei. At a supersaturation of 1%, we found a kappa value of 0.09. Once regional populations of these stink bugs stablilize and the populations estimates can be made, the additional impacts of their contribution to regional air quality can be calculated.

  13. Modeling organic aerosols in a megacity: potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

    Energy Technology Data Exchange (ETDEWEB)

    Hodzic, Alma; Jimenez, Jose L.; Madronich, Sasha; Canagaratna, M. R.; DeCarlo, Peter F.; Kleinman, Lawrence I.; Fast, Jerome D.

    2010-06-21

    It has been established that observed local and regional levels of secondary organic aerosols (SOA) in polluted areas cannot be explained by the oxidation and partitioning of traditional anthropogenic and biogenic VOC precursors. In this study, the 3D regional air quality model CHIMERE is applied to quantify the contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic vapors (S/IVOC) in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to explicitly include the volatility distribution of primary organic aerosols (POA), their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007) ("ROB") and Grieshop et al. (2009) ("GRI") are compared and evaluated against surface and aircraft measurements. For the first time, 3D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS) data, but also against and oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (3-6 times) with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009), both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. The predicted anthropogenic POA levels are found to agree within 20% with the observed HOA concentrations for both the ROB and GRI simulations, consistent with the interpretation of the emissions inventory by previous studies. The impact of biomass burning POA within the city is underestimated in comparison to the AMS BBOA, presumably due to insufficient nighttime smoldering emissions. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The production from anthropogenic and biomass burning

  14. A secondary organic aerosol formation model considering successive oxidation aging and kinetic condensation of organic compounds: global scale implications

    Directory of Open Access Journals (Sweden)

    F. Yu

    2011-02-01

    Full Text Available The widely used two-product secondary organic aerosol (SOA formation model has been extended in this study to consider the volatility changes of secondary organic gases (SOG arising from the aging process as well as the kinetic condensation of low volatile SOG (LV-SOG. In addition to semi-volatile SOG (SV-SOG with saturation vapor pressure at 290 K (C*290 in the range of ~3 ppt–3 ppb and medium-volatile SOG (MV-SOG with C*290 in the range of ~0.3–300 ppb, we add a third component representing LV-SOG with C*290 below ~3 ppt and design a scheme to transfer MV-SOG to SV-SOG and SV-SOG to LV-SOG associated with oxidation aging. This extended SOA formation model has been implemented in a global aerosol model (GEOS-Chem and the co-condensation of H2SO4 and LV-SOG on pre-existing particles is explicitly simulated. We show that, over many parts of the continents, LV-SOG concentrations are generally a factor of ~2–20 higher than those of H2SO4 and the kinetic condensation of LV-SOG significantly enhances particle growth rates. Comparisons of the simulated and observed evolution of particle size distributions at a boreal forest site (Hyytiälä, Finland clearly show that LV-SOG condensation is critical in order to bring the simulations closer to the observations. With the new SOA formation scheme, annual mean SOA mass increases by a factor of 2–10 in many parts of the boundary layer and reaches above 0.5 μg m−3 in most parts of the main continents, improving the agreement with aerosol mass spectrometer (AMS SOA measurements. While the new scheme generally decreases the concentration of condensation nuclei larger than 10 nm by 3–30% in the lower boundary layer as a result of enhanced surface area and reduced nucleation rates, it substantially increases the concentration of cloud condensation nuclei at a

  15. Secondary Organic Aerosol Formation and Aging in a Flow Reactor in the Forested Southeast US during SOAS

    Science.gov (United States)

    Hu, W.; Palm, B. B.; Hacker, L.; Campuzano Jost, P.; Day, D. A.; de Sá, S. S.; Ayres, B. R.; Draper, D.; Fry, J.; Ortega, A. M.; Kiendler-Scharr, A.; Pajunoja, A.; Virtanen, A.; Krechmer, J.; Canagaratna, M. R.; Thompson, S.; Yatavelli, R. L. N.; Stark, H.; Worsnop, D. R.; Martin, S. T.; Farmer, D.; Brown, S. S.; Jimenez, J. L.

    2015-12-01

    A major field campaign (Southern Oxidant and Aerosol Study, SOAS) was conducted in summer 2013 in a forested area in Centreville Supersite, AL (SEARCH network) in the southeast U.S. To investigate secondary organic aerosol (SOA) formation from biogenic volatile organic compounds (BVOCs), 3 oxidation flow reactors (OFR) were used to expose ambient air to oxidants and their output was analyzed by state-of-the-art gas and aerosol instruments including a High-Resolution Aerosol Mass Spectrometer (HR-AMS), a HR Proton-Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-TOFMS), and Two HR-TOF Chemical Ionization Mass Spectrometers (HRToF-CIMS). Ambient air was exposed 24/7 to variable concentrations of each of the 3 main atmospheric oxidants (OH, NO3 radicals and O3) to investigate the oxidation of BVOCs (including isoprene derived epoxydiols, IEPOX) and SOA formation and aging. Effective OH exposures up to 1×1013 molec cm-3 s were achieved, equivalent to over a month of aging in the atmosphere. Multiple oxidation products from isoprene and monoterpenes including small gas-phase acids were observed in OH OFR. High SOA formation of up to 12 μg m-3 above ambient concentrations of 5 μg m-3 was observed under intermediate OH exposures, while very high OH exposures led to destruction of ~30% of ambient OA, indicating shifting contributions of functionalization vs. fragmentation, consistent with results from urban and terpene-dominated environments. The highest SOA enhancements were 3-4 times higher than ambient OA. More SOA is typically formed during nighttime when terpenes are higher and photochemistry is absent, and less during daytime when isoprene is higher, although the IEPOX pathway is suppressed in the OFR. SOA is also observed after exposure of ambient air to O3 or NO3, although the amounts and oxidation levels were lower than for OH. Formation of organic nitrates in the NO3 reaction will also be discussed.A major field campaign (Southern Oxidant and Aerosol

  16. Reactions of SIV species with organic compounds: formation mechanisms of organo-sulfur derivatives in atmospheric aerosols

    Science.gov (United States)

    Passananti, Monica; Shang, Jing; Dupart, Yoan; Perrier, Sébastien; George, Christian

    2015-04-01

    Secondary organic aerosol (SOA) have an important impact on climate, air quality and human health. However the chemical reactions involved in their formation and growth are not fully understood or well-constrained in climate models. It is well known that inorganic sulfur (mainly in oxidation states (+IV) and (+VI)) plays a key role in aerosol formation, for instance sulfuric acid is known to be a good nucleating gas. In addition, acid-catalyzed heterogeneous reactions of organic compounds has shown to produce new particles, with a clear enhancement in the presence of ozone (Iinuma 2013). Organosulfates have been detected in tropospheric particles and aqueous phases, which suggests they are products of secondary organic aerosol formation process (Tolocka 2012). Originally, the production of organosulfates was explained by the esterification reaction of alcohols, but this reaction in atmosphere is kinetically negligible. Other formation pathways have been suggested such as hydrolysis of peroxides and reaction of organic matter with sulfite and sulfate radical anions (SO3-, SO4-) (Nozière 2010), but it remains unclear if these can completely explain atmospheric organo-sulfur aerosol loading. To better understand the formation of organo-sulfur compounds, we started to investigate the reactivity of SIV species (SO2 and SO32-) with respect to specific functional groups (organic acids and double bonds) on atmospherically relevant carboxylic acids and alkenes. The experiments were carried out in the homogeneous aqueous phase and at the solid-gas interface. A custom built coated-wall flow tube reactor was developed to control relativity humidity, SO2 concentration, temperature and gas flow rate. Homogeneous and heterogeneous reaction kinetics were measured and resulting products were identified using liquid chromatography coupled with an orbitrap mass spectrometer (LC-HR-MS). The experiments were performed with and without the presence of ozone in order to evaluate any

  17. Modeling organic aerosols in a megacity: Potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

    Energy Technology Data Exchange (ETDEWEB)

    Hodzic, A.; Kleinman, L.; Jimenez, J. L.; Madronich, S.; Canagaratna, M. R.; DeCarlo, P. F.; Fast, J.

    2010-06-01

    It has been established that observed local and regional levels of secondary organic aerosols (SOA) in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (S/IVOC) in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA), their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007) ('ROB') and Grieshop et al. (2009) ('GRI') are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS) data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (2-4 times) with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009), both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40-60% of the total measured SOA at the surface during the day and is somewhat larger than that from commonly measured aromatic VOCs, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively

  18. Modeling organic aerosols in a megacity: potential contribution of semi-volatile and intermediate volatility primary organic compounds to secondary organic aerosol formation

    Directory of Open Access Journals (Sweden)

    A. Hodzic

    2010-06-01

    Full Text Available It has been established that observed local and regional levels of secondary organic aerosols (SOA in polluted areas cannot be explained by the oxidation and partitioning of anthropogenic and biogenic VOC precursors, at least using current mechanisms and parameterizations. In this study, the 3-D regional air quality model CHIMERE is applied to estimate the potential contribution to SOA formation of recently identified semi-volatile and intermediate volatility organic precursors (S/IVOC in and around Mexico City for the MILAGRO field experiment during March 2006. The model has been updated to include explicitly the volatility distribution of primary organic aerosols (POA, their gas-particle partitioning and the gas-phase oxidation of the vapors. Two recently proposed parameterizations, those of Robinson et al. (2007 ("ROB" and Grieshop et al. (2009 ("GRI" are compared and evaluated against surface and aircraft measurements. The 3-D model results are assessed by comparing with the concentrations of OA components from Positive Matrix Factorization of Aerosol Mass Spectrometer (AMS data, and for the first time also with oxygen-to-carbon ratios derived from high-resolution AMS measurements. The results show a substantial enhancement in predicted SOA concentrations (2–4 times with respect to the previously published base case without S/IVOCs (Hodzic et al., 2009, both within and downwind of the city leading to much reduced discrepancies with the total OA measurements. Model improvements in OA predictions are associated with the better-captured SOA magnitude and diurnal variability. The predicted production from anthropogenic and biomass burning S/IVOC represents 40–60% of the total measured SOA at the surface during the day and is somewhat larger than that from commonly measured aromatic VOCs, especially at the T1 site at the edge of the city. The SOA production from the continued multi-generation S/IVOC oxidation products continues actively

  19. Formation of Epoxide Derived SOA and Gas-Phase Acids through Aqueous Aerosol Processing in the Southeastern United States during SOAS

    Science.gov (United States)

    Skog, K.; Teng, A.; Nguyen, T. B.; Nguyen, K.; Suda, S. R.; Xu, L.; Isaacman-VanWertz, G. A.; Feiner, P. A.; Zhang, L.; Olson, K. F.; Koss, A.; Wild, R. J.; St Clair, J.; Crounse, J.; Baumann, K.; Wennberg, P. O.; Petters, M.; Carlton, A. M. G.; Ng, N. L.; Brune, W. H.; De Gouw, J. A.; Goldstein, A. H.; Brown, S. S.; Edgerton, E. S.; McNeill, V. F.; Keutsch, F. N.

    2015-12-01

    Secondary organic aerosol (SOA) contributes to climate and adversely affects human health, but the formation of SOA is poorly understood. Recent studies have proposed that aqueous processing of water-soluble compounds like glyoxal and IEPOX can help explain the abundance of organosulfates, higher oxygen to carbon ratios, and SOA abundance. A comprehensive set of ambient gas- and aerosol-phase data was collected during June and July of 2013 as part of the Southern Oxidant and Aerosol Study (SOAS) at the Centreville, AL ground site. Both gas-phase photochemistry and aqueous-phase aerosol chemistry were modeled using a zero-dimensional box model. While it has been suggested that glyoxal can contribute to aqueous aerosol through the formation of acids and higher-molecular-weight compounds, it did not produce enhanced aqSOA concentrations. Instead, processing of aqueous glyoxal resulted in the production of gas-phase acids. AqSOA consisted almost entirely of epoxide processing products, mainly from the processing of IEPOX to methyl tetrol, and the organosulfate. In addition, the pinene oxides contributed to the formation of aqSOA, through the formation of organosulfates, diols, and organonitrates. These data are consistent with the abundance of IEPOX and pinene oxide organonitrate derived SOA seen at this site.

  20. Modelling of organic aerosols over Europe (2002–2007 using a volatility basis set (VBS framework: application of different assumptions regarding the formation of secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    K. E. Yttri

    2012-09-01

    Full Text Available A new organic aerosol module has been implemented into the EMEP chemical transport model. Four different volatility basis set (VBS schemes have been tested in long-term simulations for Europe, covering the six years 2002–2007. Different assumptions regarding partitioning of primary organic aerosol and aging of primary semi-volatile and intermediate volatility organic carbon (S/IVOC species and secondary organic aerosol (SOA have been explored. Model results are compared to filter measurements, aerosol mass spectrometry (AMS data and source apportionment studies, as well as to other model studies. The present study indicates that many different sources contribute significantly to organic aerosol in Europe. Biogenic and anthropogenic SOA, residential wood combustion and vegetation fire emissions may all contribute more than 10% each over substantial parts of Europe. This study shows smaller contributions from biogenic SOA to organic aerosol in Europe than earlier work, but relatively greater anthropogenic SOA. Simple VBS based organic aerosol models can give reasonably good results for summer conditions but more observational studies are needed to constrain the VBS parameterisations and to help improve emission inventories. The volatility distribution of primary emissions is one important issue for further work. Emissions of volatile organic compounds from biogenic sources are also highly uncertain and need further validation. We can not reproduce winter levels of organic aerosol in Europe, and there are many indications that the present emission inventories substantially underestimate emissions from residential wood combustion in large parts of Europe.

  1. Analysis of secondary organic aerosol formation and aging using positive matrix factorization of high-resolution aerosol mass spectra: application to the dodecane low-NOx system

    Directory of Open Access Journals (Sweden)

    R. C. Flagan

    2012-12-01

    Full Text Available Positive matrix factorization (PMF of high-resolution laboratory chamber aerosol mass spectra is applied for the first time, the results of which are consistent with molecular level MOVI-HRToF-CIMS aerosol-phase and CIMS gas-phase measurements. Secondary organic aerosol was generated by photooxidation of dodecane under low-NOx conditions in the Caltech environmental chamber. The PMF results exhibit three factors representing a combination of gas-particle partitioning, chemical conversion in the aerosol, and wall deposition. The slope of the measured high-resolution aerosol mass spectrometer (HR-ToF-AMS composition data on a Van Krevelen diagram is consistent with that of other low-NOx alkane systems in the same O : C range. Elemental analysis of the PMF factor mass spectral profiles elucidates the combinations of functionality that contribute to the slope on the Van Krevelen diagram.

  2. Protein corona formation in bronchoalveolar fluid enhances diesel exhaust nanoparticle uptake and pro-inflammatory responses in macrophages.

    Science.gov (United States)

    Shaw, Catherine A; Mortimer, Gysell M; Deng, Zhou J; Carter, Edwin S; Connell, Shea P; Miller, Mark R; Duffin, Rodger; Newby, David E; Hadoke, Patrick W F; Minchin, Rodney F

    2016-09-01

    In biological fluids nanoparticles bind a range of molecules, particularly proteins, on their surface. The resulting protein corona influences biological activity and fate of nanoparticle in vivo. Corona composition is often determined by the biological milieu encountered at the entry portal into the body, and, can therefore, depend on the route of exposure to the nanoparticle. For environmental nanoparticles where exposure is by inhalation, this will be lung lining fluid. This study examined plasma and bronchoalveolar fluid (BALF) protein binding to engineered and environmental nanoparticles. We hypothesized that protein corona on nanoparticles would influence nanoparticle uptake and subsequent pro-inflammatory biological response in macrophages. All nanoparticles bound plasma and BALF proteins, but the profile of bound proteins varied between nanoparticles. Focusing on diesel exhaust nanoparticles (DENP), we identified proteins bound from plasma to include fibrinogen, and those bound from BALF to include albumin and surfactant proteins A and D. The presence on DENP of a plasma-derived corona or one of purified fibrinogen failed to evoke an inflammatory response in macrophages. However, coronae formed in BALF increased DENP uptake into macrophages two fold, and increased nanoparticulate carbon black (NanoCB) uptake fivefold. Furthermore, a BALF-derived corona increased IL-8 release from macrophages in response to DENP from 1720 ± 850 pg/mL to 5560 ± 1380 pg/mL (p = 0.014). These results demonstrate that the unique protein corona formed on nanoparticles plays an important role in determining biological reactivity and fate of nanoparticle in vivo. Importantly, these findings have implications for the mechanism of detrimental properties of environmental nanoparticles since the principle route of exposure to such particles is via the lung.

  3. Open burning of rice, corn and wheat straws: primary emissions, photochemical aging, and secondary organic aerosol formation

    Science.gov (United States)

    Fang, Zheng; Deng, Wei; Zhang, Yanli; Ding, Xiang; Tang, Mingjin; Liu, Tengyu; Hu, Qihou; Zhu, Ming; Wang, Zhaoyi; Yang, Weiqiang; Huang, Zhonghui; Song, Wei; Bi, Xinhui; Chen, Jianmin; Sun, Yele; George, Christian; Wang, Xinming

    2017-12-01

    Agricultural residues are among the most abundant biomass burned globally, especially in China. However, there is little information on primary emissions and photochemical evolution of agricultural residue burning. In this study, indoor chamber experiments were conducted to investigate primary emissions from open burning of rice, corn and wheat straws and their photochemical aging as well. Emission factors of NOx, NH3, SO2, 67 non-methane hydrocarbons (NMHCs), particulate matter (PM), organic aerosol (OA) and black carbon (BC) under ambient dilution conditions were determined. Olefins accounted for > 50 % of the total speciated NMHCs emission (2.47 to 5.04 g kg-1), indicating high ozone formation potential of straw burning emissions. Emission factors of PM (3.73 to 6.36 g kg-1) and primary organic carbon (POC, 2.05 to 4.11 gC kg-1), measured at dilution ratios of 1300 to 4000, were lower than those reported in previous studies at low dilution ratios, probably due to the evaporation of semi-volatile organic compounds under high dilution conditions. After photochemical aging with an OH exposure range of (1.97-4.97) × 1010 molecule cm-3 s in the chamber, large amounts of secondary organic aerosol (SOA) were produced with OA mass enhancement ratios (the mass ratio of total OA to primary OA) of 2.4-7.6. The 20 known precursors could only explain 5.0-27.3 % of the observed SOA mass, suggesting that the major precursors of SOA formed from open straw burning remain unidentified. Aerosol mass spectrometry (AMS) signaled that the aged OA contained less hydrocarbons but more oxygen- and nitrogen-containing compounds than primary OA, and carbon oxidation state (OSc) calculated with AMS resolved O / C and H / C ratios increased linearly (p < 0.001) with OH exposure with quite similar slopes.

  4. A new source of oxygenated organic aerosol and oligomers

    Directory of Open Access Journals (Sweden)

    J. Liggio

    2013-03-01

    Full Text Available A large oxygenated organic uptake to aerosols was observed when exposing ambient urban air to inorganic acidic and non-acidic sulfate seed aerosol. For non-acidic seed aerosol the uptake was attributed to the direct dissolution of primary vehicle exhaust gases into the aqueous aerosol fraction, and was correlated to the initial seed sulphate mass. The uptake of primary oxygenated organic gases to aerosols in this study represents a significant amount of organic aerosol (OA that may be considered primary when compared to that reported for primary organic aerosol (POA, but is considerably more oxygenated (O : C ~ 0.3 than traditional POA. Consequently, a fraction of measured ambient oxygenated OA, which correlates with secondary sulphate, may in fact be of a primary, rather than secondary source. These results represent a new source of oxygenated OA on neutral aerosol and imply that the uptake of primary organic gases will occur in the ambient atmosphere, under dilute conditions, and in the presence of pre-existing SO4 aerosols which contain water. Conversely, under acidic seed aerosol conditions, oligomer formation was observed with the uptake of organics being enhanced by a factor of three or more compared to neutral aerosols, and in less than 2 min, representing an additional source of SOA to the atmosphere. This resulted in a trajectory in Van Krevelen space towards higher O : C (slope ~ −1.5, despite a lack of continual gas-phase oxidation in this closed system. The results demonstrate that high molecular weight species will form on acidic aerosols at the ambient level and mixture of organic gases, but are otherwise unaffected by subsequent aerosol neutralization, and that aerosol acidity will affect the organic O : C via aerosol-phase reactions. These two processes, forming oxygenated POA under neutral conditions and SOA under acidic conditions can contribute to the total ambient OA mass and the evolution of ambient aerosol O : C ratios

  5. Lidar Observation of Aerosol and Temperature Stratification over Urban Area During the Formation of a Stable Atmospheric PBL

    Science.gov (United States)

    Kolev, I.; Parvanov, O.; Kaprielov, B.; Mitev, V.; Simeonov, V.; Grigorov, I.

    1992-01-01

    In recent years, the processes in the atmospheric planetary boundary layer (PBL) over urban areas were intensely investigated, due to ecological problems related to the air, soil, and water pollution. New pollution sources in new residential districts, when in contradiction to the microclimate and topography requirements of that region, create a number of considerable hazards and problems. The present study is a continuation of our preceding investigations and aims at revealing the aerosol structure and stratification during the transition after sunset as measured by two lidars. Such observation of the nocturnal, stable PBL formation over an urban area in Bulgaria has not been reported before. The lidars' high time and spatial resolutions allow the changes of the internal structure of the PBL's part located above the surface layer to be observed.

  6. Regional and global impacts of Criegee intermediates on atmospheric sulphuric acid concentrations and first steps of aerosol formation.

    Science.gov (United States)

    Percival, Carl J; Welz, Oliver; Eskola, Arkke J; Savee, John D; Osborn, David L; Topping, David O; Lowe, Douglas; Utembe, Steven R; Bacak, Asan; McFiggans, Gordon; Cooke, Michael C; Xiao, Ping; Archibald, Alexander T; Jenkin, Michael E; Derwent, Richard G; Riipinen, Ilona; Mok, Daniel W K; Lee, Edmond P F; Dyke, John M; Taatjes, Craig A; Shallcross, Dudley E

    2013-01-01

    Carbonyl oxides ("Criegee intermediates"), formed in the ozonolysis of alkenes, are key species in tropospheric oxidation of organic molecules and their decomposition provides a non-photolytic source of OH in the atmosphere (Johnson and Marston, Chem. Soc. Rev., 2008, 37, 699, Harrison et al, Sci, Total Environ., 2006, 360, 5, Gäb et al., Nature, 1985, 316, 535, ref. 1-3). Recently it was shown that small Criegee intermediates, C.I.'s, react far more rapidly with SO2 than typically represented in tropospheric models, (Welz, Science, 2012, 335, 204, ref. 4) which suggested that carbonyl oxides could have a substantial influence on the atmospheric oxidation of SO2. Oxidation of 502 is the main atmospheric source of sulphuric acid (H2SO4), which is a critical contributor to aerosol formation, although questions remain about the fundamental nucleation mechanism (Sipilä et al., Science, 2010, 327, 1243, Metzger et al., Proc. Natl. Acad. Sci. U. S. A., 2010 107, 6646, Kirkby et al., Nature, 2011, 476, 429, ref. 5-7). Non-absorbing atmospheric aerosols, by scattering incoming solar radiation and acting as cloud condensation nuclei, have a cooling effect on climate (Intergovernmental Panel on Climate Change (IPCC), Climate Change 2007: The Physical Science Basis, Cambridge University Press, 2007, ref. 8). Here we explore the effect of the Criegees on atmospheric chemistry, and demonstrate that ozonolysis of alkenes via the reaction of Criegee intermediates potentially has a large impact on atmospheric sulphuric acid concentrations and consequently the first steps in aerosol production. Reactions of Criegee intermediates with SO2 will compete with and in places dominate over the reaction of OH with SO2 (the only other known gas-phase source of H2SO4) in many areas of the Earth's surface. In the case that the products of Criegee intermediate reactions predominantly result in H2SO4 formation, modelled particle nucleation rates can be substantially increased by the improved

  7. Formation and Growth of Sulfate Aerosols in the Presence of Hydrocarbons: Results from the 2013 Summer Oil Sands FOSSILs Field Campaign, Alberta, Canada

    Science.gov (United States)

    Amiri, N.; Ghahremaninezhad, R.; Rempillo, O. T.; Norman, A. L.

    2014-12-01

    Sulfur dioxide oxidation and the effect of oxidation products in formation and growth of aerosols have been studied widely. Despite this, significant gaps still exist in understanding the role of organic matter in SO2 oxidation. Organic molecules, such as Criegee radicals originating from biogenic sources, are expected to be important for SO2 oxidation in addition to organic molecules of anthropogenic origin. A study of SO2 and aerosol sulfate downwind of the oil sands region was conducted as part of the FOSSILS campaign in the summer of 2013 to better understand aerosol growth from SO2 oxidation in the presence of hydrocarbons and the distribution of sulfate in size-segregated aerosols. Hydrocarbons present in the atmosphere during the sampling campaign, collected using evacuated canisters, were characterized using a pre-concentration trap coupled to a GC-FID. The results from this campaign will be explored to determine SO2 oxidation pathways and the effects of oxidation products to aerosol formation and growth.

  8. Formation of carbonate pipes in the northern Okinawa Trough linked to strong sulfate exhaustion and iron supply

    Science.gov (United States)

    Peng, Xiaotong; Guo, Zixiao; Chen, Shun; Sun, Zhilei; Xu, Hengchao; Ta, Kaiwen; Zhang, Jianchao; Zhang, Lijuan; Li, Jiwei; Du, Mengran

    2017-05-01

    The microbial anaerobic oxidation of methane (AOM), a key biogeochemical process that consumes substantial amounts of methane produced in seafloor sediments, can lead to the formation of carbonate deposits at or beneath the sea floor. Although Fe oxide-driven AOM has been identified in cold seep sediments, the exact mode by which it may influence the formation of carbonate deposits remains poorly understood. Here, we characterize the morphology, petrology and geochemistry of a methane-derived Fe-rich carbonate pipe in the northern Okinawa Trough (OT). We detect abundant authigenic pyrites, as well as widespread trace Fe, within microbial mat-like carbonate veins in the pipe. The in situ δ34S values of these pyrites range from -3.9 to 31.6‰ (VCDT), suggesting a strong consumption of seawater sulfate by sulfate-driven AOM at the bottom of sulfate reduction zone. The positive δ56Fe values of pyrite and notable enrichment of Fe in the OT pipe concurrently indicate that the pyrites are primarily derived from Fe oxides in deep sediments. We propose that the Fe-rich carbonate pipe formed at the bottom of sulfate reduction zone, below which Fe-driven AOM, rather than Fe-oxide reduction coupled to organic matter degradation, might be responsible for the abundantly available Fe2+ in the fluids from which pyrites precipitated. The Fe-rich carbonate pipe described in this study probably represents the first fossil example of carbonate deposits linked to Fe-driven AOM. Because Fe-rich carbonate deposits have also been found at other cold seeps worldwide, we infer that similar processes may play an essential role in biogeochemical cycling of sub-seafloor methane and Fe at continental margins.

  9. The Formation of Porous Membranes by Filtration of Aerosol Nano-particles

    DEFF Research Database (Denmark)

    Andersen, Sune Klint; Johannessen, Tue; Mosleh, Majid

    2002-01-01

    Flame-generated aerosol particles of Al2O3 were deposited by gas filtration on two types of porous and ceramic tubes of α-Al2O3 with mean pore diameters of 450 and 2700 nm, respectively. The particles were aggregates with average mobility diameters in the range of 30¨¢100 nm and primary particle...... diameters of 4¨¢8 nm. The particles are characterized by differential mobility analysis, transmission electron microscopy, and by their specific surface area. The deposited membranes are characterized by gas permeability measurements, scanning electron microscopy, and by their pore size distribution from...... nitrogen capillary condensation. The particles form a distinct, homogeneous membrane layer with a porosity of ∼90% on top of the substrate surface and only penetrate slightly into the substrate structure. The mean pore sizes of the deposited membranes determined by nitrogen condensation agree approximately...

  10. Phase, size and shape controlled formation of aerosol generated nickel and nickel oxide nanoparticles

    Energy Technology Data Exchange (ETDEWEB)

    Ortega, D., E-mail: d.ponce@ucl.ac.uk [Department of Physics and Astronomy, University College London, WC1E 6BT London (United Kingdom); London Centre for Nanotechnology, Gordon Street, WC1H 0AH London (United Kingdom); Kuznetsov, M.V. [N.P. Ogarev Mordovian State University, Saransk, Republic of Mordovia 430005 (Russian Federation); Morozov, Yu.G.; Belousova, O.V. [Institute of Structural Macrokinetics and Materials Science, Chernogolovka, Moscow Region 142432 (Russian Federation); Parkin, I.P. [Department of Chemistry, Materials Chemistry Centre, University College London, 20 Gordon Street, WC1H 0AJ London (United Kingdom)

    2013-12-05

    Highlights: •Structural and magnetic characterization of aerosol Ni nanoparticles. •Experimental parameters affecting size, shape and composition are discussed. •Larger spherical particles with the highest Ni content are produced by using an Ar flow. •Coalescence rate of primary particles is accelerated by increasing Ni feeding rate. •Ni nanoparticles show bulk-like saturation magnetization values. -- Abstract: Ferromagnetic Ni nanoparticles were formed by a levitation-jet aerosol synthesis under different gas environments and metal precursor feed rates. At a constant background gas inlet temperature, it was found that a higher Ni loading resulted in enhanced particle growth through coalescence. He partial atmosphere favors surface condensation of evaporated Ni atoms over coalescence as the surface area reduction mechanism in the nanoparticles. A flow of 2.5% air in the background gas mixture was enough to oxidize 75% of the initial Ni load, inducing a drastic destabilization of particle size and shape distribution. Regardless of the background inert gas composition, necked nanoparticles were observed in samples prepared with a 1 g/h Ni feed rate, whereas discrete nanoparticles resulted from a higher feed rate of ca. 4 g/h, confirming the key role of Ni loading on the rate of coalescence. The highest saturation magnetization (51.75 A m{sup 2} kg{sup −1} measured at 300 K) and the lowest coercivity (0.008 T) were obtained under an Ar flow. Zero-field cooled and field-cooled magnetization curves measured under an applied field of 10{sup −2} T revealed that the blocking processes of nanoparticles are dominated by their particle size distributions, with some features attributable to interparticle interactions.

  11. Reactive Uptake of Ammonia to Secondary Organic Aerosols: Kinetics of Organonitrogen Formation

    Science.gov (United States)

    Liu, Yongchun; Liggio, John; Staebler, Ralf; Li, Shao-Meng

    2015-04-01

    Organonitrogen compounds originating from the heterogeneous uptake of NH3 or amines by secondary organic aerosol (SOA) has received significant attention recently. This is primarily due to its potential contribution to brown carbon (BrC), which can absorb solar radiation and affect climate. In addition, particle phase Organonitrogen species may represent a means of altering regional nitrogen cycles and/or nitrogen deposition patterns though the sequestering of ambient ammonia which is ultimately deposited downwind. Several reduced nitrogen forming heterogeneous reactions have previously been proposed, including Schiff base and/or Mannich reactions between NH3, ammonium salts or amines and organic carbonyl functional groups in particles. In order to assess and model the possible impact of Schiff base, Mannich or other N-forming reactions (via NH3) on the radiative forcing ability of ambient SOA and/or its impact on N-deposition, the kinetics of such heterogeneous reactions are required, and yet remain largely unknown. In the current study, the uptake kinetics of NH3 to form organonitrogen compounds in SOA derived from the ozonolysis of α-pinene and the OH oxidation of m-xylene is reported for the first time from experiments performed in a 9 m3 smog chamber equipped with a High Resolution Time-of-Flight Aerosol Mass Spectrometer. The results demonstrate that particle bound organonitrogen compounds are mainly formed by NH3 uptake onto newly formed SOA (~1 hr), but relatively little onto more aged SOA. The uptake coefficients of NH3 to form organonitrogen compounds (between 0-150 min) are on the order of 10-4-10-3 and are prominently dependent upon particle acidity. Following 6 hours of reaction, the total organonitrogen mass contributed up to 10.0±1.5 wt% and 31.5±4.4 wt% to the total SOA mass from the ozonolysis of α-pinene and OH oxidation of m-xylene. The influence of VOC precursors, seed particle acidity and gaseous NH3 concentration on the obtained uptake

  12. Impact of chamber wall loss of gaseous organic compounds on secondary organic aerosol formation: explicit modeling of SOA formation from alkane and alkene oxidation

    Directory of Open Access Journals (Sweden)

    Y. S. La

    2016-02-01

    Full Text Available Recent studies have shown that low volatility gas-phase species can be lost onto the smog chamber wall surfaces. Although this loss of organic vapors to walls could be substantial during experiments, its effect on secondary organic aerosol (SOA formation has not been well characterized and quantified yet. Here the potential impact of chamber walls on the loss of gaseous organic species and SOA formation has been explored using the Generator for Explicit Chemistry and Kinetics of the Organics in the Atmosphere (GECKO-A modeling tool, which explicitly represents SOA formation and gas–wall partitioning. The model was compared with 41 smog chamber experiments of SOA formation under OH oxidation of alkane and alkene series (linear, cyclic and C12-branched alkanes and terminal, internal and 2-methyl alkenes with 7 to 17 carbon atoms under high NOx conditions. Simulated trends match observed trends within and between homologous series. The loss of organic vapors to the chamber walls is found to affect SOA yields as well as the composition of the gas and the particle phases. Simulated distributions of the species in various phases suggest that nitrates, hydroxynitrates and carbonylesters could substantially be lost onto walls. The extent of this process depends on the rate of gas–wall mass transfer, the vapor pressure of the species and the duration of the experiments. This work suggests that SOA yields inferred from chamber experiments could be underestimated up a factor of 2 due to the loss of organic vapors to chamber walls.

  13. The effect of gas-phase polycyclic aromatic hydrocarbons on the formation and properties of biogenic secondary organic aerosol particles

    Energy Technology Data Exchange (ETDEWEB)

    Zelenyuk, Alla [Pacific Northwest National Laboratory; USA; Imre, Dan G. [Imre Consulting; USA; Wilson, Jacqueline [Pacific Northwest National Laboratory; USA; Bell, David M. [Pacific Northwest National Laboratory; USA; Suski, Kaitlyn J. [Pacific Northwest National Laboratory; USA; Shrivastava, Manish [Pacific Northwest National Laboratory; USA; Beránek, Josef [Pacific Northwest National Laboratory; USA; Alexander, M. Lizabeth [Pacific Northwest National Laboratory; USA; Kramer, Amber L. [Department of Chemistry; Oregon State University; USA; Massey Simonich, Staci L. [Department of Chemistry; Oregon State University; USA; Environmental and Molecular Toxicology; Oregon State University

    2017-01-01

    When secondary organic aerosol (SOA) particles are formed by ozonolysis in the presence of gas-phase polycyclic aromatic hydrocarbons (PAHs), their formation and properties are significantly different from SOA particles formed without PAHs. For all SOA precursors and all PAHs, discussed in this study, the presence of the gas-phase PAHs during SOA formation significantly affects particle mass loadings, composition, growth, evaporation kinetics, and viscosity. SOA particles formed in the presence of PAHs have, as part of their compositions, trapped unreacted PAHs and products of heterogeneous reactions between PAHs and ozone. Compared to ‘pure’ SOA particles, these particles exhibit slower evaporation kinetics, have higher fractions of non-volatile components, like oligomers, and higher viscosities, assuring their longer atmospheric lifetimes. In turn, the increased viscosity and decreased volatility provide a shield that protects PAHs from chemical degradation and evaporation, allowing for the long-range transport of these toxic pollutants. The magnitude of the effect of PAHs on SOA formation is surprisingly large. The presence of PAHs during SOA formation increases mass loadings by factors of two to five, and particle number concentrations, in some cases, by more than a factor of 100. Increases in SOA mass, particle number concentrations, and lifetime have important implications to many atmospheric processes related to climate, weather, visibility, and human health, all of which relate to the interactions between biogenic SOA and anthropogenic PAHs. The synergistic relationship between SOA and PAHs presented here are clearly complex and call for future research to elucidate further the underlying processes and their exact atmospheric implications.

  14. Improving the simulation of organic aerosols from anthropogenic and burning sources: a simplified SOA formation mechanism and the impact of trash burning

    Science.gov (United States)

    Hodzic, A.; Wiedinmyer, C.; Jimenez, J. L.

    2011-12-01

    Organic aerosols (OA) are an major component of fine aerosols, but their sources are poorly understood. We present results of two methods to improve OA predictions in anthropogenic pollution and biomass-burning impacted regions. (1) An empirical parameterization for secondary organic aerosol (SOA) formation in polluted air and biomass burning smoke is implemented into community chemistry-transport models (WRF/Chem and CHIMERE) and tested in this work, towards the goal of a computationally inexpensive method to calculate pollution and biomass burning SOA. This approach is based on the observed proportionality of SOA concentrations to excess CO and photochemical age of the airmass, as described in Hodzic and Jimenez (GMDD, 2011). The oxygen to carbon ratio in organic aerosols is also parameterizated vs. photochemical aged based on the ambient observations, and is used to estimate the aerosol hygroscopicity and CCN activity. The predicted SOA is assessed against observations from the Mexico City metropolitan area during the MILAGRO 2006 field experiment, and compared to previous model results using the more complex volatility basis approach (VBS) of Robinson et al.. The results suggest that the simplified approach reproduces the observed average SOA mass within 30% in the urban area and downwind, and gives better results than the original VBS. In addition to being much less computationally expensive than VBS-type methods, the empirical approach can also be used in regions where the emissions of SOA precursors are not yet available. (2) The contribution of trash burning emissions to primary and secondary organic aerosols in Mexico City are estimated, using a recently-developed emission inventory. Submicron antimony (Sb) is used as a garbage-burning tracer following the results of Christian et al. (ACP 2010), which allows evaluation of the emissions inventory. Results suggests that trash burning may be an appreciable source of organic aerosols in the Mexico City

  15. Exhaust emissions of volatile organic compounds of powered two-wheelers: effect of cold start and vehicle speed. Contribution to greenhouse effect and tropospheric ozone formation.

    Science.gov (United States)

    Costagliola, M Antonietta; Murena, Fabio; Prati, M Vittoria

    2014-01-15

    Powered two-wheeler (PTW) vehicles complying with recent European type approval standards (stages Euro 2 and Euro 3) were tested on chassis dynamometer in order to measure exhaust emissions of about 25 volatile organic compounds (VOCs) in the range C1-C7, including carcinogenic compounds as benzene and 1,3-butadiene. The fleet consists of a moped (engine capacity ≤ 50 cm(3)) and three fuel injection motorcycles of different engine capacities (150, 300 and 400 cm(3)). Different driving conditions were tested (US FPT cycle, constant speed). Due to the poor control of the combustion and catalyst efficiency, moped is the highest pollutant emitter. In fact, fuel injection strategy and three way catalyst with lambda sensor are able to reduce VOC motorcycles' emission of about one order of magnitude with respect to moped. Cold start effect, that is crucial for the assessment of actual emission of PTWs in urban areas, was significant: 30-51% of extra emission for methane. In the investigated speed range, moped showed a significant maximum of VOC emission factor at minimum speed (10 km/h) and a slightly decreasing trend from 20 to 60 km/h; motorcycles showed on the average a less significant peak at 10 km/h, a minimum at 30-40 km/h and then an increasing trend with a maximum emission factor at 90 km/h. Carcinogenic VOCs show the same pattern of total VOCs. Ozone Formation Potential (OFP) was estimated by using Maximum Incremental Reactivity scale. The greatest contribution to tropospheric ozone formation comes from alkenes group which account for 50-80% to the total OFP. VOC contribution effect on greenhouse effect is negligible with respect to CO2 emitted. © 2013.

  16. Smog chamber experiments to investigate Henry's law constants of glyoxal using different seed aerosols as well as imidazole formation in the presence of ammonia

    Science.gov (United States)

    Jakob, Ronit

    2015-04-01

    Aerosols play an important role in the chemistry and physics of the atmosphere. Hence, they have a direct as well as an indirect impact on the earth's climate. Depending on their formation, one distinguishes between primary and secondary aerosols[1]. Important groups within the secondary aerosols are the secondary organic aerosols (SOAs). In order to improve predictions about these impacts on the earth's climate the existing models need to be optimized, because they still underestimate SOA formation[2]. Glyoxal, the smallest α-dicarbonyl, not only acts as a tracer for SOA formation but also as a direct contributor to SOA. Because glyoxal has such a high vapour pressure, it was common knowledge that it does not take part in gas-particle partitioning and therefore has no impact on direct SOA formation. However, the Henry's law constant for glyoxal is surprisingly high. This has been explained by the hydration of the aldehyde groups, which means that a species with a lower vapour pressure is produced. Therefore the distribution of glyoxal between gas- and particle phase is atmospherically relevant and the direct contribution of glyoxal to SOA can no longer be neglected[3]. Besides this particulate glyoxal is able to undergo heterogeneous chemistry with gaseous ammonia to form imidazoles. This plays an important role for regions with aerosols exhibiting alkaline pH values for example from lifestock or soil dust because imidazoles as nitrogen containing compounds change the optical properties of aerosols[4]. A high salt concentration present in chamber seed aerosols leads to an enhanced glyoxal uptake into the particle. This effect is called "salting-in". The salting effect depends on the composition of the seed aerosol as well as the soluble compound. For very polar compounds, like glyoxal, a "salting-in" is observed[3]. Glyoxal particle formation during a smog chamber campaign at Paul-Scherrer-Institut (PSI) in Switzerland was examined using different seed aerosols

  17. Radiative effects of tropospheric aerosols on the evolution of the atmospheric boundary layer and its feedback on the haze formation

    Science.gov (United States)

    Wei, Chao; Su, Hang; Cheng, Yafang

    2016-04-01

    Planetary boundary layer (PBL) plays a key role in air pollution dispersion and influences day-to-day air quality. Some studies suggest that high aerosol loadings during severe haze events may modify PBL dynamics by radiative effects and hence enhance the development of haze. This study mainly investigates the radiative effects of tropospheric aerosols on the evolution of the atmospheric boundary layer by conducting simulations with Weather Research and Forecasting single-column model (WRF-SCM). We find that high aerosol loading in PBL depressed boundary layer height (PBLH). But the magnitude of the changes of PBLH after adding aerosol loadings in our simulations are small and can't explain extreme high aerosol concentrations observed. We also investigate the impacts of the initial temperature and moisture profiles on the evolution of PBL. Our studies show that the impact of the vertical profile of moisture is comparable with aerosol effects.

  18. Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area

    Directory of Open Access Journals (Sweden)

    A. P. Tsimpidi

    2010-01-01

    Full Text Available New primary and secondary organic aerosol modules have been added to PMCAMx, a three dimensional chemical transport model (CTM, for use with the SAPRC99 chemistry mechanism based on recent smog chamber studies. The new modelling framework is based on the volatility basis-set approach: both primary and secondary organic components are assumed to be semivolatile and photochemically reactive and are distributed in logarithmically spaced volatility bins. This new framework with the use of the new volatility basis parameters for low-NOx and high-NOx conditions tends to predict 4–6 times higher anthropogenic SOA concentrations than those predicted with the older generation of models. The resulting PMCAMx-2008 was applied in Mexico City Metropolitan Area (MCMA for approximately a week during April 2003 during a period of very low regional biomass burning impact. The emission inventory, which uses as a starting point the MCMA 2004 official inventory, is modified and the primary organic aerosol (POA emissions are distributed by volatility based on dilution experiments. The predicted organic aerosol (OA concentrations peak in the center of Mexico City, reaching values above 40 μg m−3. The model predictions are compared with the results of the Positive Matrix Factorization (PMF analysis of the Aerosol Mass Spectrometry (AMS observations. The model reproduces both Hydrocarbon-like Organic Aerosol (HOA and Oxygenated Organic Aerosol (OOA concentrations and diurnal profiles. The small OA underprediction during the rush-hour periods and overprediction in the afternoon suggest potential improvements to the description of fresh primary organic emissions and the formation of the oxygenated organic aerosols, respectively, although they may also be due to errors in the simulation of dispersion and vertical mixing. However, the AMS OOA data are not specific enough to prove that the model reproduces the organic aerosol

  19. Secondary organic aerosol formation from phenolic compounds in the absence of NOx

    Science.gov (United States)

    Nakao, S.; Clark, C.; Tang, P.; Sato, K.; Cocker, D., III

    2011-10-01

    SOA formation from benzene, toluene, m-xylene, and their corresponding phenolic compounds were investigated using the UCR/CE-CERT Environmental Chamber to evaluate the importance of phenolic compounds as intermediate species in aromatic SOA formation. SOA formation yield measurements coupled to gas-phase yield measurements indicate that approximately 20% of the SOA of benzene, toluene, and m-xylene could be ascribed to the phenolic route under low NOx conditions. The SOA densities tend to be initially as high as approximately 1.8 g cm-3 and eventually reach the range of 1.3-1.4 g cm-3. The final SOA density was found to be independent of elemental ratio (O/C) indicating that applying constant density (e.g., 1.4 g cm-3) to SOA formed from different aromatic compounds tested in this study is a reasonable approximation. Results from a novel on-line PILS-TOFMS (Particle-into-Liquid Sampler coupled with Agilent Time-of-Flight Mass Spectrometer) are reported. Major signals observed by the on-line/off-line Agilent TOFMS indicated that products had the same number of carbon atoms as their parent aromatics, suggesting importance of ring-retaining products or ring-opening products following ring-cleavage.

  20. Assessing the impact of anthropogenic pollution on isoprene-derived secondary organic aerosol formation in PM2.5 collected from the Birmingham, Alabama, ground site during the 2013 Southern Oxidant and Aerosol Study

    Directory of Open Access Journals (Sweden)

    W. Rattanavaraha

    2016-04-01

    Full Text Available In the southeastern US, substantial emissions of isoprene from deciduous trees undergo atmospheric oxidation to form secondary organic aerosol (SOA that contributes to fine particulate matter (PM2.5. Laboratory studies have revealed that anthropogenic pollutants, such as sulfur dioxide (SO2, oxides of nitrogen (NOx, and aerosol acidity, can enhance SOA formation from the hydroxyl radical (OH-initiated oxidation of isoprene; however, the mechanisms by which specific pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected at the Birmingham, Alabama (BHM, ground site during the 2013 Southern Oxidant and Aerosol Study (SOAS. Sample extracts were analyzed by gas chromatography–electron ionization-mass spectrometry (GC/EI-MS with prior trimethylsilylation and ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS to identify known isoprene SOA tracers. Tracers quantified using both surrogate and authentic standards were compared with collocated gas- and particle-phase data as well as meteorological data provided by the Southeastern Aerosol Research and Characterization (SEARCH network to assess the impact of anthropogenic pollution on isoprene-derived SOA formation. Results of this study reveal that isoprene-derived SOA tracers contribute a substantial mass fraction of organic matter (OM ( ∼  7 to  ∼  20 %. Isoprene-derived SOA tracers correlated with sulfate (SO42− (r2 = 0.34, n = 117 but not with NOx. Moderate correlations between methacrylic acid epoxide and hydroxymethyl-methyl-α-lactone (together abbreviated MAE/HMML-derived SOA tracers with nitrate radical production (P[NO3] (r2 = 0.57, n = 40 were observed during nighttime, suggesting a

  1. Exposure of BALB/c mice to diesel engine exhaust origin secondary organic aer-osol (DE-SOA during the developmental stages impairs the social behavior in adult life of the males

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    Tin-Tin eWin-Shwe

    2016-01-01

    Full Text Available Secondary organic aerosol (SOA is a component of particulate matter (PM 2.5 and formed in the atmosphere by oxidation of volatile organic compounds. Recently, we have reported that inhalation exposure to diesel engine exhaust (DE originated SOA (DE-SOA affect novel object recognition ability and impair maternal behavior in adult mice. However, it is not clear whether early life exposure to SOA during the de-velopmental stages affect social behavior in adult life or not. In the present study, to investigate the effects of early life exposure to DE-SOA during the gestational and lactation stages on the social behavior in the adult life, BALB/c mice were exposed to clean air (control, DE, DE-SOA and gas without any particulate matter in the inhala-tion chambers from gestational day 14 to postnatal day 21 for 5 h a day and 5 days per week. Then adult mice were examined for changes in their social behavior at the age of 13 week by a sociability and social novelty preference, social interaction with a juvenile mouse and light-dark transition test, hypothalamic mRNA expression levels of social behavior-related genes, estrogen receptor-alpha and oxytocin receptor as well as of the oxidative stress marker gene, heme oxygenase (HO-1 by real-time RT-PCR method. In addition, hypothalamic level of neuronal excitatory marker, glutamate was determined by ELISA method. We observed that sociability and social novelty pref-erence as well as social interaction were remarkably impaired, expression levels of es-trogen receptor-alpha, oxytocin receptor mRNAs were significantly decreased, ex-pression levels of HO-1 mRNAs and glutamate levels were significantly increased in adult male mice exposed to DE-SOA compared to the control ones. Findings of this study indicate early life exposure of BALB/c mice to DE-SOA may affect their late-onset hypothalamic expression of social behavior related genes, trigger neurotoxi-city and impair social behavior in the males.

  2. Exposure of BALB/c Mice to Diesel Engine Exhaust Origin Secondary Organic Aerosol (DE-SOA) during the Developmental Stages Impairs the Social Behavior in Adult Life of the Males.

    Science.gov (United States)

    Win-Shwe, Tin-Tin; Kyi-Tha-Thu, Chaw; Moe, Yadanar; Fujitani, Yuji; Tsukahara, Shinji; Hirano, Seishiro

    2015-01-01

    Secondary organic aerosol (SOA) is a component of particulate matter (PM) 2.5 and formed in the atmosphere by oxidation of volatile organic compounds. Recently, we have reported that inhalation exposure to diesel engine exhaust (DE) originated SOA (DE-SOA) affect novel object recognition ability and impair maternal behavior in adult mice. However, it is not clear whether early life exposure to SOA during the developmental stages affect social behavior in adult life or not. In the present study, to investigate the effects of early life exposure to DE-SOA during the gestational and lactation stages on the social behavior in the adult life, BALB/c mice were exposed to clean air (control), DE, DE-SOA and gas without any PM in the inhalation chambers from gestational day 14 to postnatal day 21 for 5 h a day and 5 days per week. Then adult mice were examined for changes in their social behavior at the age of 13 week by a sociability and social novelty preference, social interaction with a juvenile mouse and light-dark transition test, hypothalamic mRNA expression levels of social behavior-related genes, estrogen receptor-alpha and oxytocin receptor as well as of the oxidative stress marker gene, heme oxygenase (HO)-1 by real-time RT-PCR method. In addition, hypothalamic level of neuronal excitatory marker, glutamate was determined by ELISA method. We observed that sociability and social novelty preference as well as social interaction were remarkably impaired, expression levels of estrogen receptor-alpha, oxytocin receptor mRNAs were significantly decreased, expression levels of HO-1 mRNAs and glutamate levels were significantly increased in adult male mice exposed to DE-SOA compared to the control ones. Findings of this study indicate early life exposure of BALB/c mice to DE-SOA may affect their late-onset hypothalamic expression of social behavior related genes, trigger neurotoxicity and impair social behavior in the males.

  3. Isomerization of Second-Generation Isoprene Peroxy Radicals: Epoxide Formation and Implications for Secondary Organic Aerosol Yields

    Energy Technology Data Exchange (ETDEWEB)

    D’Ambro, Emma L.; Møller, Kristian H.; Lopez-Hilfiker, Felipe D.; Schobesberger, Siegfried; Liu, Jiumeng; Shilling, John E.; Lee, Ben Hwan; Kjaergaard, Henrik G.; Thornton, Joel A.

    2017-04-11

    We report chamber measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation, where radical concentrations were systematically varied and the molecular composition of semi to low volatility gases and SOA were measured online. Using a detailed chemical mechanism, we find that to explain the behavior of low volatility products and SOA mass yields relative to input H2O2 concentrations, the second generation dihydroxy hydroperoxy peroxy radical (C5H11O6•) must undergo an intra-molecular H-shift with a net forward rate constant of order 0.1 s-1 or higher, consistent with quantum chemical calculations which suggest a net forward rate constant of 0.3-0.9 s-1. Furthermore, these calculations suggest the dominant product of this isomerization is a dihydroxy hydroperoxy epoxide (C5H10O5) which is expected to have a saturation vapor pressure ~2 orders of magnitude higher than the dihydroxy dihydroperoxide, ISOP(OOH)2 (C5H12O6), a major product of the peroxy radical reacting with HO2. These results provide strong constraints on the likely volatility distribution of isoprene oxidation products under atmospheric conditions and thus on the importance of non-reactive gas-particle partitioning of isoprene oxidation products as an SOA source.

  4. Effects of inorganic seeds on secondary organic aerosol formation from photochemical oxidation of acetone in a chamber

    Science.gov (United States)

    Ge, Shuangshuang; Xu, Yongfu; Jia, Long

    2017-12-01

    Photochemical oxidations of acetone were studied under different inorganic seed (NaCl, (NH4)2SO4 and NaNO3) conditions in a self-made chamber. The results show that no secondary organic aerosol (SOA) can be formed in the experiments either in the absence of artificially added seed particles or in the presence of solid status of the added particles. Liquid water content is the key factor for the formation of SOA in the experiments with seeds. The amount of SOA was only about 4-7 μg m-3 in the experiments with the initial acetone of ∼15 ppm under different seed conditions. The analysis of SOA compositions by Exactive-Orbitrap mass spectrometer equipped with electro-spray interface (ESI-MS) shows that chlorine-containing and sulfur-containing compounds were detected in SOA formed from the experiments with NaCl and (NH4)2SO4 seeds, respectively, which were not identified in SOA from those with NaNO3. The compositions of SOA were mainly esters, organonitrates, hydroperoxides, etc. It is concluded that inorganic seed particles participated into the formation of SOA. Acetone SOA was mainly formed in the aqueous phase in which dissolved SOA precursors underwent further oxidation reactions, esterification reactions and/or radical-radical reactions. Our experiments further demonstrate that low-molecular-weight VOCs, such as acetone, can form SOA under certain conditions in the atmosphere, although their contributions to SOA may not be large.

  5. Effect of particle water on ozone and secondary organic aerosol formation from benzene-NO2-NaCl irradiations

    Science.gov (United States)

    Wang, Yujie; Luo, Hao; Jia, Long; Ge, Shuangshuang

    2016-09-01

    Ozone (O3) and secondary organic aerosol (SOA) are important pollutants in the urban atmosphere. Benzene is one of the most important aromatic species in urban air, which could produce O3 and SOA in the presence of NOx (x = 1, 2) and UV light. A series of experiments was carried out to study the effect of particle water on O3 and SOA formation from benzene under various humid conditions in an indoor smog chamber. The results show that the peak O3 concentrations decreased with the increase of RH or the mass concentration of liquid NaCl particles. The peak O3 concentration reduced by 30% as RH increased from 9% to 87% with the similar initial concentrations of NaCl (about 46 μg m-3), and decreased by 10% as the initial NaCl concentrations increased from 36.0 μg m-3 to 152.1 μg m-3 at about 73% RH. The relationships between liquid water content (LWC) and O3 or SOA were investigated. The results show that LWC is the key factor that leads to an opposite effect on O3 and SOA formation from benzene. The peak O3 concentration exponentially decreased 37% as LWC0 increased from zero to 349.8 μg m-3. Heterogeneous reaction of dinitrogen pentoxide (N2O5) with particle water is the major reason for the decrease of O3. The yields of SOA increased from 5.2 to 10.5% as LWC0 increased from zero to 349.8 μg m-3. The relative intensities of bands Osbnd H, Cdbnd O, Csbnd OH and NO3- increased by 22.9, 6.8, 6.7 and 13.1 times respectively as compared with dry condition. Alcohols or hydrates are confirmed to be the major contributors to SOA with increasing LWC.

  6. Direct deposition of gas phase generated aerosol gold nanoparticles into biological fluids--corona formation and particle size shifts.

    Directory of Open Access Journals (Sweden)

    Christian R Svensson

    Full Text Available An ongoing discussion whether traditional toxicological methods are sufficient to evaluate the risks associated with nanoparticle inhalation has led to the emergence of Air-Liquid interface toxicology. As a step in this process, this study explores the evolution of particle characteristics as they move from the airborne state into physiological solution. Airborne gold nanoparticles (AuNP are generated using an evaporation-condensation technique. Spherical and agglomerate AuNPs are deposited into physiological solutions of increasing biological complexity. The AuNP size is characterized in air as mobility diameter and in liquid as hydrodynamic diameter. AuNP:Protein aggregation in physiological solutions is determined using dynamic light scattering, particle tracking analysis, and UV absorption spectroscopy. AuNPs deposited into homocysteine buffer form large gold-aggregates. Spherical AuNPs deposited in solutions of albumin were trapped at the Air-Liquid interface but was readily suspended in the solutions with a size close to that of the airborne particles, indicating that AuNP:Protein complex formation is promoted. Deposition into serum and lung fluid resulted in larger complexes, reflecting the formation of a more complex protein corona. UV absorption spectroscopy indicated no further aggregation of the AuNPs after deposition in solution. The corona of the deposited AuNPs shows differences compared to AuNPs generated in suspension. Deposition of AuNPs from the aerosol phase into biological fluids offers a method to study the protein corona formed, upon inhalation and deposition in the lungs in a more realistic way compared to particle liquid suspensions. This is important since the protein corona together with key particle properties (e.g. size, shape and surface reactivity to a large extent may determine the nanoparticle effects and possible translocation to other organs.

  7. Program and Poster Abstracts from the Workshop on the Formation and Growth of Atmospheric Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    McMurry, Peter H. [Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Mechanical Engineering; Kulmala, Markku [Univ. of Helsinki (Finland). Dept. of Physics. Division of Atmospheric Sciences

    2006-09-09

    DOE provided $11,000 to sponsor the Workshop on New Particle Formation in the Atmosphere, which was held at The Riverwood Inn and Conference Center near Minneapolis, MN from September 7 to 9, 2006. Recent work has shown that new particle formation is an important atmospheric process that must be better understood due to its impact on cloud cover and the Earth's radiation balance. The conference was an informal gathering of atmospheric and basic scientists with expertise pertinent to this topic. The workshop included discussions of: • atmospheric modeling; • computational chemistry pertinent to clustering; • ions and ion induced nucleation; • basic laboratory and theoretical studies of nucleation; • studies on neutral molecular clusters; • interactions of organic compounds and sulfuric acid; • composition of freshly nucleated particles. Fifty six scientists attended the conference. They included 27 senior scientists, 9 younger independent scientists (assistant professor or young associate professor level), 7 postdocs, 13 graduate students, 10 women, 35 North Americans (34 from the U.S.), 1 Asian, and 20 Europeans. This was an excellent informal workshop on an important topic. An effort was made to include individuals from communities that do not regularly interact. A number of participants have provided informal feedback indicating that the workshop led to research ideas and possible future collaborations. This document includes abstracts from this workshop.

  8. Micro-physics of aircraft-generated aerosols and their potential impact on heterogeneous plume chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Kaercher, B.; Luo, B.P. [Muenchen Univ., Freising (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung

    1997-12-31

    Answers are attempted to give to open questions concerning physico-chemical processes in near-field aircraft plumes, with emphasis on their potential impact on subsequent heterogeneous chemistry. Research issues concerning the nucleation of aerosols and their interactions among themselves and with exhaust gases are summarized. Microphysical properties of contrail ice particles, formation of liquid ternary mixtures, and nucleation of nitric acid trihydrate particles in contrails are examined and possible implications for heterogeneous plume chemistry are discussed. (author) 19 refs.

  9. Secondary organic aerosol formation from photo-oxidation of toluene with NOx and SO2: Chamber simulation with purified air versus urban ambient air as matrix

    Science.gov (United States)

    Deng, Wei; Liu, Tengyu; Zhang, Yanli; Situ, Shuping; Hu, Qihou; He, Quanfu; Zhang, Zhou; Lü, Sujun; Bi, Xinhui; Wang, Xuemei; Boreave, Antoinette; George, Christian; Ding, Xiang; Wang, Xinming

    2017-02-01

    Chamber studies on the formation of secondary aerosols are mostly performed with purified air as matrix, it is of wide concern in what extent they might be different from the situations in ambient air, where a variety of gaseous and particulate components preexist. Here we compared the photo-oxidation of "toluene + NOx + SO2" combinations in a smog chamber in real urban ambient air matrix with that in purified air matrix. The secondary organic aerosols (SOA) mass concentrations and yields from toluene in the ambient air matrix, after subtracted ambient air background primary and secondary organic aerosols, were 9.0-34.0 and 5.6-12.9 times, respectively, greater than those in purified air matrix. Both homogeneous and heterogeneous oxidation of SO2 were enhanced in ambient air matrix experiments with observed 2.0-7.5 times higher SO2 degradation rates and 2.6-6.8 times faster sulfate formation than that in purified air matrix, resulting in higher in-situ particle acidity and consequently promoting acid-catalyzed SOA formation. In the ambient air experiments although averaged OH radical levels were elevated probably due to heterogeneous formation of OH on particle surface and/or ozonolysis of alkenes, non-OH oxidation pathways of SO2 became even more dominating. Under the same organic aerosol mass concentration, the SOA yields of toluene in purified air matrix experiments matched very well with the two-product model curve by Ng et al. (2007), yet the yields in ambient air on average was over two times larger. The results however were much near the best fit curve by Hildebrandt et al. (2009) with the volatility basis set (VBS) approach.

  10. Aqueous-phase mechanism for secondary organic aerosol formation from isoprene: application to the southeast United States and co-benefit of SO2 emission controls

    Directory of Open Access Journals (Sweden)

    E. A. Marais

    2016-02-01

    Full Text Available Isoprene emitted by vegetation is an important precursor of secondary organic aerosol (SOA, but the mechanism and yields are uncertain. Aerosol is prevailingly aqueous under the humid conditions typical of isoprene-emitting regions. Here we develop an aqueous-phase mechanism for isoprene SOA formation coupled to a detailed gas-phase isoprene oxidation scheme. The mechanism is based on aerosol reactive uptake coefficients (γ for water-soluble isoprene oxidation products, including sensitivity to aerosol acidity and nucleophile concentrations. We apply this mechanism to simulation of aircraft (SEAC4RS and ground-based (SOAS observations over the southeast US in summer 2013 using the GEOS-Chem chemical transport model. Emissions of nitrogen oxides (NOx  ≡  NO + NO2 over the southeast US are such that the peroxy radicals produced from isoprene oxidation (ISOPO2 react significantly with both NO (high-NOx pathway and HO2 (low-NOx pathway, leading to different suites of isoprene SOA precursors. We find a mean SOA mass yield of 3.3 % from isoprene oxidation, consistent with the observed relationship of total fine organic aerosol (OA and formaldehyde (a product of isoprene oxidation. Isoprene SOA production is mainly contributed by two immediate gas-phase precursors, isoprene epoxydiols (IEPOX, 58 % of isoprene SOA from the low-NOx pathway and glyoxal (28 % from both low- and high-NOx pathways. This speciation is consistent with observations of IEPOX SOA from SOAS and SEAC4RS. Observations show a strong relationship between IEPOX SOA and sulfate aerosol that we explain as due to the effect of sulfate on aerosol acidity and volume. Isoprene SOA concentrations increase as NOx emissions decrease (favoring the low-NOx pathway for isoprene oxidation, but decrease more strongly as SO2 emissions decrease (due to the effect of sulfate on aerosol acidity and volume. The US Environmental Protection Agency (EPA projects 2013–2025 decreases in

  11. Particulate matter (PM) episodes at a suburban site in Hong Kong: evolution of PM characteristics and role of photochemistry in secondary aerosol formation

    Science.gov (United States)

    Qin, Yi Ming; Jie Li, Yong; Wang, Hao; Lee, Berto Paul Yok Long; Huang, Dan Dan; Keung Chan, Chak

    2016-11-01

    Episodes with high concentrations of particulate matter (PM) across the seasons were investigated during four 1-month campaigns at a suburban site in Hong Kong. High-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) measurements revealed that both regional transport and secondary formation contributed to high PM levels during the episodes at this site. Based on distinct meteorological conditions, episodes were categorized into three types: liquid water content (LWC), solar irradiance (IR), and long-range transport (LRT). Despite the difference in meteorological conditions, all episodes were characterized by a high fraction of sulfate (45-56 %) and organics (23-34 %). However, aerosols in LWC episodes were less aged, consisting of the lowest fraction of secondary organic aerosol (SOA) and the highest fraction of small particles. Large particles mixed internally while freshly formed small particles mixed externally in LWC episodes. Aerosols in LRT episodes, by contrast, were the most aged and consisted of the highest proportion of low-volatility oxygenated organic aerosol (LVOOA) and the lowest proportion of small particles. Both small and large particles mixed externally in LRT episodes. The highest proportion of semi-volatile oxygenated organic aerosol (SVOOA) and a medium proportion of small particles were observed in IR episodes. Both small and large particles were likely externally mixed during IR episodes. Furthermore, aerosols experienced the most dramatic size increase and diurnal variation, with a time lag between SVOOA and LVOOA and a gradual increase in carbon oxidation state (OSc ≈ 2 × O : C - H : C). Five out of 10 episodes were of the IR type, further reflecting the importance of this type of episode. The evolution of aerosol components in one particular episode of the IR type, which exhibited a clear land-sea breeze pattern, was examined in detail. Sulfate and SOA due to photochemical aging were very efficiently produced during the

  12. Seawater Dynamic Surface Tension: A case for bubble sorption as a primary mechanism in the formation of particulate marine organic aerosol (Invited)

    Science.gov (United States)

    Long, M. S.; Keene, W. C.; Henderson, G. R.; Kieber, D. J.; Maben, J. R.; Kinsey, J. D.; Quinn, P.; Bates, T. S.

    2013-12-01

    Much attention has been given to size-resolved particulate fluxes of marine organic material (OM) into the atmosphere. Observations of ambient and artificially generated aerosol produced in seawater consistently show a size-dependent enrichment of OM relative to background seawater concentrations. Proposed mechanisms leading to particle enrichment have generally focused on the formation and scavenging of micelle-like exopolymers and interactions of bubble surfaces at the sea-surface microlayer. Previous work hypothesized that organic enrichment is controlled by adsorption processes at bubble surfaces within wave-generated bubble plumes. Here we present observations of dynamic surface tension of seawater supporting this hypothesis. In seawater samples taken from the surface and at 5m depth, interfacial surface tension was depressed by up to several dyn/cm within 0.2 to 0.5 s. These observations demonstrate that bubble surface area was saturated by surfactant material very quickly relative to bubble lifetimes beneath breaking waves. Dynamic surface tension profiles also show multiple surfactants competing for available surface area. Corresponding observed aerosol OM enrichment factors were similar. This supports several conclusions: 1) Biological activity does not directly control OM enrichments. 2) The process of particulate OM formation is surface-area limited, rather than OM limited. 3) There are multiple surfactants in seawater capable of saturating bubble surfaces. These results, when combined with theory of bubble-film drainage and rupture suggest that bubble adsorption processes alone are capable of reproducing observed OM enrichments of marine aerosol. We hypothesize that the formation of amphiphillic surfactant layers on bubble surfaces would behave as a Stern layer capable of binding divalent cations, which may account for enrichments of Mg2+ and Ca2+ reported in some samples of primary marine aerosol.

  13. Impacts of Aerosols on UV Radiation and Ozone Formation and Analysis of Chemical Processes using a 3-D Chemical Transport Model in the Mexico City Metropolitan Area

    Science.gov (United States)

    Lei, W.; de Foy, B.; Volkamer, R.; Frey, S.; Molina, L. T.; Molina, M. J.

    2004-12-01

    The influence of aerosols on UV radiation is investigated by calculating the photolysis rate coefficients using the NCAR tropospheric ultraviolet and visible radiation model (TUV) constrained by aerosol extinction vertical profiles as well as other optical properties provided by Lidar and spectroradiometer observations. The calculated photolysis rates are validated by measured values for key species. The computed photolysis rates are incorporated into a 3-D chemical transport model CAMx (Environ) to assess the impacts of aerosols on O3 formation in the Mexico City Metropolitan Area. Understanding the chemical processes governing O3 formation and the sensitivity of O3 to emissions reductions is a key issue in formulating an effective O3 control strategy . We performed episodic simulations using the CAMx model and analyzed the chemical processes in terms of the budgets of free radicals, NOy and O3, and O3 production rate and efficiency, which gave us useful information about important chemical processes controlling O3 production and sensitivity to precursor reductions. We analyzed as well the effects of chemistry, transport and deposition on O3 production in Mexico City.

  14. Observation of aerosol size distribution and new particle formation at a coastal city in the Yangtze River Delta, China.

    Science.gov (United States)

    Shen, Lijuan; Wang, Honglei; Lü, Sheng; Li, Li; Yuan, Jing; Zhang, Xiaohan; Tian, Xudong; Tang, Qian

    2016-09-15

    Aerosol number size distribution in the range of 10nm-10μm, trace gases (O3, CO, SO2 and NO2), particular matter (PM: PM2.5 and PM10) and meteorological elements were measured from the 1st to the 31st of May, 2015, in the coastal city of Jiaxing in the Yangtze River Delta (YRD). The average number concentration and surface area concentration were 19,639cm(-3) and 427μm(2)cm(-3) during the observation period. The different mode particle concentrations ranked in the order of Aitken mode (12,361cm(-3))>nucleation (4926.7cm(-3))>accumulation (2349.3cm(-3))>coarse mode (1.7cm(-3)). The average concentrations of CO, SO2, NO2, O3, PM2.5 and PM10 were 0.545mgm(-3), 14.7, 35.1, 89.8, 43.5 and 64.6μgm(-3), respectively. Eight precipitation processes and 15 new particle formation (NPF) events (3 NPF events occurred on a rainy day) were observed. Results show that the precipitation process had greater scavenging effects on particles smaller than 120nm and larger than 2μm. The spectral distributions of number concentrations were unimodal at different weather conditions, with peaks at 20nm, 40-60nm, 50-80nm on NPF days, rainy days and normal days. During the NPF events, the formation rate (FR), growth rate (GR), condensational sink (CS), vapor source rate (Q) and condensing vapor concentration (C) were in the range of 4.0-17.0cm(-3)s(-1), 2.2-15.7nmh(-1), 1.5-5.8×10(-2)s(-1), 0.5-7.7×10(6)cm(-3)s(-1) and 3.0-21.5×10(7)cm(-3), with mean values of 9.6cm(-3)s(-1), 6.8nmh(-1), 3.4×10(-2)s(-1), 3.3×10(6)cm(-3)s(-1) and 9.4×10(7)cm(-3), respectively. NPF events normally occurred under clean atmospheric conditions with low PM concentrations but high levels of trace gases. It was also found that SO2 plays an important role in NPF and growth in Jiaxing. Copyright © 2016 Elsevier B.V. All rights reserved.

  15. Assessing the Dynamics of Organic Aerosols over the North Atlantic Ocean.

    Science.gov (United States)

    Kasparian, Jérôme; Hassler, Christel; Ibelings, Bas; Berti, Nicolas; Bigorre, Sébastien; Djambazova, Violeta; Gascon-Diez, Elena; Giuliani, Grégory; Houlmann, Raphaël; Kiselev, Denis; de Laborie, Pierric; Le, Anh-Dao; Magouroux, Thibaud; Neri, Tristan; Palomino, Daniel; Pfändler, Stéfanie; Ray, Nicolas; Sousa, Gustavo; Staedler, Davide; Tettamanti, Federico; Wolf, Jean-Pierre; Beniston, Martin

    2017-03-31

    The influence of aerosols on climate is highly dependent on the particle size distribution, concentration, and composition. In particular, the latter influences their ability to act as cloud condensation nuclei, whereby they impact cloud coverage and precipitation. Here, we simultaneously measured the concentration of aerosols from sea spray over the North Atlantic on board the exhaust-free solar-powered vessel "PlanetSolar", and the sea surface physico-chemical parameters. We identified organic-bearing particles based on individual particle fluorescence spectra. Organic-bearing aerosols display specific spatio-temporal distributions as compared to total aerosols. We propose an empirical parameterization of the organic-bearing particle concentration, with a dependence on water salinity and sea-surface temperature only. We also show that a very rich mixture of organic aerosols is emitted from the sea surface. Such data will certainly contribute to providing further insight into the influence of aerosols on cloud formation, and be used as input for the improved modeling of aerosols and their role in global climate processes.

  16. Modeling the formation and aging of secondary organic aerosols in Los Angeles during CalNex 2010

    Science.gov (United States)

    Hayes, P. L.; Carlton, A. G.; Baker, K. R.; Ahmadov, R.; Washenfelder, R. A.; Alvarez, S.; Rappengluck, B.; Gilman, J. B.; Kuster, W. C.; de Gouw, J. A.; Zotter, P.; Prevot, A. S. H.; Szidat, S.; Kleindienst, T. E.; Offenberg, J. H.; Ma, P. K.; Jimenez, J. L.

    2015-05-01

    Four different literature parameterizations for the formation and evolution of urban secondary organic aerosol (SOA) frequently used in 3-D models are evaluated using a 0-D box model representing the Los Angeles metropolitan region during the California Research at the Nexus of Air Quality and Climate Change (CalNex) 2010 campaign. We constrain the model predictions with measurements from several platforms and compare predictions with particle- and gas-phase observations from the CalNex Pasadena ground site. That site provides a unique opportunity to study aerosol formation close to anthropogenic emission sources with limited recirculation. The model SOA that formed only from the oxidation of VOCs (V-SOA) is insufficient to explain the observed SOA concentrations, even when using SOA parameterizations with multi-generation oxidation that produce much higher yields than have been observed in chamber experiments, or when increasing yields to their upper limit estimates accounting for recently reported losses of vapors to chamber walls. The Community Multiscale Air Quality (WRF-CMAQ) model (version 5.0.1) provides excellent predictions of secondary inorganic particle species but underestimates the observed SOA mass by a factor of 25 when an older VOC-only parameterization is used, which is consistent with many previous model-measurement comparisons for pre-2007 anthropogenic SOA modules in urban areas. Including SOA from primary semi-volatile and intermediate-volatility organic compounds (P-S/IVOCs) following the parameterizations of Robinson et al. (2007), Grieshop et al. (2009), or Pye and Seinfeld (2010) improves model-measurement agreement for mass concentration. The results from the three parameterizations show large differences (e.g., a factor of 3 in SOA mass) and are not well constrained, underscoring the current uncertainties in this area. Our results strongly suggest that other precursors besides VOCs, such as P-S/IVOCs, are needed to explain the observed

  17. Abundance of fluorescent biological aerosol particles at temperatures conducive to the formation of mixed-phase and cirrus clouds

    Energy Technology Data Exchange (ETDEWEB)

    Twohy, Cynthia H.; McMeeking, Gavin R.; DeMott, Paul J.; McCluskey, Christina S.; Hill, Thomas C. J.; Burrows, Susannah M.; Kulkarni, Gourihar R.; Tanarhte, Meryem; Kafle, Durga N.; Toohey, Darin W.

    2016-01-01

    Some types of biological particles are known to nucleate ice at warmer temperatures than mineral dust, with the potential to influence cloud microphysical properties and climate. However, the prevalence of these particle types above the atmospheric boundary layer is not well known. Many types of biological particles fluoresce when exposed to ultraviolet light, and the Wideband Integrated Bioaerosol Sensor takes advantage of this characteristic to perform real-time measurements of fluorescent biological aerosol particles (FBAPs). This instrument was flown on the National Center for Atmospheric Research Gulfstream V aircraft to measure concentrations of fluorescent biological particles from different potential sources and at various altitudes over the US western plains in early autumn. Clear-air number concentrations of FBAPs between 0.8 and 12 µm diameter usually decreased with height and generally were about 10–100 L-1 in the continental boundary layer but always much lower at temperatures colder than 255 K in the free troposphere. At intermediate temperatures where biological ice-nucleating particles may influence mixed-phase cloud formation (255 K ≤ T ≤ 270 K), concentrations of fluorescent particles were the most variable and were occasionally near boundary-layer concentrations. Predicted vertical distributions of ice-nucleating particle concentrations based on FBAP measurements in this temperature regime sometimes reached typical concentrations of primary ice in clouds but were often much lower. If convection was assumed to lift boundary-layer FBAPs without losses to the free troposphere, better agreement between predicted ice-nucleating particle concentrations and typical ice crystal concentrations was achieved. Ice-nucleating particle concentrations were also measured during one flight and showed a decrease with height, and concentrations were consistent with a relationship to FBAPs established previously at the forested surface

  18. Compact Layers of Hybrid Halide Perovskites Fabricated via the Aerosol Deposition Process—Uncoupling Material Synthesis and Layer Formation

    Directory of Open Access Journals (Sweden)

    Fabian Panzer

    2016-04-01

    Full Text Available We present the successful fabrication of CH3NH3PbI3 perovskite layers by the aerosol deposition method (ADM. The layers show high structural purity and compactness, thus making them suitable for application in perovskite-based optoelectronic devices. By using the aerosol deposition method we are able to decouple material synthesis from layer processing. Our results therefore allow for enhanced and easy control over the fabrication of perovskite-based devices, further paving the way for their commercialization.

  19. Using GC×GC-ToF-MS to characterise SVOC from diesel exhaust emissions

    Science.gov (United States)

    Alam, M. S.; Ramadhas, A. S.; Stark, C. P.; Liu, D.; Xu, H.; Harrison, R. M.

    2014-12-01

    Despite intensive research over the last 20 years, a number of major research questions remain concerning the sources and properties of road traffic-generated particulate matter. There are major knowledge gaps concerning the composition of primary vehicle exhaust aerosol, and its contribution to secondary organic aerosol (SOA) formation. These uncertainties relate especially to the semi-volatile component of the particles. Semi-Volatile Organic Compounds (SVOC) are compounds which partition directly between the gas and aerosol phases under ambient conditions, and include compounds with saturation concentrations roughly between 0.1 and 104 μg m-3. The SVOC in engine exhaust are typically hydrocarbons in the C15-C35 range. They are largely uncharacterised, other than the n-alkanes, because they are unresolved by traditional gas chromatography and form a large hump in the chromatogram referred to as Unresolved Complex Mixture (UCM). In this study, samples were collected from the exhaust of a diesel engine with and without abatement devices fitted. Engine exhaust was diluted with air and collected using both filter and impaction (MOUDI), to resolve total mass and size resolved mass respectively. Particle size distribution was evaluated by sampling simultaneously with a Scanning Mobility Particle Sizer (SMPS). 2D Gas-Chromatography Time-of-Flight Mass-Spectrometry (GC×GC-ToF-MS) was exploited to characterise and quantify the composition of SVOC from the exhaust emission. The SVOC was observed to contain predominantly n-alkanes, alkyl-cyclohexanes and aromatics; similar to both fresh lubricating oil and fuel. Preliminary results indicate that the contribution of diesel fuel to the exhaust SVOC composition is dominant at high speeds, and a more pronounced contribution from lubricating oil is observed at low speeds. Differences were also observed in the SVOC composition when using different fuel types, engine lubricants, starting temperatures and collecting samples with

  20. The 2005 catastrophic acid crater lake drainage, lahar, and acidic aerosol formation at Mount Chiginagak volcano, Alaska, USA: Field observations and preliminary water and vegetation chemistry results

    Science.gov (United States)

    Schaefer, J.R.; Scott, W.E.; Evans, William C.; Jorgenson, J.; McGimsey, R.G.; Wang, B.

    2008-01-01

    A mass of snow and ice 400-m-wide and 105-m-thick began melting in the summit crater of Mount Chiginagak volcano sometime between November 2004 and early May 2005, presumably owing to increased heat flux from the hydrothermal system, or possibly from magma intrusion and degassing. In early May 2005, an estimated 3.8??106 m3 of sulfurous, clay-rich debris and acidic water, with an accompanying acidic aerosol component, exited the crater through a tunnel at the base of a glacier that breaches the south crater rim. Over 27 km downstream, the acidic waters of the flood inundated an important salmon spawning drainage, acidifying Mother Goose Lake from surface to depth (approximately 0.5 km3 in volume at a pH of 2.9 to 3.1), killing all aquatic life, and preventing the annual salmon run. Over 2 months later, crater lake water sampled 8 km downstream of the outlet after considerable dilution from glacial meltwater was a weak sulfuric acid solution (pH = 3.2, SO4 = 504 mg/L, Cl = 53.6 mg/L, and F = 7.92 mg/L). The acid flood waters caused severe vegetation damage, including plant death and leaf kill along the flood path. The crater lake drainage was accompanied by an ambioructic flow of acidic aerosols that followed the flood path, contributing to defoliation and necrotic leaf damage to vegetation in a 29 km2 area along and above affected streams, in areas to heights of over 150 m above stream level. Moss species killed in the event contained high levels of sulfur, indicating extremely elevated atmospheric sulfurcontent. The most abundant airborne phytotoxic constituent was likely sulfuric acid aerosols that were generated during the catastrophic partial crater lake drainage event. Two mechanisms of acidic aerosol formation are proposed: (1) generation of aerosol mist through turbulent flow of acidic water and (2) catastrophic gas exsolution. This previously undocumented phenomenon of simultaneous vegetationdamaging acidic aerosols accompanying drainage of an acidic crater

  1. Size Distributions and Formation Pathways of Organic and Inorganic Constituents in Spring Aerosols from Okinawa Island in the Western North Pacific Rim: An Outflow Region of Asian Dusts

    Science.gov (United States)

    Deshmukh, D. K.; Lazaar, M.; Kawamura, K.; Kunwar, B.; Tachibana, E.; Boreddy, S. K. R.

    2015-12-01

    Size-segregated aerosols (9-stages) were collected at Okinawa Island in the western North Pacific Rim in spring 2008. The samples were analyzed for diacids (C2-C12), ω-oxoacids (ωC2-ωC9), a-dicarbonyls (C2-C3), organic carbon (OC), water-soluble OC (WSOC) and major ions to understand the sources and atmospheric processes in the outflow region of Asian pollutants. The molecular distribution of diacids showed the predominance of oxalic acid (C2) followed by malonic and succinic acids in all the size-segregated aerosols. ω-Oxoacids showed the predominance of glyoxylic acid (ωC2) whereas glyoxal (Gly) was more abundant than methylglyoxal in all the sizes. The abundant presence of sulfate as well as phthalic and adipic acids in Okinawa aerosols suggested a significant contribution of anthropogenic sources in East Asia via long-range atmospheric transport. Diacids (C2-C5), ωC2 and Gly as well as WSOC and OC peaked at 0.65-1.1 µm in fine mode whereas azelaic (C9) and 9-oxononanoic (ωC9) acids peaked at 3.3-4.7 µm in coarse mode. Sulfate and ammonium are enriched in fine mode whereas sodium and chloride are in coarse mode. An important mechanism for the formation of these organic species in Okinawa aerosols is probably gas phase oxidation of VOCs and subsequent in-cloud processing during long-range transport. Their characteristics size distribution implies that fine particles enriched with these organic and inorganic species could act as CCN to develop the cloud cover over the western North Pacific. The major peak of C9 and ωC9 on coarse mode suggest that they are produced by photooxidation of unsaturated fatty acids mainly derived from phytoplankton via heterogeneous reactions on sea spray particles. This study demonstrates that anthropogenic aerosols emitted from East Asia have significant influence on the compositions of organic and inorganic aerosols in the western North Pacific Rim.

  2. Modeling ozone and aerosol formation and transport in the pacific northwest with the community Multi-Scale Air Quality (CMAQ) modeling system.

    Science.gov (United States)

    O'Neill, Susan M; Lamb, Brian K; Chen, Jack; Claiborn, Candis; Finn, Dennis; Otterson, Sally; Figueroa, Cristiana; Bowman, Clint; Boyer, Mike; Wilson, Rob; Arnold, Jeff; Aalbers, Steven; Stocum, Jeffrey; Swab, Christopher; Stoll, Matt; Dubois, Mike; Anderson, Mary

    2006-02-15

    The Community Multi-Scale Air Quality (CMAQ) modeling system was used to investigate ozone and aerosol concentrations in the Pacific Northwest (PNW) during hot summertime conditions during July 1-15, 1996. Two emission inventories (El) were developed: emissions for the first El were based upon the National Emission Trend 1996 (NET96) database and the BEIS2 biogenic emission model, and emissions for the second El were developed through a "bottom up" approach that included biogenic emissions obtained from the GLOBEIS model. The two simulations showed that elevated PM2.5 concentrations occurred near and downwind of the Interstate-5 corridor along the foothills of the Cascade Mountains and in forested areas of central Idaho. The relative contributions of organic and inorganic aerosols varied by region, but generally organic aerosols constituted the largest fraction of PM2.5. In wilderness areas near the 1-5 corridor, organic carbon from anthropogenic sources contributed approximately 50% of the total organic carbon with the remainder from biogenic precursors, while in wilderness areas in Idaho, biogenic organic carbon accounted for 80% of the total organic aerosol. Regional analysis of the secondary organic aerosol formation in the Columbia River Gorge, Central Idaho, and the Olympics/Puget Sound showed that the production rate of secondary organic carbon depends on local terpene concentrations and the local oxidizing capacity of the atmosphere, which was strongly influenced by anthropogenic emissions. Comparison with observations from 12 IMPROVE sites and 21 ozone monitoring sites showed that results from the two El simulations generally bracketed the average observed PM parameters and that errors calculated for the model results were within acceptable bounds. Analysis across all statistical parameters indicated that the NW-AIRQUEST El solution performed better at predicting PM2.5, PM1, and beta(ext) even though organic carbon PM was over-predicted, and the NET96 El

  3. Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: evaluation of the volatility-basis-set approach within the CHIMERE model

    Directory of Open Access Journals (Sweden)

    Q. J. Zhang

    2013-06-01

    Full Text Available Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS is implemented into this model, taking into account the volatility of primary organic aerosol (POA and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization, to emission input data, and to simulated OH levels can be responsible for

  4. Effect of a gas-gas-heater on H2SO4 aerosol formation: implications for mist formation in amine based carbon capture

    NARCIS (Netherlands)

    Mertens, J.; Bruns, R.; Schallert, B.; Faniel, N.; Khakharia, P.M.; Albrecht, W.; Goetheer, E.L.V.; Blondeau, J.; Schaber, K.

    2015-01-01

    This study is to our knowledge the first to describe the effect of a Gas-Gas Heater (GGH) of a coal fired power plant's has on (i) the H2SO4 concentration and (ii) the particle/aerosol number concentration and particle size distribution present in the flue gas. In the absence of a GGH, homogenous

  5. Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN

    Directory of Open Access Journals (Sweden)

    P. Reutter

    2009-09-01

    Full Text Available We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm, we have calculated initial cloud droplet number concentrations (NCD for a wide range of updraft velocities (w=0.25–20 m s−1 and aerosol particle number concentrations (NCN=200–105 cm−3 at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN, we found three distinctly different regimes of CCN activation and cloud droplet formation:

    (1 An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10−3 m s−1 cm3, high maximum values of water vapour supersaturation (Smax>≈0.5%, and high activated fractions of aerosol particles (NCN/NCN>≈90%. In this regime NCD is directly proportional to NCN and practically independent of w.

    (2 An updraft-limited regime that is characterized by low w/NCN ratios (<≈10−4 m s−1 cm3, low maximum values of water vapour supersaturation (Smax<≈0.2%, and low activated fractions of aerosol particles (NCD/NCN<≈20%. In this regime NCD is directly proportional to w and practically independent of NCN.

    (3 An aerosol- and updraft-sensitive regime (transitional regime, which is characterized by parameter values in between

  6. The effect of mixing rates on the formation and growth of condensation aerosols in a model stagnation flow

    KAUST Repository

    Alshaarawi, Amjad

    2015-03-01

    A steady, laminar stagnation flow configuration is adopted to investigate numerically the interaction between condensing aerosol particles and gas-phase transport across a canonical mixing layer. The mixing rates are varied by adjusting the velocity and length scales of the stagnation flow parametrically. The effect of mixing rates on particle concentration, polydispersity, and mean droplet diameter is explored and discussed. This numerical study reveals a complex response of the aerosol to varying flow times. Depending on the flow time, the variation of the particle concentration in response to varying mixing rates falls into one of the two regimes. For fast mixing rates, the number density and volume fraction of the condensing particles increase with residence time (nucleation regime). On the contrary, for low mixing rates, number density decreases with residence time and volume fraction reaches a plateau (condensation regime). It is shown that vapor scavenging by the aerosol phase is key to explaining the transition between these two regimes. The results reported here are general and illustrate genuine features of the evolution of aerosols forming by condensation of supersaturated vapor from heat and mass transport across mixing layers.

  7. Formation of brown carbon via reactions of ammonia with secondary organic aerosols from biogenic and anthropogenic precursors

    Science.gov (United States)

    Updyke, Katelyn M.; Nguyen, Tran B.; Nizkorodov, Sergey A.

    2012-12-01

    Filter samples of secondary organic aerosols (SOA) generated from the ozone (O3)- and hydroxyl radical (OH)-initiated oxidation of various biogenic (isoprene, α-pinene, limonene, α-cedrene, α-humulene, farnesene, pine leaf essential oils, cedar leaf essential oils) and anthropogenic (tetradecane, 1,3,5-trimethylbenzene, naphthalene) precursors were exposed to humid air containing approximately 100 ppb of gaseous ammonia (NH3). Reactions of SOA compounds with NH3 resulted in production of light-absorbing "brown carbon" compounds, with the extent of browning ranging from no observable change (isoprene SOA) to visible change in color (limonene SOA). The aqueous phase reactions with dissolved ammonium (NH4+) salts, such as ammonium sulfate, were equally efficient in producing brown carbon. Wavelength-dependent mass absorption coefficients (MAC) of the aged SOA were quantified by extracting known amounts of SOA material in methanol and recording its UV/Vis absorption spectra. For a given precursor, the OH-generated SOA had systematically lower MAC compared to the O3-generated SOA. The highest MAC values, for brown carbon from SOA resulting from O3 oxidation of limonene and sesquiterpenes, were comparable to MAC values for biomass burning particles but considerably smaller than MAC values for black carbon aerosols. The NH3/NH4+ + SOA brown carbon aerosol may contribute to aerosol optical density in regions with elevated concentrations of NH3 or ammonium sulfate and high photochemical activity.

  8. The relative importance of competing pathways for the formation of high-molecular-weight peroxides in the ozonolysis of organic aerosol particles

    Directory of Open Access Journals (Sweden)

    M. Mochida

    2006-01-01

    Full Text Available High-molecular-weight (HMW organic compounds are an important component of atmospheric particles, although their origins, possibly including in situ formation pathways, remain incompletely understood. This study investigates the formation of HMW organic peroxides through reactions involving stabilized Criegee intermediates (SCI's. The model system is methyl oleate (MO mixed with dioctyl adipate (DOA and myristic acid (MA in submicron aerosol particles, and Criegee intermediates are formed by the ozonolysis of the double bond in methyl oleate. An aerosol flow tube coupled to a quadrupole aerosol mass spectrometer (AMS is employed to determine the relative importance of different HMW organic peroxides following the ozonolysis of different mixing mole fractions of MO in DOA and MA. Possible peroxide products include secondary ozonides (SOZ's, α-acyloxyalkyl hydroperoxides and α-acyloxyalkyl alkyl peroxides (αAAHP-type compounds, diperoxides, and monoperoxide oligomers. Of these, the AMS data identify two SOZ's as major HMW products in the ozonolysis of pure methyl oleate as well as in an inert matrix of DOA to as low as 0.04 mole fraction MO. In comparison, in mixed particles of MO and MA, αAAHP-type compounds form in high yields for MO mole fractions of 0.5 or less, suggesting that SCI's efficiently attack the carboxylic acid group of myristic acid. The reactions of SCI's with carboxylic acid groups to form αAAHP-type compounds therefore compete with those of SCI's with aldehydes to form SOZ's, provided that both types of functionalities are present at significant concentrations. The results therefore suggest that SCI's in atmospheric particles contribute to the transformation of carboxylic acids and other protic groups into HMW organic peroxides.

  9. A dual-chamber method for quantifying the effects of atmospheric perturbations on secondary organic aerosol formation from biomass burning emissions

    Science.gov (United States)

    Tkacik, Daniel S.; Robinson, Ellis S.; Ahern, Adam; Saleh, Rawad; Stockwell, Chelsea; Veres, Patrick; Simpson, Isobel J.; Meinardi, Simone; Blake, Donald R.; Yokelson, Robert J.; Presto, Albert A.; Sullivan, Ryan C.; Donahue, Neil M.; Robinson, Allen L.

    2017-06-01

    Biomass burning (BB) is a major source of atmospheric pollutants. Field and laboratory studies indicate that secondary organic aerosol (SOA) formation from BB emissions is highly variable. We investigated sources of this variability using a novel dual-smog-chamber method that directly compares the SOA formation from the same BB emissions under two different atmospheric conditions. During each experiment, we filled two identical Teflon smog chambers simultaneously with BB emissions from the same fire. We then perturbed the smoke with UV lights, UV lights plus nitrous acid (HONO), or dark ozone in one or both chambers. These perturbations caused SOA formation in nearly every experiment with an average organic aerosol (OA) mass enhancement ratio of 1.78 ± 0.91 (mean ± 1σ). However, the effects of the perturbations were highly variable ranging with OA mass enhancement ratios ranging from 0.7 (30% loss of OA mass) to 4.4 across the set of perturbation experiments. There was no apparent relationship between OA enhancement and perturbation type, fuel type, and modified combustion efficiency. To better isolate the effects of different perturbations, we report dual-chamber enhancement (DUCE), which is the quantity of the effects of a perturbation relative to a reference condition. DUCE values were also highly variable, even for the same perturbation and fuel type. Gas measurements indicate substantial burn-to-burn variability in the magnitude and composition of SOA precursor emissions, even in repeated burns of the same fuel under nominally identical conditions. Therefore, the effects of different atmospheric perturbations on SOA formation from BB emissions appear to be less important than burn-to-burn variability.

  10. Marine Aerosols and Clouds.

    Science.gov (United States)

    Brooks, Sarah D; Thornton, Daniel C O

    2017-10-13

    The role of marine bioaerosols in cloud formation and climate is currently so uncertain that even the sign of the climate forcing is unclear. Marine aerosols form through direct emissions and through the conversion of gasphase emissions to aerosols in the atmosphere. The composition and size of aerosols determine how effective they are in catalyzing the formation of water droplets and ice crystals in clouds by acting as cloud condensation nuclei and ice nucleating particles, respectively. Marine organic aerosols may be sourced both from recent regional phytoplankton blooms that add labile organic matter to the surface ocean and from long-term global processes, such as the upwelling of old refractory dissolved organic matter from the deep ocean. Understanding the formation of marine aerosols and their propensity to catalyze cloud formation processes are challenges that must be addressed given the major uncertainties associated with aerosols in climate models. Expected final online publication date for the Annual Review of Marine Science Volume 10 is January 3, 2018. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.

  11. Heavy Ion Formation in Titan's Ionosphere: Magnetospheric Introduction of Free Oxygen and a Source of Titan's Aerosols?

    Science.gov (United States)

    Sittler, E. C., Jr.; Ali, A.; Cooper, J. F.; Hartle, R. E.; Johnson, R. E.; Coates, A. J.; Young, D. T.

    2009-01-01

    Discovery by Cassini's plasma instrument of heavy positive and negative ions within Titan's upper atmosphere and ionosphere has advanced our understanding of ion neutral chemistry within Titan's upper atmosphere, primarily composed of molecular nitrogen, with approx.2.5% methane. The external energy flux transforms Titan's upper atmosphere and ionosphere into a medium rich in complex hydrocarbons, nitriles and haze particles extending from the surface to 1200 km altitudes. The energy sources are solar UV, solar X-rays, Saturn's magnetospheric ions and electrons, solar wind and shocked magnetosheath ions and electrons, galactic cosmic rays (CCR) and the ablation of incident meteoritic dust from Enceladus' E-ring and interplanetary medium. Here it is proposed that the heavy atmospheric ions detected in situ by Cassini for heights >950 km, are the likely seed particles for aerosols detected by the Huygens probe for altitudes ions. The latter provide keV oxygen, hydroxyl and water ions to Titan's upper atmosphere and can become trapped within the fullerene molecules and ions. Pickup keV N(2+), N(+) and CH(4+) can also be implanted inside of fullerenes. Attachment of oxygen ions to PAH molecules is uncertain, but following thermalization O(+) can interact with abundant CH4 contributing to the CO and CO2 observed in Titan's atmosphere. If an exogenic keV O(+) ion is implanted into the haze particles, it could become free oxygen within those aerosols that eventually fall onto Titan's surface. The process of freeing oxygen within aerosols could be driven by cosmic ray interactions with aerosols at all heights. This process could drive pre-biotic chemistry within the descending aerosols. Cosmic ray interactions with grains at the surface, including water frost depositing on grains from cryovolcanism, would further add to abundance of trapped free oxygen. Pre-biotic chemistry could arise within surface microcosms of the composite organic-ice grains, in part driven by free

  12. Exhaustion from prolonged gambling

    Directory of Open Access Journals (Sweden)

    Fatimah Lateef

    2013-01-01

    Full Text Available Complaints of fatigue and physical exhaustion are frequently seen in the acute medical setting, especially amongst athletes, army recruits and persons involved in strenuous and exertional physical activities. Stress-induced exhaustion, on the other hand, is less often seen, but can present with very similar symptoms to physical exhaustion. Recently, three patients were seen at the Department of Emergency Medicine, presenting with exhaustion from prolonged involvement in gambling activities. The cases serve to highlight some of the physical consequences of prolonged gambling.

  13. Online characterization of regulated and unregulated gaseous and particulate exhaust emissions from two-stroke mopeds: a chemometric approach.

    Science.gov (United States)

    Clairotte, M; Adam, T W; Chirico, R; Giechaskiel, B; Manfredi, U; Elsasser, M; Sklorz, M; DeCarlo, P F; Heringa, M F; Zimmermann, R; Martini, G; Krasenbrink, A; Vicet, A; Tournié, E; Prévôt, A S H; Astorga, C

    2012-03-02

    Two-stroke mopeds are a popular and convenient mean of transport in particular in the highly populated cities. These vehicles can emit potentially toxic gaseous and aerosol pollutants due to their engine technology. The legislative measurements of moped emissions are based on offline methods; however, the online characterization of gas and particulate phases offers great possibilities to understand aerosol formation mechanism and to adapt future emission standards. The purpose of this work was to study the emission behavior of two mopeds complying with different European emission standards (EURO-1 and EURO-2). A sophisticated set of online analyzers was applied to simultaneously monitor the gas phase and particulate phase of exhaust on a real time basis. The gaseous emission was analyzed with a high resolution Fourier transform infrared spectrometer (FTIR; nitrogen species) and a resonance-enhanced multiphoton ionization time-of-flight mass spectrometer (REMPI-ToF-MS; polycyclic aromatic hydrocarbons: PAH), whereas the particulate phase was chemically characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS; organic, nitrate and chloride aerosol) and a multiangle absorption photometer (MAAP; black carbon). The physical characterization of the aerosol was carried out with a condensation particle counter (CPC; particle number concentration) and a fast mobility particle sizer (FMPS; size distribution in real time). In order to extract underlying correlation between gas and solid emissions, principal component analysis was applied to the comprehensive online dataset. Multivariate analysis highlighted the considerable effect of the exhaust temperature on the particles and heavy PAH emissions. The results showed that the after-treatment used to comply with the latest EURO-2 emission standard may be responsible for the production of more potentially harmful particles compared to the EURO-1 moped emissions. Copyright © 2011 Elsevier B.V. All

  14. Using the chemical equilibrium partitioning space to explore factors influencing the phase distribution of compounds involved in secondary organic aerosol formation

    Science.gov (United States)

    Wania, F.; Lei, Y. D.; Wang, C.; Abbatt, J. P. D.; Goss, K.-U.

    2015-03-01

    Many atmospheric and chemical variables influence the partitioning equilibrium between gas phase and condensed phases of compounds implicated in the formation of secondary organic aerosol (SOA). The large number of factors and their interaction makes it often difficult to assess their relative importance and concerted impact. Here we introduce a two-dimensional space which maps regions of dominant atmospheric phase distribution within a coordinate system defined by equilibrium partition coefficients between the gas phase, an aqueous phase and a water-insoluble organic matter (WIOM) phase. Placing compounds formed from the oxidation of n-alkanes, terpenes and mono-aromatic hydrocarbons on the maps based on their predicted partitioning properties allows for a simple graphical assessment of their equilibrium phase distribution behaviour. Specifically, it allows for the simultaneous visualisation and quantitative comparison of the impact on phase distribution of changes in atmospheric parameters (such as temperature, salinity, WIOM-phase polarity, organic aerosol load, and liquid water content) and chemical properties (such as oxidation state, molecular size, functionalisation, and dimerisation). The graphical analysis reveals that the addition of hydroxyl, carbonyl and carboxyl groups increases the affinity of aliphatic, alicyclic and aromatic hydrocarbons for the aqueous phase more rapidly than their affinity for WIOM, suggesting that the aqueous phase may often be relevant even for substances that are considerably larger than the C2 and C3 compounds that are typically believed to be associated with aqueous SOA. In particular, the maps identify some compounds that contribute to SOA formation if partitioning to both WIOM and aqueous phase is considered but would remain in the gas phase if either condensed phase were neglected. For example, many semi-volatile α-pinene oxidation products will contribute to aqueous SOA under the conditions of high liquid water content

  15. Studies on the Effect of Sub-zero Temperatures on the Formation of Extremely Low Volatility Dimer Esters in Secondary Organic Aerosol from Alpha-Pinene

    Science.gov (United States)

    Kristensen, Kasper; Normann Jensen, Louise; Bilde, Merete

    2016-04-01

    The oxidation of volatile organic compounds (VOC) is considered a major source of secondary organic aerosols (SOA) in the atmosphere. Recently, extremely low volatility organic compounds, or ELVOC, formed from the oxidation of VOCs have been shown to play a crucial role in new particle formation (Ehn et al., 2014). In addition, higher molecular weight dimer esters originating from the oxidation of the biogenic VOC alpha-pinene have been observed in both laboratory-generated and ambient SOA (Kristensen et al., 2013). The low volatility of the dimer esters along with an observed rapid formation makes these high molecular weight compounds likely candidates involved in new particle formation from the oxidation of alpha-pinene. Furthermore, laboratory experiments show that the dimer esters only form in the presence of ozone, thus may be used as tracers for the ozone-initiated oxidation of alpha-pinene, and are therefore indicative of enhanced anthropogenic activities. In this work, we present the results of a series of oxidation experiments performed in the newly constructed cold-room smog chamber at Aarhus University. This unique and state-of-the-art Teflon chamber allows for atmospheric simulations of the oxidation VOCs and subsequent SOA formation at temperatures down to -16 °C. In this study, ozonolysis and photochemical oxidations of alpha-pinene are performed at temperatures ranging from +20 to -16 °C. Chemical characterization of the formed SOA is performed using liquid chromatography coupled to quadrupole time-of-flight mass spectrometry. The results show significant differences in the chemical composition related to the experiment temperature. In particularly, the concentration of the high molecular weight dimer esters showed to be highly affected by temperature. Interestingly, preliminary results show higher formation of dimer esters related to increased SOA formation rate, thus indicating that these particle-phase ELVOCs may be linked with new particle

  16. Hyperventilation and exhaustion syndrome.

    Science.gov (United States)

    Ristiniemi, Heli; Perski, Aleksander; Lyskov, Eugene; Emtner, Margareta

    2014-12-01

    Chronic stress is among the most common diagnoses in Sweden, most commonly in the form of exhaustion syndrome (ICD-10 classification - F43.8). The majority of patients with this syndrome also have disturbed breathing (hyperventilation). The aim of this study was to investigate the association between hyperventilation and exhaustion syndrome. Thirty patients with exhaustion syndrome and 14 healthy subjects were evaluated with the Nijmegen Symptom Questionnaire (NQ). The participants completed questionnaires about exhaustion, mental state, sleep disturbance, pain and quality of life. The evaluation was repeated 4 weeks later, after half of the patients and healthy subjects had engaged in a therapy method called 'Grounding', a physical exercise inspired by African dance. The patients reported significantly higher levels of hyperventilation as compared to the healthy subjects. All patients' average score on NQ was 26.57 ± 10.98, while that of the healthy subjects was 15.14 ± 7.89 (t = -3.48, df = 42, p exhaustion (Karolinska Exhaustion Scale KES r = 0.772, p exhaustion scores and scores of depression and anxiety. The conclusion is that hyperventilation is common in exhaustion syndrome patients and that it can be reduced by systematic physical therapy such as Grounding. © 2013 The Authors. Scandinavian Journal of Caring Sciences published by John Wiley & Sons Ltd on behalf of Nordic College of Caring Science.

  17. Local Exhaust Ventilation

    DEFF Research Database (Denmark)

    Madsen, Ulla; Breum, N. O.; Nielsen, Peter V.

    Capture efficiency of a local exhaust system, e.g. a kitchen hood, should include only contaminants being direct captured. In this study basic concepts of local exhaust capture efficiency are given, based on the idea of a control box. A validated numerical model is used for estimation...

  18. Immune Exhaustion and Transplantation.

    Science.gov (United States)

    Sanchez-Fueyo, A; Markmann, J F

    2016-07-01

    Exhaustion of lymphocyte function through chronic exposure to a high load of foreign antigen is well established for chronic viral infection and antitumor immunity and has been found to be associated with a distinct molecular program and characteristic cell surface phenotype. Although exhaustion has most commonly been studied in the context of CD8 viral responses, recent studies indicate that chronic antigen exposure may affect B cells, NK cells and CD4 T cells in a parallel manner. Limited information is available regarding the extent of lymphocyte exhaustion development in the transplant setting and its impact on anti-graft alloreactivity. By analogy to the persistence of a foreign virus, the large mass of alloantigen presented by an allograft in chronic residence could provide an ideal setting for exhausting donor-reactive T cells. The extent of T cell exhaustion occurring with various allografts, the kinetics of its development, whether exhaustion is influenced positively or negatively by different immunosuppressants, and the impact of exhaustion on graft survival and tolerance development remains a fertile area for investigation. Harnessing or encouraging the natural processes of exhaustion may provide a novel means to promote graft survival and transplantation tolerance. © Copyright 2016 The American Society of Transplantation and the American Society of Transplant Surgeons.

  19. Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

    Science.gov (United States)

    Ortega, Amber M.; Hayes, Patrick L.; Peng, Zhe; Palm, Brett B.; Hu, Weiwei; Day, Douglas A.; Li, Rui; Cubison, Michael J.; Brune, William H.; Graus, Martin; Warneke, Carsten; Gilman, Jessica B.; Kuster, William C.; de Gouw, Joost; Gutiérrez-Montes, Cándido; Jimenez, Jose L.

    2016-06-01

    Field studies in polluted areas over the last decade have observed large formation of secondary organic aerosol (SOA) that is often poorly captured by models. The study of SOA formation using ambient data is often confounded by the effects of advection, vertical mixing, emissions, and variable degrees of photochemical aging. An oxidation flow reactor (OFR) was deployed to study SOA formation in real-time during the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign in Pasadena, CA, in 2010. A high-resolution aerosol mass spectrometer (AMS) and a scanning mobility particle sizer (SMPS) alternated sampling ambient and reactor-aged air. The reactor produced OH concentrations up to 4 orders of magnitude higher than in ambient air. OH radical concentration was continuously stepped, achieving equivalent atmospheric aging of 0.8 days-6.4 weeks in 3 min of processing every 2 h. Enhancement of organic aerosol (OA) from aging showed a maximum net SOA production between 0.8-6 days of aging with net OA mass loss beyond 2 weeks. Reactor SOA mass peaked at night, in the absence of ambient photochemistry and correlated with trimethylbenzene concentrations. Reactor SOA formation was inversely correlated with ambient SOA and Ox, which along with the short-lived volatile organic compound correlation, indicates the importance of very reactive (τOH ˜ 0.3 day) SOA precursors (most likely semivolatile and intermediate volatility species, S/IVOCs) in the Greater Los Angeles Area. Evolution of the elemental composition in the reactor was similar to trends observed in the atmosphere (O : C vs. H : C slope ˜ -0.65). Oxidation state of carbon (OSc) in reactor SOA increased steeply with age and remained elevated (OSC ˜ 2) at the highest photochemical ages probed. The ratio of OA in the reactor output to excess CO (ΔCO, ambient CO above regional background) vs. photochemical age is similar to previous studies at low to moderate ages and also extends to

  20. Spatial and seasonal variability of PM2.5 acidity at two Chinese megacities: insights into the formation of secondary inorganic aerosols

    Directory of Open Access Journals (Sweden)

    Z. Shi

    2012-02-01

    Full Text Available Aerosol acidity is one of the most important parameters influencing atmospheric chemistry and physics. Based on continuous field observations from January 2005 to May 2006 and thermodynamic modeling, we investigated the spatial and seasonal variations in PM2.5 acidity in two megacities in China, Beijing and Chongqing. Spatially, PM2.5 was generally more acidic in Chongqing than in Beijing, but a reverse spatial pattern was found within the two cities, with more acidic PM2.5 at the urban site in Beijing whereas the rural site in Chongqing. Ionic compositions of PM2.5 revealed that it was the higher concentrations of NO3− at the urban site in Beijing and the lower concentrations of Ca2+ within the rural site in Chongqing that made their PM2.5 more acidic. Temporally, PM2.5 was more acidic in summer and fall than in winter, while in the spring of 2006, the acidity of PM2.5 was higher in Beijing but lower in Chongqing than that in 2005. These were attributed to the more efficient formation of nitrate relative to sulfate as a result of the influence of Asian desert dust in 2006 in Beijing and the greater wet deposition of ammonium compared to sulfate and nitrate in 2005 in Chongqing. Furthermore, simultaneous increase of PM2.5 acidity was observed from spring to early summer of 2005 in both cities. This synoptic-scale evolution of PM2.5 acidity was accompanied by the changes in air masses origins, which were influenced by the movements of a subtropical high over the northwestern Pacific in early summer. Finally, the correlations between [NO3−]/[SO42−] and [NH4+]/[SO42−] suggests that under conditions of high aerosol acidity, heterogeneous reactions became one of the major pathways for the formation of nitrate at both cities. These findings provided new insights in our understanding of the spatial and temporal variations in aerosol acidity in Beijing and Chongqing, as well as those reported in other cities in China.

  1. Can scooter emissions dominate urban organic aerosol?

    Science.gov (United States)

    El Haddad, Imad; Platt, Stephen; Huang, Ru-Jin; Zardini, Alessandro; Clairotte, Micheal; Pieber, Simone; Pfaffenberger, Lisa; Fuller, Steve; Hellebust, Stig; Temime-Roussel, Brice; Slowik, Jay; Chirico, Roberto; Kalberer, Markus; Marchand, Nicolas; Dommen, Josef; Astorga, Covadonga; Baltensperger, Urs; Prevot, Andre

    2014-05-01

    In urban areas, where the health impact of pollutants increases due to higher population density, traffic is a major source of ambient organic aerosol (OA). A significant fraction of OA from traffic is secondary, produced via the reaction of exhaust volatile organic compounds (VOCs) with atmospheric oxidants. Secondary OA (SOA) has not been systematically assessed for different vehicles and driving conditions and thus its relative importance compared to directly emitted, primary OA (POA) is unknown, hindering the design of effective vehicle emissions regulations. 2-stroke (2S) scooters are inexpensive and convenient and as such a popular means of transportation globally, particularly in Asia. European regulations for scooters are less stringent than for other vehicles and thus primary particulate emissions and SOA precursor VOCs from 2S engines are estimated to be much higher. Assessing the effects of scooters on public health requires consideration of both POA, and SOA production. Here, we quantify POA emission factors and potential SOA EFs from 2S scooters, and the effect of using aromatic free fuel instead of standard gasoline thereon. During the tests, Euro 1 and Euro 2 2S scooters were run in idle or simulated low power conditions. Emissions from a Euro 2 2S scooter were also sampled during regulatory driving cycles on a chassis dynamometer. Vehicle exhaust was introduced into smog chambers, where POA emission and SOA production were quantified using a high-resolution time-of-flight aerosol mass spectrometer. A high resolution proton transfer time-of-flight mass spectrometer was used to investigate volatile organic compounds and a suite of instruments was utilized to quantify CO, CO2, O3, NOX and total hydrocarbons. We show that the oxidation of VOCs in the exhaust emissions of 2S scooters produce significant SOA, exceeding by up to an order of magnitude POA emissions. By monitoring the decay of VOC precursors, we show that SOA formation from 2S scooter

  2. Organic aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Penner, J.E.

    1994-01-01

    Organic aerosols scatter solar radiation. They may also either enhance or decrease concentrations of cloud condensation nuclei. This paper summarizes observed concentrations of aerosols in remote continental and marine locations and provides estimates for the sources of organic aerosol matter. The anthropogenic sources of organic aerosols may be as large as the anthropogenic sources of sulfate aerosols, implying a similar magnitude of direct forcing of climate. The source estimates are highly uncertain and subject to revision in the future. A slow secondary source of organic aerosols of unknown origin may contribute to the observed oceanic concentrations. The role of organic aerosols acting as cloud condensation nuclei (CCN) is described and it is concluded that they may either enhance or decrease the ability of anthropogenic sulfate aerosols to act as CCN.

  3. Formation of TiO2 film with lower electrical resistance by aerosol beam and fiber laser irradiation

    Science.gov (United States)

    Shinonaga, T.; Tsukamoto, M.; Takahashi, M.; Fujita, M.; Abe, N.

    2013-07-01

    Titanium dioxide (TiO2) is a functional ceramic with unique photoconductive and photocatalytic properties. In our previous study, a TiO2 film was formed by aerosol beam irradiation. The films were darkened by femtosecond laser irradiation in air. Then electrical resistance of the darkened area on the film decreased. The heating process is also a useful method to vary the TiO2 film property. Local heating can be performed by using a continuous wave (CW) fiber laser. In this study, the film was irradiated with a commercial CW fiber laser in vacuum. Laser irradiated area on the film was also darkened after CW fiber laser irradiation. The electrical resistance of the darkened area on the films was decreased as laser fluence was increased. Electrical resistance of the darkened area after CW fiber laser irradiation in vacuum was much smaller than that after femtosecond laser irradiation.

  4. Aerosols from biomass combustion

    Energy Technology Data Exchange (ETDEWEB)

    Nussbaumer, T.

    2001-07-01

    This report is the proceedings of a seminar on biomass combustion and aerosol production organised jointly by the International Energy Agency's (IEA) Task 32 on bio energy and the Swiss Federal Office of Energy (SFOE). This collection of 16 papers discusses the production of aerosols and fine particles by the burning of biomass and their effects. Expert knowledge on the environmental impact of aerosols, formation mechanisms, measurement technologies, methods of analysis and measures to be taken to reduce such emissions is presented. The seminar, visited by 50 participants from 11 countries, shows, according to the authors, that the reduction of aerosol emissions resulting from biomass combustion will remain a challenge for the future.

  5. Examining the Effects of Anthropogenic Emissions on Isoprene-Derived Secondary Organic Aerosol Formation During the 2013 Southern Oxidant and Aerosol Study (SOAS) at the Look Rock, Tennessee, Ground Site

    Science.gov (United States)

    A suite of offline and real-time gas- and particle-phase measurements was deployed atLook Rock, Tennessee (TN), during the 2013 Southern Oxidant and Aerosol Study (SOAS) to examine the effects of anthropogenic emissions on isoprene-derived secondary organic aerosol (SOA) formatio...

  6. Aerosol dynamics in porous media

    NARCIS (Netherlands)

    Ghazaryan, L.

    2014-01-01

    In this thesis, a computational model was developed for the simulation of aerosol formation through nucleation, followed by condensation and evaporation and filtration by porous material. Understanding aerosol dynamics in porous media can help improving engineering models that are used in various

  7. Comparison of Gasoline Direct-Injection (GDI) and Port Fuel Injection (PFI) Vehicle Emissions: Emission Certification Standards, Cold-Start, Secondary Organic Aerosol Formation Potential, and Potential Climate Impacts.

    Science.gov (United States)

    Saliba, Georges; Saleh, Rawad; Zhao, Yunliang; Presto, Albert A; Lambe, Andrew T; Frodin, Bruce; Sardar, Satya; Maldonado, Hector; Maddox, Christine; May, Andrew A; Drozd, Greg T; Goldstein, Allen H; Russell, Lynn M; Hagen, Fabian; Robinson, Allen L

    2017-06-06

    Recent increases in the Corporate Average Fuel Economy standards have led to widespread adoption of vehicles equipped with gasoline direct-injection (GDI) engines. Changes in engine technologies can alter emissions. To quantify these effects, we measured gas- and particle-phase emissions from 82 light-duty gasoline vehicles recruited from the California in-use fleet tested on a chassis dynamometer using the cold-start unified cycle. The fleet included 15 GDI vehicles, including 8 GDIs certified to the most-stringent emissions standard, superultra-low-emission vehicles (SULEV). We quantified the effects of engine technology, emission certification standards, and cold-start on emissions. For vehicles certified to the same emissions standard, there is no statistical difference of regulated gas-phase pollutant emissions between PFIs and GDIs. However, GDIs had, on average, a factor of 2 higher particulate matter (PM) mass emissions than PFIs due to higher elemental carbon (EC) emissions. SULEV certified GDIs have a factor of 2 lower PM mass emissions than GDIs certified as ultralow-emission vehicles (3.0 ± 1.1 versus 6.3 ± 1.1 mg/mi), suggesting improvements in engine design and calibration. Comprehensive organic speciation revealed no statistically significant differences in the composition of the volatile organic compounds emissions between PFI and GDIs, including benzene, toluene, ethylbenzene, and xylenes (BTEX). Therefore, the secondary organic aerosol and ozone formation potential of the exhaust does not depend on engine technology. Cold-start contributes a larger fraction of the total unified cycle emissions for vehicles meeting more-stringent emission standards. Organic gas emissions were the most sensitive to cold-start compared to the other pollutants tested here. There were no statistically significant differences in the effects of cold-start on GDIs and PFIs. For our test fleet, the measured 14.5% decrease in CO 2 emissions from GDIs was much greater than

  8. Topics in current aerosol research

    CERN Document Server

    Hidy, G M

    1971-01-01

    Topics in Current Aerosol Research deals with the fundamental aspects of aerosol science, with emphasis on experiment and theory describing highly dispersed aerosols (HDAs) as well as the dynamics of charged suspensions. Topics covered range from the basic properties of HDAs to their formation and methods of generation; sources of electric charges; interactions between fluid and aerosol particles; and one-dimensional motion of charged cloud of particles. This volume is comprised of 13 chapters and begins with an introduction to the basic properties of HDAs, followed by a discussion on the form

  9. NK Cell Exhaustion

    Science.gov (United States)

    Bi, Jiacheng; Tian, Zhigang

    2017-01-01

    Natural killer cells are important effector lymphocytes of the innate immune system, playing critical roles in antitumor and anti-infection host defense. Tumor progression or chronic infections, however, usually leads to exhaustion of NK cells, thus limiting the antitumor/infection potential of NK cells. In many tumors or chronic infections, multiple mechanisms might contribute to the exhaustion of NK cells, such as dysregulated NK cell receptors signaling, as well as suppressive effects by regulatory cells or soluble factors within the microenvironment. Better understanding of the characteristics, as well as the underlying mechanisms of NK cell exhaustion, not only should increase our understanding of the basic biology of NK cells but also could reveal novel NK cell-based antitumor/infection targets. Here, we provide an overview of our current knowledge on NK cell exhaustion in tumors, and in chronic infections. PMID:28702032

  10. Unemployment Benefit Exhaustion

    DEFF Research Database (Denmark)

    Filges, Trine; Pico Geerdsen, Lars; Knudsen, Anne-Sofie Due

    2015-01-01

    This systematic review studied the impact of exhaustion of unemployment benefits on the exit rate out of unemployment and into employment prior to benefit exhaustion or shortly thereafter. Method: We followed Campbell Collaboration guidelines to prepare this review, and ultimately located 12...... studies for final analysis and interpretation. Twelve studies could be included in the data synthesis. Results: We found clear evidence that the prospect of exhaustion of benefits results in a significantly increased incentive for finding work. Discussion: The theoretical suggestion that the prospect...... of exhaustion of benefits results in an increased incentive for finding work has been confirmed empirically by measures from seven different European countries, the United States, and Canada. The results are robust in the sense that sensitivity analyses evidenced no appreciable changes in the results. We found...

  11. Immune Exhaustion and Transplantation

    National Research Council Canada - National Science Library

    Sanchez‐Fueyo, A; Markmann, J. F

    2016-01-01

    Exhaustion of lymphocyte function through chronic exposure to a high load of foreign antigen is well established for chronic viral infection and antitumor immunity and has been found to be associated...

  12. The effect of temperature and water on secondary organic aerosol formation from ozonolysis of limonene, Δ3-carene and α-pinene

    Directory of Open Access Journals (Sweden)

    E. Ljungström

    2008-11-01

    Full Text Available The effect of reaction temperature and how water vapour influences the formation of secondary organic aerosol (SOA in ozonolysis of limonene, Δ3-carene and α-pinene, both regarding number and mass of particles, has been investigated by using a laminar flow reactor (G-FROST. Experiments with cyclohexane and 2-butanol as OH scavengers were compared to experiments without any scavenger. The reactions were conducted in the temperature range between 298 and 243 K, and at relative humidities between <10 and 80%. Results showed that there is still a scavenger effect on number and mass concentrations at low temperatures between experiments with and without an addition of an OH scavenger. This shows that the OH chemistry is influencing the SOA formation also at these temperatures. The overall temperature dependence on SOA formation is not as strong as expected from partitioning theory. In some cases there is even a positive temperature dependence that must be related to changes in the chemical mechanism and/or reduced rates of secondary chemistry at low temperatures. The precursor's α-pinene and Δ3-carene exhibit a similar temperature dependence regarding both number and mass of particles formed, whereas limonene shows a different dependence. The water effect at low temperature could be explained by physical uptake and cluster stabilisation. At higher temperatures, only a physical explanation is not sufficient and the observations are in line with water changing the chemical mechanism or reaction rates. The data presented adds to the understanding of SOA contribution to new particle formation and atmospheric degradation mechanisms.

  13. ­­Secondary organic aerosol formation from photo-oxidation of wood combustion emissions: Characterization of gas phase precursors and their link to SOA budget

    Science.gov (United States)

    Bhattu, D.; Stefenelli, G.; Zotter, P.; Zhou, J.; Nussbaumer, T.; Bertrand, A.; Marchand, N.; Termine-Roussel, B.; Baltensperger, U.; Slowik, J.; Prevot, A. S.; El-Haddad, I.; Dommen, J.

    2016-12-01

    Current legislation limits the emission of particulate matter, but does not regulate the precursors potentially forming secondary organic aerosol (SOA). Recent literature has shown that only 22 non-traditional SOA precursors from residential wood combustion explains 84-116% of the observed SOA mass whereas traditional precursors in the models account for only 3-27% of the SOA mass (Bruns et al., 2016). Investigation of gas phase emissions from wood combustion and their SOA formation potential have largely focused on single combustion devices with limited operating conditions. As, both primary emissions and SOA formation is a strong function of device type, load, fuel and operating conditions, we have performed a detailed chamber study investigating the gas-phase precursors from beech wood using three combustion devices namely a pellet boiler (combustion conditions: optimum, lack and excess of oxygen), an industrial wood chip grate boiler (30% and 100% power), and a log wood stove (varying fuel load and moisture content) using a potential aerosol mass reactor (PAM) with varying OH exposure. The short residence time in the reactor allowed a time resolved picture of SOA production potential and reduced wall losses. The main aim of this study is to characterize the primary and aged gaseous emissions and investigate their SOA formation potential depending on their mass yield, molecular structures, functional groups and OH reactivity in order to ascertain the contribution of residential wood burning in total carbonaceous OA budget. The physical and chemical effects of different OA aging conditions were monitored using an SMPS, an Aethalometer, an HR-ToF-AMS, as well as a PTR-ToF-MS and other gas monitors. In pellet boiler, significant SOA mass enhancement is observed in excess oxygen conditions compared to optimum and oxygen deprived conditions. Highest gas phase emissions from wood stove are observed at cold start (start of each burn cycle) and lowest in burn out phase

  14. Indoor secondary organic aerosols formation from ozonolysis of monoterpene: An example of d-limonene with ammonia and potential impacts on pulmonary inflammations.

    Science.gov (United States)

    Niu, Xinyi; Ho, Steven Sai Hang; Ho, Kin Fai; Huang, Yu; Cao, Junji; Shen, Zhenxing; Sun, Jian; Wang, Xiumei; Wang, Yu; Lee, Shuncheng; Huang, Rujin

    2017-02-01

    Monoterpene is one class of biogenic volatile organic compounds (BVOCs) which widely presents in household cleaning products and air fresheners. It plays reactive role in secondary organic aerosols (SOAs) formation with ozone (O3) in indoor environments. Such ozonolysis can be influenced by the presence of gaseous pollutants such as ammonia (NH3). This study focuses on investigations of ozone-initiated formation of indoor SOAs with d-limonene, one of the most abundant indoor monoterpenes, in a large environmental chamber. The maximum total particle number concentration from the ozonolysis in the presence of NH3 was 60% higher than that in the absence of NH3. Both of the nuclei coagulation and condensation involve in the SOAs growth. The potential risks of pulmonary injury for the exposure to the secondary particles formed were presented with the indexes of tumor necrosis factor-α (TNF-α), interleukin-6 (IL-6) and interleukin-10 (IL-10) expression levels in bronchoalveolar lavage fluid (BALF) upon intratracheal instillation in mice lung for 6 and 12h. The results indicated that there was 22-39% stronger pulmonary inflammatory effect on the particles generated with NH3. This is a pilot study which demonstrates the toxicities of the indoor SOAs formed from the ozonolysis of a monoterpene. Copyright © 2016 Elsevier B.V. All rights reserved.

  15. Aerosol Observing System (AOS) Handbook

    Energy Technology Data Exchange (ETDEWEB)

    Jefferson, A

    2011-01-17

    The Aerosol Observing System (AOS) is a suite of in situ surface measurements of aerosol optical and cloud-forming properties. The instruments measure aerosol properties that influence the earth’s radiative balance. The primary optical measurements are those of the aerosol scattering and absorption coefficients as a function of particle size and radiation wavelength and cloud condensation nuclei (CCN) measurements as a function of percent supersaturation. Additional measurements include those of the particle number concentration and scattering hygroscopic growth. Aerosol optical measurements are useful for calculating parameters used in radiative forcing calculations such as the aerosol single-scattering albedo, asymmetry parameter, mass scattering efficiency, and hygroscopic growth. CCN measurements are important in cloud microphysical models to predict droplet formation.

  16. An Investigation of Aerosol Scattering and Absorption Properties in Wuhan, Central China

    Directory of Open Access Journals (Sweden)

    Wei Gong

    2015-04-01

    Full Text Available Aerosol scattering and absorption properties were continuously measured and analyzed at the urban Laboratory for Information Engineering in Surveying, Mapping and Remote Sensing (LIESMARS site in Wuhan, central China, from 1 December 2009 to 31 March 2014. The mean aerosol scattering coefficient , absorption coefficient , and single scattering albedo (SSA were 377.54 Mm−1, 119.06 Mm−1, and 0.73, respectively. Both  and  showed obvious annual variability with large values in winter and small values in summer, principally caused by the annual characteristics of meteorological conditions, especially planetary boundary layer height (PBLH and local emissions. The SSA showed a slight annual variation. High values of SSA were related to formation of secondary aerosols in winter hazes and aerosol hygroscopic growth in humid summer. The large SSA in June can be attributed to the biomass combustion in Hubei and surrounding provinces. Both  and  showed double peak phenomena in diurnal variation resulting from the shallow stable PBLH at night and automobile exhaust emission during morning rush hours. The SSA also exhibited a double peak phenomenon related to the proportional variation of black carbon (BC and light scattering particulates in the day and night. The long-term exploration on quantified aerosol optical properties can help offer scientific basis of introducing timely environmental policies for local government.

  17. 9,10-phenanthrenequinone, a component of diesel exhaust particles, inhibits the reduction of 4-benzoylpyridine and all-trans-retinal and mediates superoxide formation through its redox cycling in pig heart.

    Science.gov (United States)

    Shimada, Hideaki; Oginuma, Michiko; Hara, Akira; Imamura, Yorishige

    2004-08-01

    We have recently purified a tetrameric carbonyl reductase from the cytosolic fraction of pig heart (pig heart carbonyl reductase, PHCR), using 4-benzoylpyridine (4-BP) as the substrate. PHCR has the ability to catalyze efficiently the reduction of 9,10-phenanthrenequinone (PQ) contained in diesel exhaust particles (DEPs). Thus, the present study was attempted to characterize the inhibitory effect of PQ on the reduction of 4-BP and all-trans-retinal in pig heart cytosol. Of the DEP components examined, PQ was the most potent inhibitor for the reduction of 4-BP and all-trans-retinal in pig heart cytosol. PQ also inhibited competitively the 4-BP reduction. These results indicate that PQ inhibits the reduction of 4-BP and all-trans-retinal by acting PHCR present in pig heart cytosol. Furthermore, whether PQ induces the formation of superoxide anion radical was examined in pig heart cytosol. The absorbance of cytochrome c at 550 nm was increased with the time by adding PQ, and the increased absorbance was decreased in the presence of superoxide dismutase. A similar result was observed in the reaction system of recombinant PHCR. On the basis of these results, it is concluded that PQ not only inhibits the reduction of 4-BP and all-trans-retinal catalyzed by PHCR but also mediates superoxide formation through its redox cycling involved in PHCR. We propose the possibility that PQ disturbs the homeostasis of retinoid metabolism and induces oxidative stress in pig heart.

  18. Atmospheric hydrogen peroxide and organic hydroperoxides during PRIDE-PRD'06, China: their concentration, formation mechanism and contribution to secondary aerosols

    Directory of Open Access Journals (Sweden)

    W. Hua

    2008-11-01

    detected in this region can account for the production of hydroperoxides, while the moderate level of NOx suppressed the formation of hydroperoxides. High concentrations of hydroperoxides were detected in samples of rainwater collected in a heavy shower on 25 July when a typhoon passed through, indicating that a considerable mixing ratio of hydroperoxides, particularly MHP, resided above the boundary layer, which might be transported on a regional scale and further influence the redistribution of HOx and ROx radicals. It was found that hydroperoxides, in particular H2O2, play an important role in the formation of secondary sulfate in the aerosol phase, where the heterogeneous reaction might contribute substantially. A negative correlation between hydroperoxides and water-soluble organic compounds (WSOC, a considerable fraction of the secondary organic aerosol (SOA, was observed, possibly providing field evidence for the importance of hydroperoxides in the formation of SOA found in previous laboratory studies. We suggest that hydroperoxides act as an important link between sulfate and organic aerosols, which needs further study and should be considered in current atmospheric models.

  19. Theoretical model on the formation possibility of secondary organic aerosol from radOH initialed oxidation reaction of styrene in the presence of O2/NO

    Science.gov (United States)

    Wang, Honghong; Ji, Yuemeng; Gao, Yanpeng; Li, Guiying; An, Taicheng

    2015-01-01

    Understanding radOH oxidation reaction is vital in understanding atmospheric pollution dynamics, and developing possible strategies for countering pollutant problems. This study used a theory-based approach to model the formation mechanisms of secondary organic aerosol (SOA) from styrene-radOH oxidation reactions in the presence of O2/NO. As a comparative measure, the mechanisms in the absence of NO (representing a pollution-free environment) were also investigated. The results showed that styrene can be initially attacked by radOH in two ways: OH-addition and H-abstraction. The OH-aliphatic-addition pathway occurs easily; the H-abstraction pathway may be ignored given atmospheric conditions. It was found that IMaddβ (C6H5CHCH2OH) was the main intermediate, and could be transformed to a peroxyl radical in the presence of O2. In the NO-free atmosphere, the peroxyl radical was decomposed to recycling-radOH and aldehydes. In the NO-polluted atmosphere, it could be degraded to organic nitrate (RO-NO2) which plays an important role in the production of SOA. Besides, the percent of organic nitrate in the particulate phase was calculated within the range of 2.4%-6.3% in Guangzhou city, and organic nitrates may constitute an important fraction of the total organic aerosol. The kinetic data calculated using canonical variational transition state theory with the small-curvature tunneling correction showed that, in the NO-polluted/unpolluted atmospheres, the styrene-radOH oxidation reaction easily occurred across an altitude range of 0-12 km. Especially, peroxyl radical lifetime was 10-3 s in the high NO-polluted atmosphere, indicating that the styrene-radOH oxidation reaction could significantly contribute to SOA formation in the NO-polluted atmosphere. The current results informed possible approaches for forming SOA from volatile organic compound (VOC) oxidation reactions, and could help evaluate regional air quality, especially in high NO-polluted atmospheres.

  20. Vehicle exhaust: An overstated cause of haze in China.

    Science.gov (United States)

    Zhao, Yi-Bo; Gao, Pan-Pan; Yang, Wan-Dong; Ni, Hong-Gang

    2018-01-15

    Overall, total exhaust emissions of NOX, VOC and particulate matter (PM) declined, though vehicles in use continued to increase in China. This suggested that contribution of motor vehicle exhaust to haze in China may be exaggerated. A higher frequency of haze episodes in China with lower total emissions fraction from vehicle exhaust compared with those in the USA confirmed that there exists no strict causality between vehicle and haze. No significant correlation (pvehicles to airborne PM2.5 (particulates that are aerodynamic diameter) or car ownerships. All results revealed again that vehicle exhaust is an overstated cause for haze formation in China. Copyright © 2017 Elsevier B.V. All rights reserved.

  1. Long-term aerosol and trace gas measurements in Eastern Lapland, Finland: the impact of Kola air pollution to new particle formation and potential CCN

    Science.gov (United States)

    Kyrö, Ella-Maria; Väänänen, Riikka; Kerminen, Veli-Matti; Virkkula, Aki; Asmi, Ari; Nieminen, Tuomo; Dal Maso, Miikka; Petäjä, Tuukka; Keronen, Petri; Aalto, Pasi; Riipinen, Ilona; Lehtipalo, Katrianne; Hari, Pertti; Kulmala, Markku

    2014-05-01

    Sulphur and primary emissions have been decreasing largely all over Europe, resulting in improved air quality and decreased direct radiation forcing by aerosols. The smelter industry in Kola Peninsula is one of largest sources of anthropogenic SO2 within the Arctic domain and since late 1990s the sulphur emissions have been decreasing rapidly (Paatero et al., 2008; Prank et al., 2010). New particle formation (NPF) is tightly linked with the oxidizing product of SO2, namely sulphuric acid (H2SO4), since it is known to be the key component in atmospheric nucleation (Sipilä et al., 2010). Thus, decreasing sulphur pollution may lead to less NPF. However, low values of condensation sink (CS), which is determined by the amount of pre-existing particles, favours NPF. We used 14 years (1998-2011) of aerosol number size distribution and trace gas data from SMEAR I station in Eastern Lapland, Finland, to investigate these relationships between SO2, NPF and CS. The station is a clean background station with occasional sulphur pollution episodes when the air masses arrive over Kola Peninsula. We found that while SO2 decreased by 11.3 % / year, the number of clear NPF event days was also decreasing by 9.9 % / year. At the same time, CS was decreasing also (-8.0 % / year) leading to formation of more particles per single NPF event (J3 increased by 29.7 % / year in 2006-2011) but the low vapour concentrations of H2SO4 (proxy decreased by 6.2 % / year) did not allow them to grow into climatically relevant sizes. Over the time, concentrations of potential CCN (cloud condensing nuclei) were also decreasing with more moderate pace, -4.0 % / year. The events started on average earlier after sunrise when the SO2 concentration during the start of the event was higher and NPF occurred more frequently in air masses which were travelling over Kola. Despite the total decrease in sulphur pollution originating from Kola there is currently no evidence of cleaning of the emissions, rather the

  2. Aerosol accumulation intensity and composition variations under different weather conditions in urban environment

    Science.gov (United States)

    Steinberga, Iveta; Bikshe, Janis; Eindorfa, Aiva

    2014-05-01

    activities and transportation by rail. The type of prevailing secondary aerosol formation was estimated by linear regression analysis which shows NOx prevalence in street canyons and urban background and SO2 associated reactions in industrial sites. Linear regression of traffic intensity in connection with aerosol pollution level shows domination of exhaust emissions during traffic jams and resuspension intensity during middle of the week.

  3. Secondary Organic Aerosol Formation by Cloud Processing: Accretion Reactions Involving Glyoxal and Methylglyoxal in Evaporating Cloud Droplets

    Science.gov (United States)

    de Haan, D. O.; Hastings, W. P.; Corrigan, A. L.; Lee, F. E.; Hanley, S. W.

    2006-12-01

    Glyoxal and methyl glyoxal are dicarbonyl compounds found in atmospheric cloud and fog water, typically at low micromolar concentrations. These two compounds are known to form copolymers under certain industrial conditions by the nucleophilic addition of S, N and O-containing molecules. We report ambient FTIR-ATR and particle chamber data on a range of reactions between glyoxal and S, N and O-containing molecules found in cloudwater, some of which are triggered by droplet evaporation. Liquid-phase formation of adducts between glyoxal and S(IV) is seen to halt sulfur oxidation during droplet drying on the ATR crystal. Formation of glyoxal / S(VI) adducts, however, are not observed by ATR. At neutral or acidic pH, droplet evaporation triggers a reaction between glyoxal and amino acids in the residue left behind, forming imines. Glyoxal reacts under similar conditions with glycol compounds, forming cyclic acetals, but not with sugars, perhaps due to a lack of conformational freedom. Glyoxal is not observed to react with carboxylic acids, either in particle chambers or while drying on an ATR crystal.

  4. Aerodynamic Control of Exhaust

    DEFF Research Database (Denmark)

    Hyldgård, Carl-Erik

    In the autumn of 1985 the Unive!Sity of Aalborg was approached by the manufacturer C. P. Aaberg, who had obtained aerodynilmic control of the exhaust by means of injection. The remaining investigations comprising optimizations of the system with regard to effect, consumption, requirements...

  5. Exhaust bypass flow control for exhaust heat recovery

    Science.gov (United States)

    Reynolds, Michael G.

    2015-09-22

    An exhaust system for an engine comprises an exhaust heat recovery apparatus configured to receive exhaust gas from the engine and comprises a first flow passage in fluid communication with the exhaust gas and a second flow passage in fluid communication with the exhaust gas. A heat exchanger/energy recovery unit is disposed in the second flow passage and has a working fluid circulating therethrough for exchange of heat from the exhaust gas to the working fluid. A control valve is disposed downstream of the first and the second flow passages in a low temperature region of the exhaust heat recovery apparatus to direct exhaust gas through the first flow passage or the second flow passage.

  6. On the diurnal cycle of urban aerosols, black carbon and the occurrence of new particle formation events in springtime São Paulo, Brazil

    Directory of Open Access Journals (Sweden)

    J. Backman

    2012-12-01

    Full Text Available Large conurbations are a significant source of the anthropogenic pollution and demographic differences between cities that result in a different pollution burden. The metropolitan area of São Paulo (MASP, population 20 million accounts for one fifth of the Brazilian vehicular fleet. A feature of MASP is the amount of ethanol used by the vehicular fleet, known to exacerbate air quality. The study describes the diurnal behaviour of the submicron aerosol and relies on total particle number concentration, particle number size distribution, light scattering and light absorption measurements. Modelled planetary boundary layer (PBL depth and air mass movement data were used to aid the interpretation. During morning rush-hour, stagnant air and a shallow PBL height favour the accumulation of aerosol pollution. During clear-sky conditions, there was a wind shift towards the edge of the city indicating a heat island effect with implications on particulate pollution levels at the site. The median total particle number concentration for the submicron aerosol typically varied in the range 1.6 × 104–3.2 × 104 cm−3 frequently exceeding 4 × 104 cm−3 during the day. During weekdays, nucleation-mode particles are responsible for most of the particles by numbers. The highest concentrations of total particle number concentrations and black carbon (BC were observed on Fridays. Median diurnal values for light absorption and light scattering (at 637 nm wavelength varied in the range 12–33 Mm−1 and 21–64 Mm−1, respectively. The former one is equal to 1.8–5.0 μg m−3 of BC. The growth of the PBL, from the morning rush-hour until noon, is consistent with the diurnal cycle of BC mass concentrations. Weekday hourly median single-scattering albedo (ω0 varied in the range 0.59–0.76. Overall, this suggests a top of atmosphere (TOA warming effect. However

  7. CARES: Carbonaceous Aerosol and Radiative Effects Study Science Plan

    Energy Technology Data Exchange (ETDEWEB)

    Zaveri, RA; Shaw, WJ; Cziczo, DJ

    2010-05-27

    Carbonaceous aerosol components, which include black carbon (BC), urban primary organic aerosols (POA), biomass burning aerosols, and secondary organic aerosols (SOA) from both urban and biogenic precursors, have been previously shown to play a major role in the direct and indirect radiative forcing of climate. The primary objective of the CARES 2010 intensive field study is to investigate the evolution of carbonaceous aerosols of different types and their effects on optical and cloud formation properties.

  8. Filter-based Aerosol Measurement Experiments using Spherical Aerosol Particles under High Temperature and High Pressure

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Jong Chan; Jung, Woo Young; Lee, Hyun Chul; Lee, Doo Young [FNC TECH., Yongin (Korea, Republic of)

    2016-05-15

    Optical Particle Counter (OPC) is used to provide real-time measurement of aerosol concentration and size distribution. Glass fiber membrane filter also be used to measure average mass concentration. Three tests (MTA-1, 2 and 3) have been conducted to study thermal-hydraulic effect, a filtering tendency at given SiO{sub 2} particles. Based on the experimental results, the experiment will be carried out further with a main carrier gas of steam and different aerosol size. The test results will provide representative behavior of the aerosols under various conditions. The aim of the tests, MTA 1, 2 and 3, are to be able to 1) establish the test manuals for aerosol generation, mixing, sampling and measurement system, which defines aerosol preparation, calibration, operating and evaluation method under high pressure and high temperature 2) develop commercial aerosol test modules applicable to the thermal power plant, environmental industry, automobile exhaust gas, chemical plant, HVAC system including nuclear power plant. Based on the test results, sampled aerosol particles in the filter indicate that important parameters affecting aerosol behavior aerosols are 1) system temperature to keep above a evaporation temperature of ethanol and 2) aerosol losses due to the settling by ethanol liquid droplet.

  9. VOC species and emission inventory from vehicles and their SOA formation potentials estimation in Shanghai, China

    Science.gov (United States)

    Huang, C.; Wang, H. L.; Li, L.; Wang, Q.; Lu, Q.; de Gouw, J. A.; Zhou, M.; Jing, S. A.; Lu, J.; Chen, C. H.

    2015-10-01

    Volatile organic compound (VOC) species from vehicle exhausts and gas evaporation were investigated by chassis dynamometer and on-road measurements of nine gasoline vehicles, seven diesel vehicles, five motorcycles, and four gas evaporation samples. The secondary organic aerosol (SOA) mass yields of gasoline, diesel, motorcycle exhausts, and gas evaporation were estimated based on the mixing ratio of measured C2-C12 VOC species and inferred carbon number distributions. High aromatic contents were measured in gasoline exhausts and contributed comparatively more SOA yield. A vehicular emission inventory was compiled based on a local survey of on-road traffic in Shanghai and real-world measurements of vehicle emission factors from previous studies in the cities of China. The inventory-based vehicular organic aerosol (OA) productions to total CO emissions were compared with the observed OA to CO concentrations (ΔOA / ΔCO) in the urban atmosphere. The results indicate that vehicles dominate the primary organic aerosol (POA) emissions and OA production, which contributed about 40 and 60 % of OA mass in the urban atmosphere of Shanghai. Diesel vehicles, which accounted for less than 20 % of vehicle kilometers of travel (VKT), contribute more than 90 % of vehicular POA emissions and 80-90 % of OA mass derived by vehicles in urban Shanghai. Gasoline exhaust could be an important source of SOA formation. Tightening the limit of aromatic content in gasoline fuel will be helpful to reduce its SOA contribution. Intermediate-volatile organic compounds (IVOCs) in vehicle exhausts greatly contribute to SOA formation in the urban atmosphere of China. However, more experiments need to be conducted to determine the contributions of IVOCs to OA pollution in China.

  10. AEROSOL VARIABILITY OBSERVED WITH RPAS

    Directory of Open Access Journals (Sweden)

    B. Altstädter

    2013-08-01

    Full Text Available To observe the origin, vertical and horizontal distribution and variability of aerosol particles, and especially ultrafine particles recently formed, we plan to employ the remotely piloted aircraft system (RPAS Carolo-P360 "ALADINA" of TU Braunschweig. The goal of the presented project is to investigate the vertical and horizontal distribution, transport and small-scale variability of aerosol particles in the atmospheric boundary layer using RPAS. Two additional RPAS of type MASC of Tübingen University equipped with turbulence instrumentation add the opportunity to study the interaction of the aerosol concentration with turbulent transport and exchange processes of the surface and the atmosphere. The combination of different flight patterns of the three RPAS allows new insights in atmospheric boundary layer processes. Currently, the different aerosol sensors are miniaturized at the Leibniz Institute for Tropospheric Research, Leipzig and together with the TU Braunschweig adapted to fit into the RPAS. Moreover, an additional meteorological payload for measuring temperature, humidity and turbulence properties is constructed by Tübingen University. Two condensation particle counters determine the total aerosol number with a different lower detection threshold in order to investigate the horizontal and vertical aerosol variability and new particle formation (aerosol particles of some nm diameter. Further the aerosol size distribution in the range from about 0.300 to ~5 μm is given by an optical particle counter.

  11. Aerosol Variability Observed with Rpas

    Science.gov (United States)

    Altstädter, B.; Lampert, A.; Scholtz, A.; Bange, J.; Platis, A.; Hermann, M.; Wehner, B.

    2013-08-01

    To observe the origin, vertical and horizontal distribution and variability of aerosol particles, and especially ultrafine particles recently formed, we plan to employ the remotely piloted aircraft system (RPAS) Carolo-P360 "ALADINA" of TU Braunschweig. The goal of the presented project is to investigate the vertical and horizontal distribution, transport and small-scale variability of aerosol particles in the atmospheric boundary layer using RPAS. Two additional RPAS of type MASC of Tübingen University equipped with turbulence instrumentation add the opportunity to study the interaction of the aerosol concentration with turbulent transport and exchange processes of the surface and the atmosphere. The combination of different flight patterns of the three RPAS allows new insights in atmospheric boundary layer processes. Currently, the different aerosol sensors are miniaturized at the Leibniz Institute for Tropospheric Research, Leipzig and together with the TU Braunschweig adapted to fit into the RPAS. Moreover, an additional meteorological payload for measuring temperature, humidity and turbulence properties is constructed by Tübingen University. Two condensation particle counters determine the total aerosol number with a different lower detection threshold in order to investigate the horizontal and vertical aerosol variability and new particle formation (aerosol particles of some nm diameter). Further the aerosol size distribution in the range from about 0.300 to ~5 μm is given by an optical particle counter.

  12. Online differentiation of mineral phase in aerosol particles by ion formation mechanism using a LAAP-TOF single-particle mass spectrometer

    Science.gov (United States)

    Marsden, Nicholas A.; Flynn, Michael J.; Allan, James D.; Coe, Hugh

    2018-01-01

    Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is much longer than many atmospheric processes. Single-particle mass spectrometry (SPMS) is an established technique for the online size-resolved measurement of particle composition by laser desorption ionisation (LDI) followed by time-of-flight mass spectrometry (TOF-MS). Although non-quantitative, the technique is able to identify the presence of silicate minerals in airborne dust particles from markers of alkali metals and silicate molecular ions in the mass spectra. However, the differentiation of mineral phase in silicate particles by traditional mass spectral peak area measurements is not possible. This is because instrument function and matrix effects in the ionisation process result in variations in instrument response that are greater than the differences in composition between common mineral phases.In this study, we introduce a novel technique that enables the differentiation of mineral phase in silicate mineral particles by ion formation mechanism measured from subtle changes in ion arrival times at the TOF-MS detector. Using a combination of peak area and peak centroid measurements, we show that the arrangement of the interstitial alkali metals in the crystal structure, an important property in silicate mineralogy, influences the ion arrival times of elemental and molecular ion species in the negative ion mass spectra. A classification scheme is presented that allowed for the differentiation of illite-smectite, kaolinite and feldspar minerals on a single-particle basis. Online analysis of mineral dust aerosol generated from clay mineral standards produced mineral fractions that are in agreement with bulk measurements reported by

  13. Effect of EGR on the exhaust gas temperature and exhaust opacity ...

    Indian Academy of Sciences (India)

    In diesel engines, NOx formation is a highly temperature-dependent phenomenon and takes place when the temperature in the combustion chamber exceeds 2000 K. Therefore, in order to reduce NOx emissions in the exhaust, it is necessary to keep peak combustion temperatures under control. One simple way of ...

  14. Size-resolved aerosol emission factors and new particle formation/growth activity occurring in Mexico City during the MILAGRO 2006 Campaign

    Directory of Open Access Journals (Sweden)

    A. J. Kalafut-Pettibone

    2011-09-01

    Full Text Available Measurements of the aerosol size distribution from 11 nm to 2.5 microns were made in Mexico City in March 2006, during the MILAGRO (Megacity Initiative: Local and Global Research Observations field campaign. Observations at the urban supersite, referred to as T0, could often be characterized by morning conditions with high particle mass concentrations, low mixing heights, and highly correlated particle number and CO2 concentrations, indicative that particle number is controlled by primary emissions. Average size-resolved and total number- and volume-based emission factors for combustion sources impacting T0 have been determined using a comparison of peak sizes in particle number and CO2 concentration. Peaks are determined by subtracting the measured concentration from a calculated baseline concentration time series. The number emission and volume emission factors for particles from 11 nm to 494 nm are 1.56 × 1015 particles, and 9.48 × 1011 cubic microns per kg of carbon, respectively. The uncertainty of the number emission factor is approximately plus or minus 50 %. The mode of the number emission factor was between 25 and 32 nm, while the mode of the volume factor was between 0.25 and 0.32 microns. These emission factors are reported as log normal model parameters and are compared with multiple emission factors from the literature. In Mexico City in the afternoon, the CO2 concentration drops during ventilation of the polluted layer, and the coupling between CO2 and particle number breaks down, especially during new particle formation events when particle number is no longer controlled by primary emissions. Using measurements of particle number and CO2 taken aboard the NASA DC-8, the determined primary emission factor was applied to the Mexico City Metropolitan Area (MCMA plume to quantify the degree of secondary particle formation in the plume; the primary emission

  15. Size-resolved aerosol emission factors and new particle formation/growth activity occurring in Mexico City during the MILAGRO 2006 Campaign

    Energy Technology Data Exchange (ETDEWEB)

    Kalafut-Pettibone A. J.; Wang J.; Eichinger, W. E.; Clarke, A.; Vay, S. A.; Blake, D. R.; Stanier, C. O.

    2011-09-01

    Measurements of the aerosol size distribution from 11 nm to 2.5 microns were made in Mexico City in March 2006, during the MILAGRO (Megacity Initiative: Local and Global Research Observations) field campaign. Observations at the urban supersite, referred to as T0, could often be characterized by morning conditions with high particle mass concentrations, low mixing heights, and highly correlated particle number and CO{sub 2} concentrations, indicative that particle number is controlled by primary emissions. Average size-resolved and total number- and volume-based emission factors for combustion sources impacting T0 have been determined using a comparison of peak sizes in particle number and CO{sub 2} concentration. Peaks are determined by subtracting the measured concentration from a calculated baseline concentration time series. The number emission and volume emission factors for particles from 11 nm to 494 nm are 1.56 x 10{sup 15} particles, and 9.48 x 10{sup 11} cubic microns per kg of carbon, respectively. The uncertainty of the number emission factor is approximately plus or minus 50 %. The mode of the number emission factor was between 25 and 32 nm, while the mode of the volume factor was between 0.25 and 0.32 microns. These emission factors are reported as log normal model parameters and are compared with multiple emission factors from the literature. In Mexico City in the afternoon, the CO{sub 2} concentration drops during ventilation of the polluted layer, and the coupling between CO{sub 2} and particle number breaks down, especially during new particle formation events when particle number is no longer controlled by primary emissions. Using measurements of particle number and CO{sub 2} taken aboard the NASA DC-8, the determined primary emission factor was applied to the Mexico City Metropolitan Area (MCMA) plume to quantify the degree of secondary particle formation in the plume; the primary emission factor accounts for less than 50 % of the total particle

  16. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  17. Characterizing oxidative flow reactor SOA production and OH radical exposure from laboratory experiments of complex mixtures (engine exhaust) and simple precursors (monoterpenes)

    Science.gov (United States)

    Michael Link, M. L.; Friedman, B.; Ortega, J. V.; Son, J.; Kim, J.; Park, G.; Park, T.; Kim, K.; Lee, T.; Farmer, D.

    2016-12-01

    Recent commercialization of the Oxidative Flow Reactor (OFR, occasionally described in the literature as a "Potential Aerosol Mass") has created the opportunity for many researchers to explore the mechanisms behind OH-driven aerosol formation on a wide range of oxidative timescales (hours to weeks) in both laboratory and field measurements. These experiments have been conducted in both laboratory and field settings, including simple (i.e. single component) and complex (multi-component) precursors. Standard practices for performing OFR experiments, and interpreting data from the measurements, are still being developed. Measurement of gas and particle phase chemistry, from oxidation products generated in the OFR, through laboratory studies on single precursors and the measurement of SOA from vehicle emissions on short atmospheric timescales represent two very different experiments in which careful experimental design is essential for exploring reaction mechanisms and SOA yields. Two parameters essential in experimental design are (1) the role of seed aerosol in controlling gas-particle partitioning and SOA yields, and (2) the accurate determination of OH exposure during any one experiment. We investigated the role of seed aerosol surface area in controlling the observed SOA yields and gas/particle composition from the OH-initiated oxidation of four monoterpenes using an aerosol chemical ionization time-of-flight mass spectrometer and scanning mobility particle sizer. While the OH exposure during laboratory experiments is simple to constrain, complex mixtures such as diesel exhaust have high estimated OH reactivity values, and thus require careful consideration. We developed methods for constraining OH radical exposure in the OFR during vehicle exhaust oxidation experiments. We observe changes in O/C ratios and highly functionalized species over the temperature gradient employed in the aerosol-CIMS measurement. We relate this observed, speciated chemistry to the

  18. Cloud droplet activity changes of soot aerosol upon smog chamber ageing

    Science.gov (United States)

    Wittbom, C.; Eriksson, A. C.; Rissler, J.; Carlsson, J. E.; Roldin, P.; Nordin, E. Z.; Nilsson, P. T.; Swietlicki, E.; Pagels, J. H.; Svenningsson, B.

    2014-09-01

    Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC), to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA) precursors were processed by UV radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤2%, i.e. the BC core coated with primary organic aerosol (POA) from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatility organic compounds (IVOCs) in the diesel engine exhaust. The change of cloud condensation nuclei (CCN) properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I) organic fraction of the particle, (II) chemical properties of this fraction (e.g. primary or secondary organic aerosol), (III) particle size, and (IV) particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input

  19. CATALYTIC REDUCTION TECHNIQUES FOR POST-COMBUSTION DIESEL EXHAUST EMISSIONS

    OpenAIRE

    KESKİN, Ahmet; EMİROĞLU, Alaattin Osman

    2016-01-01

    Stiff exhaust emission regulations set for limiting the air pollution caused by motor vehicles have oriented the producers and researchers to investigate new techniques to reduce exhaust emissions. The main pollutants caused by diesel engines are particle matters (PM), nitrogen oxides (NOx), hydrocarbons (HC), and carbon monoxides (CO). Among the preventive actions to keep the emissions caused by motor vehicles at a certain level are enhancing the fuel quality, preventing the pollutant format...

  20. Formats

    Directory of Open Access Journals (Sweden)

    Gehmann, Ulrich

    2012-03-01

    Full Text Available In the following, a new conceptual framework for investigating nowadays’ “technical” phenomena shall be introduced, that of formats. The thesis is that processes of formatting account for our recent conditions of life, and will do so in the very next future. It are processes whose foundations have been laid in modernity and which will further unfold for the time being. These processes are embedded in the format of the value chain, a circumstance making them resilient to change. In addition, they are resilient in themselves since forming interconnected systems of reciprocal causal circuits.Which leads to an overall situation that our entire “Lebenswelt” became formatted to an extent we don’t fully realize, even influencing our very percep-tion of it.

  1. GASOLINE VEHICLE EXHAUST PARTICLE SAMPLING STUDY

    Energy Technology Data Exchange (ETDEWEB)

    Kittelson, D; Watts, W; Johnson, J; Zarling, D Schauer,J Kasper, K; Baltensperger, U; Burtscher, H

    2003-08-24

    The University of Minnesota collaborated with the Paul Scherrer Institute, the University of Wisconsin (UWI) and Ricardo, Inc to physically and chemically characterize the exhaust plume from recruited gasoline spark ignition (SI) vehicles. The project objectives were: (1) Measure representative particle size distributions from a set of on-road SI vehicles and compare these data to similar data collected on a small subset of light-duty gasoline vehicles tested on a chassis dynamometer with a dilution tunnel using the Unified Drive Cycle, at both room temperature (cold start) and 0 C (cold-cold start). (2) Compare data collected from SI vehicles to similar data collected from Diesel engines during the Coordinating Research Council E-43 project. (3) Characterize on-road aerosol during mixed midweek traffic and Sunday midday periods and determine fleet-specific emission rates. (4) Characterize bulk- and size-segregated chemical composition of the particulate matter (PM) emitted in the exhaust from the gasoline vehicles. Particle number concentrations and size distributions are strongly influenced by dilution and sampling conditions. Laboratory methods were evaluated to dilute SI exhaust in a way that would produce size distributions that were similar to those measured during laboratory experiments. Size fractionated samples were collected for chemical analysis using a nano-microorifice uniform deposit impactor (nano-MOUDI). In addition, bulk samples were collected and analyzed. A mixture of low, mid and high mileage vehicles were recruited for testing during the study. Under steady highway cruise conditions a significant particle signature above background was not measured, but during hard accelerations number size distributions for the test fleet were similar to modern heavy-duty Diesel vehicles. Number emissions were much higher at high speed and during cold-cold starts. Fuel specific number emissions range from 1012 to 3 x 1016 particles/kg fuel. A simple

  2. Sources and formation mechanisms of carbonaceous aerosol at a regional background site in the Netherlands : insights from a year-long radiocarbon study

    NARCIS (Netherlands)

    Dusek, Ulrike; Hitzenberger, Regina; Kasper-Giebl, Anne; Kistler, Magdalena; Meijer, Harro A. J.; Szidat, Sonke; Wacker, Lukas; Holzinger, Rupert; Rockmann, Thomas

    2017-01-01

    We measured the radioactive carbon isotope C-14 (radiocarbon) in various fractions of the carbonaceous aerosol sampled between February 2011 and March 2012 at the Cesar Observatory in the Netherlands. Based on the radiocarbon content in total carbon (TC), organic carbon (OC), water-insoluble organic

  3. Aerosol beam-focus laser-induced plasma spectrometer device

    Science.gov (United States)

    Cheng, Meng-Dawn

    2002-01-01

    An apparatus for detecting elements in an aerosol includes an aerosol beam focuser for concentrating aerosol into an aerosol beam; a laser for directing a laser beam into the aerosol beam to form a plasma; a detection device that detects a wavelength of a light emission caused by the formation of the plasma. The detection device can be a spectrometer having at least one grating and a gated intensified charge-coupled device. The apparatus may also include a processor that correlates the wavelength of the light emission caused by the formation of the plasma with an identity of an element that corresponds to the wavelength. Furthermore, the apparatus can also include an aerosol generator for forming an aerosol beam from bulk materials. A method for detecting elements in an aerosol is also disclosed.

  4. Aircraft exhaust sulfur emissions

    Energy Technology Data Exchange (ETDEWEB)

    Brown, R.C.; Anderson, M.R.; Miake-Lye, R.C.; Kolb, C.E. [Aerodyne Research, Inc., Billerica, MA (United States). Center for Chemical and Environmental Physics; Sorokin, A.A.; Buriko, Y.I. [Scientific Research Center `Ecolen`, Moscow (Russian Federation)

    1997-12-31

    The extent to which fuel sulfur is converted to SO{sub 3} during combustion and the subsequent turbine flow in supersonic and subsonic aircraft engines is estimated numerically. The analysis is based on: a flamelet model with non-equilibrium sulfur chemistry for the combustor, and a one-dimensional, two-stream model with finite rate chemical kinetics for the turbine. The results indicate that between 2% and 10% of the fuel sulfur is emitted as SO{sub 3}. It is also shown that, for a high fuel sulfur mass loading, conversion in the turbine is limited by the level of atomic oxygen at the combustor exit, leading to higher SO{sub 2} oxidation efficiency at lower fuel sulfur loadings. While SO{sub 2} and SO{sub 3} are the primary oxidation products, the model results further indicate H{sub 2}SO{sub 4} levels on the order of 0.1 ppm for supersonic expansions through a divergent nozzle. This source of fully oxidized S(6) (SO{sub 3} + H{sub 2}SO{sub 4}) exceeds previously calculated S(6) levels due to oxidation of SO{sub 2} by OH in the exhaust plume outside the engine nozzle. (author) 26 refs.

  5. Aerosol and monsoon climate interactions over Asia

    Science.gov (United States)

    Li, Zhanqing; Lau, W. K.-M.; Ramanathan, V.; Wu, G.; Ding, Y.; Manoj, M. G.; Liu, J.; Qian, Y.; Li, J.; Zhou, T.; Fan, J.; Rosenfeld, D.; Ming, Y.; Wang, Y.; Huang, J.; Wang, B.; Xu, X.; Lee, S.-S.; Cribb, M.; Zhang, F.; Yang, X.; Zhao, C.; Takemura, T.; Wang, K.; Xia, X.; Yin, Y.; Zhang, H.; Guo, J.; Zhai, P. M.; Sugimoto, N.; Babu, S. S.; Brasseur, G. P.

    2016-12-01

    The increasing severity of droughts/floods and worsening air quality from increasing aerosols in Asia monsoon regions are the two gravest threats facing over 60% of the world population living in Asian monsoon regions. These dual threats have fueled a large body of research in the last decade on the roles of aerosols in impacting Asian monsoon weather and climate. This paper provides a comprehensive review of studies on Asian aerosols, monsoons, and their interactions. The Asian monsoon region is a primary source of emissions of diverse species of aerosols from both anthropogenic and natural origins. The distributions of aerosol loading are strongly influenced by distinct weather and climatic regimes, which are, in turn, modulated by aerosol effects. On a continental scale, aerosols reduce surface insolation and weaken the land-ocean thermal contrast, thus inhibiting the development of monsoons. Locally, aerosol radiative effects alter the thermodynamic stability and convective potential of the lower atmosphere leading to reduced temperatures, increased atmospheric stability, and weakened wind and atmospheric circulations. The atmospheric thermodynamic state, which determines the formation of clouds, convection, and precipitation, may also be altered by aerosols serving as cloud condensation nuclei or ice nuclei. Absorbing aerosols such as black carbon and desert dust in Asian monsoon regions may also induce dynamical feedback processes, leading to a strengthening of the early monsoon and affecting the subsequent evolution of the monsoon. Many mechanisms have been put forth regarding how aerosols modulate the amplitude, frequency, intensity, and phase of different monsoon climate variables. A wide range of theoretical, observational, and modeling findings on the Asian monsoon, aerosols, and their interactions are synthesized. A new paradigm is proposed on investigating aerosol-monsoon interactions, in which natural aerosols such as desert dust, black carbon from

  6. TOMS Absorbing Aerosol Index

    Data.gov (United States)

    Washington University St Louis — TOMS_AI_G is an aerosol related dataset derived from the Total Ozone Monitoring Satellite (TOMS) Sensor. The TOMS aerosol index arises from absorbing aerosols such...

  7. Experiment to Characterize Aircraft Volatile Aerosol and Trace-Species Emissions (EXCAVATE)

    Science.gov (United States)

    Anderson, B. E.; Branham, H.-S.; Hudgins, C. H.; Plant, J. V.; Ballenthin, J. O.; Miller, T. M.; Viggiano, A. A.; Blake, D. R.; Boudries, H.; Canagaratna, M.

    2005-01-01

    The Experiment to Characterize Aircraft Volatile and Trace Species Emissions (EXCAVATE) was conducted at Langley Research Center (LaRC) in January 2002 and focused upon assaying the production of aerosols and aerosol precursors by a modern commercial aircraft, the Langley B757, during ground-based operation. Remaining uncertainty in the postcombustion fate of jet fuel sulfur contaminants, the need for data to test new theories of particle formation and growth within engine exhaust plumes, and the need for observations to develop air quality models for predicting pollution levels in airport terminal areas were the primary factors motivating the experiment. NASA's Atmospheric Effects of Aviation Project (AEAP) and the Ultra Effect Engine Technology (UEET) Program sponsored the experiment which had the specific objectives of determining ion densities; the fraction of fuel S converted from S(IV) to S(VI); the concentration and speciation of volatile aerosols and black carbon; and gas-phase concentrations of long-chain hydrocarbon and PAH species, all as functions of engine power, fuel composition, and plume age.

  8. Modeling urban and regional aerosols

    Science.gov (United States)

    Sun, Qing

    Aerosol particles in Earth's atmosphere have long been associated with adverse human health effects. They also play an important role in visibility reduction and global climate change. Atmospheric formation and removal of particles are governed by a number of complex dynamic processes which make the aerosol modeling a far more challenging task than the modeling of gas-phase species. Wexler et al. (1994) identified and analyzed the atmospheric aerosol processes that govern particulate mass concentrations and estimated the relative importance of each term using typical atmospheric conditions. In this thesis I start from the general dynamic equation resulted from their analysis and develop a working and optimized aerosol model that can be incorporated into a host Eulerian air quality model to simulate particulate pollution on an urban or a regional scale. Chapter 1 presents the background of the model and highlights the important issues that need to be addressed. Chapter 2 presents the mathematical representation of the aerosol model and introduces an acid equilibrium assumption, that is, when the aerosol particles are close to acid neutral the aerosol hydrogen ion concentration can be assumed to be in equilibrium with the gas-phase acidity. This assumption greatly reduced the CPU requirement of the aerosol model and hence enable us to complete the simulation of an particulate pollution episode in a reasonable time. In Chapter 3 the aerosol model IS incorporated into the Urban Airshed Model to predict the size and composition distribution of particulate matter (PM) during the June 24-25 1987 SCAQS episode. The predicted size distribution is compared to available SCAQS measurement data. In Chapter 4 the aerosol model is further optimized and incorporated into MCNC's Multiscale Air Quality Simulation Platform (MAQSIP) to investigate the particulate pollution in eastern United States using a July 9-13 1995 episode. A cloud model is modified for the sectional

  9. Electronic cigarette solutions and resultant aerosol profiles.

    Science.gov (United States)

    Herrington, Jason S; Myers, Colton

    2015-10-30

    Electronic cigarettes (e-cigarettes) are growing in popularity exponentially. Despite their ever-growing acceptance, their aerosol has not been fully characterized. The current study focused on evaluating e-cigarette solutions and their resultant aerosol for potential differences. A simple sampling device was developed to draw e-cigarette aerosol into a multi-sorbent thermal desorption (TD) tube, which was then thermally extracted and analyzed via a gas chromatography (GC) mass spectrometry (GC-MS) method. This novel application provided detectable levels of over one hundred fifteen volatile organic compounds (VOCs) and semivolatile organic compounds (SVOCs) from a single 40mL puff. The aerosol profiles from four commercially available e-cigarettes were compared to their respective solution profiles with the same GC-MS method. Solution profiles produced upwards of sixty four unidentified and identified (some only tentatively) constituents and aerosol profiles produced upwards of eighty two compounds. Results demonstrated distinct analyte profiles between liquid and aerosol samples. Most notably, formaldehyde, acetaldehyde, acrolein, and siloxanes were found in the aerosol profiles; however, these compounds were never present in the solutions. These results implicate the aerosolization process in the formation of compounds not found in solutions; have potential implications for human health; and stress the need for an emphasis on electronic cigarette aerosol testing. Copyright © 2015 The Authors. Published by Elsevier B.V. All rights reserved.

  10. Aerosol composition of the tropical upper troposphere

    Directory of Open Access Journals (Sweden)

    K. D. Froyd

    2009-07-01

    Full Text Available Aerosol composition was measured by the NOAA single-particle mass spectrometer (PALMS aboard the NASA WB-57 high altitude aircraft platform during two Aura Validation Experiment (AVE campaigns based in Costa Rica in 2004 and 2006. These studies yielded the most complete set of aerosol composition measurements to date throughout the tropical tropopause layer (TTL and tropical lower stratosphere. We describe the aerosol properties of the tropical atmosphere and use composition tracers to examine particle sources, the role of recent convection, and cirrus-forming potential in the TTL. Tropical dynamics and regional air sources played principal roles in dictating tropospheric aerosol properties. There was a sharp change in aerosol chemical composition at about 12 km altitude coincident with a change in convective influence. Below this level, maritime convection lofted condensable material that generated acidic, sulfate-rich aerosol. These particles contained significant amounts of methanesulfonic acid (MSA and showed evidence of cloud processes. In contrast, continental convection injected particles and precursors directly into the TTL, yielding a population of neutralized, organic-rich aerosol. The organics were often highly oxidized and particles with oxidized organics also contained nitrate. Above the tropopause, chemical composition gradually changed toward sulfuric acid particles but neutralized particles were still abundant 2 km above the tropopause. Deep continental convection, though sporadic and geographically localized, may strongly influence TTL aerosol properties on a global scale. The abundance of organic-rich aerosol may inhibit ice nucleation and formation of tropopause level cirrus.

  11. More surprises in the global greenhouse: Human health impacts from recent toxic marine aerosol formations, due to centennial alterations of world-wide coastal food webs.

    Science.gov (United States)

    Walsh, J J; Lenes, J M; Weisberg, R H; Zheng, L; Hu, C; Fanning, K A; Snyder, R; Smith, J

    2017-03-15

    Reductions of zooplankton biomasses and grazing pressures were observed during overfishing-induced trophic cascades and concurrent oil spills at global scales. Recent phytoplankton increments followed, once Fe-, P-, and N-nutrient limitations of commensal diazotrophs and dinoflagellates were also eliminated by respective human desertification, deforestation, and eutrophication during climate changes. Si-limitation of diatoms instead ensued during these last anthropogenic perturbations of agricultural effluents and sewage loadings. Consequently, ~15% of total world-wide annual asthma trigger responses, i.e. amounting to ~45 million adjacent humans during 2004, resulted from brevetoxin and palytoxin poisons in aerosol forms of western boundary current origins. They were denoted by greater global harmful algal bloom [HAB] abundances and breathing attacks among sea-side children during prior decadal surveys of asthma prevalence, compiled here in ten paired shelf ecosystems of western and eutrophied boundary currents. Since 1965, such inferred onshore fluxes of aerosolized DOC poisons of HABs may have served as additional wind-borne organic carriers of toxic marine MeHg, phthalate, and DDT/DDE vectors, traced by radio-iodine isotopes to potentially elicit carcinomas. During these exchanges, as much as 40% of mercury poisonings may instead have been effected by inhalation of collateral HAB-carried marine neurotoxic aerosols of MeHg, not just from eating marine fish. Health impacts in some areas were additional asthma and pneumonia episodes, as well as endocrine disruptions among the same adjacent humans, with known large local rates of thyroid cancers, physician-diagnosed pulmonary problems, and ubiquitous high indices of mercury in hair, pesticides in breast milk, and phthalates in urine. Copyright © 2017 Elsevier Ltd. All rights reserved.

  12. Influence of physical properties and chemical composition of sample on formation of aerosol particles generated by nanosecond laser ablation at 213 nm

    Energy Technology Data Exchange (ETDEWEB)

    Hola, Marketa, E-mail: mhola@sci.muni.c [Department of Chemistry, Faculty of Science, Masaryk University, Kotlarska 2, 611 37 Brno (Czech Republic); Konecna, Veronika [Department of Chemistry, Faculty of Science, Masaryk University, Kotlarska 2, 611 37 Brno (Czech Republic); Mikuska, Pavel [Institute of Analytical Chemistry, Academy of Sciences of the Czech Republic v.v.i., Veveri 97, 602 00 Brno (Czech Republic); Kaiser, Jozef [Institute of Physical Engineering, Faculty of Mechanical Engineering, Brno University of Technology, Technicka 2896/2, 616 69 Brno (Czech Republic); Kanicky, Viktor [Department of Chemistry, Faculty of Science, Masaryk University, Kotlarska 2, 611 37 Brno (Czech Republic)

    2010-01-15

    The influence of sample properties and composition on the size and concentration of aerosol particles generated by nanosecond Nd:YAG laser ablation at 213 nm was investigated for three sets of different materials, each containing five specimens with a similar matrix (Co-cemented carbides with a variable content of W and Co, steel samples with minor differences in elemental content and silica glasses with various colors). The concentration of ablated particles (particle number concentration, PNC) was measured in two size ranges (10-250 nm and 0.25-17 mum) using an optical aerosol spectrometer. The shapes and volumes of the ablation craters were obtained by Scanning Electron Microscopy (SEM) and by an optical profilometer, respectively. Additionally, the structure of the laser-generated particles was studied after their collection on a filter using SEM. The results of particle concentration measurements showed a significant dominance of particles smaller than 250 nm in comparison with larger particles, irrespective of the kind of material. Even if the number of particles larger than 0.25 mum is negligible (up to 0.1%), the volume of large particles that left the ablation cell can reach 50% of the whole particle volume depending on the material. Study of the ablation craters and the laser-generated particles showed a various number of particles produced by different ablation mechanisms (particle splashing or condensation), but the similar character of released particles for all materials was observed by SEM after particle collection on the membrane filter. The created aerosol always consisted of two main structures - spherical particles with diameters from tenths to units of micrometers originally ejected from the molten surface layer and mum-sized 'fibres' composed of primary agglomerates with diameters in the range between tens and hundreds of nanometers. The shape and structure of ablation craters were in good agreement with particle concentration

  13. EHMS: Exhaust Heat Management System

    Energy Technology Data Exchange (ETDEWEB)

    Strauss, T.; Schmidt, M.; Weinbrenner, M.; Geskes, P. [Behr GmbH und Co. KG, Stuttgart (Germany)

    2006-07-01

    Pollutant concentrations in diesel engines are reduced by cooling of the recirculated exhaust. This reduces emissions and particulate matter. The cooler technology can also be used for heating the passenger compartment faster and more economically. The authors present a model ready for seral production, including an exhaust flap for bypass control for use as auxiliary heating system. Further applications in gasoline engines are pointed out. (orig.)

  14. Model–measurement comparison of functional group abundance in α-pinene and 1,3,5-trimethylbenzene secondary organic aerosol formation

    Directory of Open Access Journals (Sweden)

    G. Ruggeri

    2016-07-01

    Full Text Available Secondary organic aerosol (SOA formed by α-pinene and 1,3,5-trimethylbenzene photooxidation under different NOx regimes is simulated using the Master Chemical Mechanism v3.2 (MCM coupled with an absorptive gas–particle partitioning module. Vapor pressures for individual compounds are estimated with the SIMPOL.1 group contribution model for determining apportionment of reaction products to each phase. We apply chemoinformatic tools to harvest functional group (FG composition from the simulations and estimate their contributions to the overall oxygen to carbon ratio. Furthermore, we compare FG abundances in simulated SOA to measurements of FGs reported in previous chamber studies using Fourier transform infrared spectroscopy. These simulations qualitatively capture the dynamics of FG composition of SOA formed from both α-pinene and 1,3,5-trimethylbenzene in low-NOx conditions, especially in the first hours after start of photooxidation. Higher discrepancies are found after several hours of simulation; the nature of these discrepancies indicates sources of uncertainty or types of reactions in the condensed or gas phase missing from current model implementation. Higher discrepancies are found in the case of α-pinene photooxidation under different NOx concentration regimes, which are reasoned through the domination by a few polyfunctional compounds that disproportionately impact the simulated FG abundance in the aerosol phase. This manuscript illustrates the usefulness of FG analysis to complement existing methods for model–measurement evaluation.

  15. Mechanism reduction for the formation of secondary organic aerosol for integration into a 3-dimensional regional air quality model: α-pinene oxidation system

    Directory of Open Access Journals (Sweden)

    D. V. Michelangeli

    2009-07-01

    Full Text Available A detailed α-pinene oxidation mechanism was reduced systematically through the successive application of five mechanism reduction techniques. The resulting reduced mechanism preserves the ozone- and organic aerosol-forming properties of the original mechanism, while using less species. The methodologies employed included a directed relation graph method with error propagation (DRGEP, which removed a large number of redundant species and reactions, principal component analysis of the rate sensitivity matrix (PCA, used to remove unnecessary reactions, the quasi-steady-state approximation (QSSA, used to remove some QSS species, an iterative screening method (ISSA, which removes redundant species and reactions simultaneously, and a new lumping approach dependent on the hydrocarbon to NOx ratio (which reduced the number of species in mechanism subsets for specific hydrocarbon to NOx ranges. This multistage methodology results in a reduction ratio of 2.5 for the number of both species and reactions compared with the full mechanism. The simplified mechanism reproduces the important gas and aerosol phase species (the latter are examined in detail by individual condensing species as well as in classes according to four functional groups: PANs, nitrates, organic peroxides, and organic acids. The total SOA mass is also well represented in the condensed mechanism, to within 16% of the detailed mechanism under a wide range of conditions. The methodology described here is general, and may be used in general mechanism reduction problems.

  16. 46 CFR 169.609 - Exhaust systems.

    Science.gov (United States)

    2010-10-01

    ... 46 Shipping 7 2010-10-01 2010-10-01 false Exhaust systems. 169.609 Section 169.609 Shipping COAST... Electrical Internal Combustion Engine Installations § 169.609 Exhaust systems. Engine exhaust installations... Yacht Council, Inc. Standard P-1, “Safe Installation of Exhaust Systems for Propulsion and Auxiliary...

  17. 49 CFR 325.91 - Exhaust systems.

    Science.gov (United States)

    2010-10-01

    ... 49 Transportation 5 2010-10-01 2010-10-01 false Exhaust systems. 325.91 Section 325.91... EMISSION STANDARDS Exhaust Systems and Tires § 325.91 Exhaust systems. Link to an amendment published at 75 FR 57193, Sept. 20, 2010. A motor vehicle does not conform to the visual exhaust system inspection...

  18. Linking Load, Fuel, and Emission Controls to Photochemical Production of Secondary Organic Aerosol from a Diesel Engine.

    Science.gov (United States)

    Jathar, Shantanu H; Friedman, Beth; Galang, Abril A; Link, Michael F; Brophy, Patrick; Volckens, John; Eluri, Sailaja; Farmer, Delphine K

    2017-02-07

    Diesel engines are important sources of fine particle pollution in urban environments, but their contribution to the atmospheric formation of secondary organic aerosol (SOA) is not well constrained. We investigated direct emissions of primary organic aerosol (POA) and photochemical production of SOA from a diesel engine using an oxidation flow reactor (OFR). In less than a day of simulated atmospheric aging, SOA production exceeded POA emissions by an order of magnitude or more. Efficient combustion at higher engine loads coupled to the removal of SOA precursors and particle emissions by aftertreatment systems reduced POA emission factors by an order of magnitude and SOA production factors by factors of 2-10. The only exception was that the retrofitted aftertreatment did not reduce SOA production at idle loads where exhaust temperatures were low enough to limit removal of SOA precursors in the oxidation catalyst. Use of biodiesel resulted in nearly identical POA and SOA compared to diesel. The effective SOA yield of diesel exhaust was similar to that of unburned diesel fuel. While OFRs can help study the multiday evolution, at low particle concentrations OFRs may not allow for complete gas/particle partitioning and bias the potential of precursors to form SOA.

  19. Development of an aerosol decontamination factor evaluation method using an aerosol spectrometer

    Energy Technology Data Exchange (ETDEWEB)

    Kanai, Taizo, E-mail: t-kanai@criepi.denken.or.jp; Furuya, Masahiro, E-mail: furuya@criepi.denken.or.jp; Arai, Takahiro, E-mail: t-arai@criepi.denken.or.jp; Nishi, Yoshihisa, E-mail: y-nishi@criepi.denken.or.jp

    2016-07-15

    Highlights: • Aerosol DF of each diameter is evaluable by using optical scattering method. • Outlet aerosol concentration shows exponential decay by the submergence. • This decay constant depends on the aerosol diameter. • Aerosol DF at water scrubber is described by simple equation. - Abstract: During a severe nuclear power plant accident, the release of fission products into containment and an increase in containment pressure are assumed to be possible. When the containment is damaged by excess pressure or temperature, radioactive materials are released. Pressure suppression pools, containment spray systems and a filtered containment venting system (FCVS) reduce containment pressure and reduce the radioactive release into the environment. These devices remove radioactive materials via various mechanisms. Pressure suppression pools remove radioactive materials by pool scrubbing. Spray systems remove radioactive materials by droplet−aerosol interaction. FCVS, which is installed in the exhaust system, comprises multi-scrubbers (venturi-scrubber, pool scrubbing, static mixer, metal−fiber filter and molecular sieve). For the particulate radioactive materials, its size affects the removal performance and a number of studies have been performed on the removal effect of radioactive materials. This study has developed a new means of evaluating aerosol removal efficiency. The aerosol number density of each effective diameter (light scattering equivalent diameter) is measured using an optical method, while the decontamination factor (DF) of each effective diameter is evaluated by the inlet outlet number density ratio. While the applicable scope is limited to several conditions (geometry of test section: inner diameter 500 mm × height 8.0 m, nozzle shape and air-water ambient pressure conditions), this study has developed a numerical model which defines aerosol DF as a function of aerosol diameter (d) and submergences (x).

  20. Motor Vehicle Exhaust Gas Suicide.

    Science.gov (United States)

    Routley, Virginia

    2007-01-01

    In many motorized countries, inhalation of carbon monoxide from motor vehicle exhaust gas (MVEG) has been one of the leading methods of suicide. In some countries it remains so (e.g., Australia 16.0% of suicides in 2005). Relative to other methods it is a planned method and one often used by middle-aged males. The study provides a review of countermeasures aimed at restricting this method of suicide. The prevention measures identified were catalytic converters (introduced to reduce carbon monoxide for environmental reasons); in-cabin sensors; exhaust pipe modification; automatic idling stops; and helpline signage at suicide "hotspots." Catalytic converters are now in 90% of new vehicles worldwide and literature supports them being associated with a reduction in exhaust-gassing suicides. There remain, however, accounts of exhaust-gas fatalities in modern vehicles, whether accidentally or by suicide. These deaths and also crashes from fatigue could potentially be prevented by in-cabin multi-gas sensors, these having been developed to the prototype stage. Helpline signage at an exhaust-gassing suicide "hotspot" had some success in reducing suicides. The evidence on method substitution and whether a reduction in MVEG suicides causes a reduction in total suicides is inconsistent.

  1. Modeling Macro- and Micro-Scale Turbulent Mixing and Chemistry in Engine Exhaust Plumes

    Science.gov (United States)

    Menon, Suresh

    1998-01-01

    Simulation of turbulent mixing and chemical processes in the near-field plume and plume-vortex regimes has been successfully carried out recently using a reduced gas phase kinetics mechanism which substantially decreased the computational cost. A detailed mechanism including gas phase HOx, NOx, and SOx chemistry between the aircraft exhaust and the ambient air in near-field aircraft plumes is compiled. A reduced mechanism capturing the major chemical pathways is developed. Predictions by the reduced mechanism are found to be in good agreement with those by the detailed mechanism. With the reduced chemistry, the computer CPU time is saved by a factor of more than 3.5 for the near-field plume modeling. Distributions of major chemical species are obtained and analyzed. The computed sensitivities of major species with respect to reaction step are deduced for identification of the dominant gas phase kinetic reaction pathways in the jet plume. Both the near field plume and the plume-vortex regimes were investigated using advanced mixing models. In the near field, a stand-alone mixing model was used to investigate the impact of turbulent mixing on the micro- and macro-scale mixing processes using a reduced reaction kinetics model. The plume-vortex regime was simulated using a large-eddy simulation model. Vortex plume behind Boeing 737 and 747 aircraft was simulated along with relevant kinetics. Many features of the computed flow field show reasonable agreement with data. The entrainment of the engine plumes into the wing tip vortices and also the partial detrainment of the plume were numerically captured. The impact of fluid mechanics on the chemical processes was also studied. Results show that there are significant differences between spatial and temporal simulations especially in the predicted SO3 concentrations. This has important implications for the prediction of sulfuric acid aerosols in the wake and may partly explain the discrepancy between past numerical studies

  2. The role of 2-methylglyceric acid and oligomer formation in the multiphase processing of secondary organic aerosol from isoprene and methacrolein photooxidation (CUMULUS project)

    Science.gov (United States)

    Giorio, Chiara; Brégonzio-Rozier, Lola; Siekmann, Frank; Cazaunau, Mathieu; Temime-Roussel, Brice; Langley DeWitt, Helen; Gratien, Aline; Michoud, Vincent; Pangui, Edouard; Morales, Sébastien; Ravier, Sylvain; Zielinski, Arthur T.; Tapparo, Andrea; Vermeylen, Reinhilde; Claeys, Magda; Voisin, Didier; Salque-Moreton, Guillaume; Kalberer, Markus; Doussin, Jean-François; Monod, Anne

    2017-04-01

    Biogenic volatile organic compounds (BVOCs) undergo atmospheric processing and form a wide range of oxidised and water-soluble compounds. These compounds could partition into atmospheric water droplets, and react within the aqueous phase producing higher molecular weight and less volatile compounds which could remain in the particle phase after water evaporation (Ervens et al., 2011). The aim of this work was the molecular characterisation of secondary organic aerosol (SOA) formed from the photooxidation of isoprene and methacrolein during cloud evapo-condensation cycles. The experiments were performed within the CUMULUS project (CloUd MULtiphase chemistry of organic compoUndS in the troposphere), at the 4.2 m3 stainless steel CESAM chamber at LISA (Brégonzio-Rozier et al., 2016). In each experiment, isoprene or methacrolein was photooxidised with HONO and clouds have been produced to study oxidation processes in a multiphase environment that well simulates the interactions between VOCs, SOA particles and cloud droplets. During all the experiments, SOA was characterised online with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and offline with gas chromatography mass spectrometry (GC-MS) and direct infusion nanoelectrospray ionisation high resolution mass spectrometry (nanoESI-HRMS). We observed that the main SOA compound in all experiments was 2-methylglyceric acid which undergoes oligomerisation reactions. A large number of long homologous series of oligomers were detected in all experiments, together with a complex co-oligomerised system made of monomers with a large variety of different structures. Comparison of SOA from multiphasic (smog chamber) experiments and samples from aqueous phase oxidation of methacrolein with •OH radical pointed out different types of oligomerisation reactions dominating the two different systems. Ervens et al. (2011) Atmos. Chem. Phys. 11, 11069 11102. Brégonzio-Rozier et al. (2016) Atmos. Chem. Phys

  3. pH of Aerosols in a Polluted Atmosphere: Source Contributions to Highly Acidic Aerosol.

    Science.gov (United States)

    Shi, Guoliang; Xu, Jiao; Peng, Xing; Xiao, Zhimei; Chen, Kui; Tian, Yingze; Guan, Xinbei; Feng, Yinchang; Yu, Haofei; Nenes, Athanasios; Russell, Armistead G

    2017-04-18

    Acidity (pH) plays a key role in the physical and chemical behavior of PM2.5. However, understanding of how specific PM sources impact aerosol pH is rarely considered. Performing source apportionment of PM2.5 allows a unique link of sources pH of aerosol from the polluted city. Hourly water-soluble (WS) ions of PM2.5 were measured online from December 25th, 2014 to June 19th, 2015 in a northern city in China. Five sources were resolved including secondary nitrate (41%), secondary sulfate (26%), coal combustion (14%), mineral dust (11%), and vehicle exhaust (9%). The influence of source contributions to pH was estimated by ISORROPIA-II. The lowest aerosol pH levels were found at low WS-ion levels and then increased with increasing total ion levels, until high ion levels occur, at which point the aerosol becomes more acidic as both sulfate and nitrate increase. Ammonium levels increased nearly linearly with sulfate and nitrate until approximately 20 μg m-3, supporting that the ammonium in the aerosol was more limited by thermodynamics than source limitations, and aerosol pH responded more to the contributions of sources such as dust than levels of sulfate. Commonly used pH indicator ratios were not indicative of the pH estimated using the thermodynamic model.

  4. Impact of aerosols on ice crystal size

    Directory of Open Access Journals (Sweden)

    B. Zhao

    2018-01-01

    Full Text Available The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (Rei, which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on Rei under different meteorological conditions using 9-year satellite observations. We find that the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the "Twomey effect" for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of Rei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of Rei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol–cloud radiative forcing produced by ice clouds.

  5. Optical manipulation of aerosol particle arrays

    Science.gov (United States)

    Reid, J. P.; Haddrell, A. E.; Walker, J. S.; Power, R.; Bones, D. L.; Davies, J. F.

    2011-10-01

    Aerosols play a crucial role in many areas of science, ranging from atmospheric chemistry and physics, to drug delivery to the lungs, combustion science and spray drying. The development of new methods to characterise the properties and dynamics of aerosol particles is of crucial importance if the complex role that particles play is to be more fully understood. Optical tweezers provide a valuable new tool to address fundamental questions in aerosol science. Single or multiple particles 1-15 μm in diameter can be manipulated over indefinite timescales using optical tweezing. Linear and non-linear Raman and fluorescence spectroscopies can be used to probe a particle's composition and size. In this paper we will report on the latest developments in the use of holographic optical trapping (HOT) to study aerosols. Although widely used to trap and manipulate arrays of particles in the condensed phase, the application of HOT to aerosols is still in its infancy. We will explore the opportunities provided by the formation of complex optical landscapes for controlling aerosol flow, for comparing the properties of multiple particles, for performing the first ever digital microfluidic operations in the aerosol phase and for examining interparticle interactions that can lead to coalescence/coagulation. Although aerosol coagulation is the primary process driving the evolution of particle size distributions, it remains very poorly understood. Using HOT, we can resolve the time-dependent motion of trapped particles and the light scattering from particles during the coalescence process.

  6. Aerosol gels

    Science.gov (United States)

    Sorensen, Christopher M. (Inventor); Chakrabarti, Amitabha (Inventor); Dhaubhadel, Rajan (Inventor); Gerving, Corey (Inventor)

    2010-01-01

    An improved process for the production of ultralow density, high specific surface area gel products is provided which comprises providing, in an enclosed chamber, a mixture made up of small particles of material suspended in gas; the particles are then caused to aggregate in the chamber to form ramified fractal aggregate gels. The particles should have a radius (a) of up to about 50 nm and the aerosol should have a volume fraction (f.sub.v) of at least 10.sup.-4. In preferred practice, the mixture is created by a spark-induced explosion of a precursor material (e.g., a hydrocarbon) and oxygen within the chamber. New compositions of matter are disclosed having densities below 3.0 mg/cc.

  7. Heterogeneous Chemistry: Understanding Aerosol/Oxidant Interactions

    Energy Technology Data Exchange (ETDEWEB)

    Joyce E. Penner

    2005-03-14

    Global radiative forcing of nitrate and ammonium aerosols has mostly been estimated from aerosol concentrations calculated at thermodynamic equilibrium or using approximate treatments for their uptake by aerosols. In this study, a more accurate hybrid dynamical approach (DYN) was used to simulate the uptake of nitrate and ammonium by aerosols and the interaction with tropospheric reactive nitrogen chemistry in a three-dimensional global aerosol and chemistry model, IMPACT, which also treats sulfate, sea salt and mineral dust aerosol. 43% of the global annual average nitrate aerosol burden, 0.16 TgN, and 92% of the global annual average ammonium aerosol burden, 0.29 TgN, exist in the fine mode (D<1.25 {micro}m) that scatters most efficiently. Results from an equilibrium calculation differ significantly from those of DYN since the fraction of fine-mode nitrate to total nitrate (gas plus aerosol) is 9.8%, compared to 13% in DYN. Our results suggest that the estimates of aerosol forcing from equilibrium concentrations will be underestimated. We also show that two common approaches used to treat nitrate and ammonium in aerosol in global models, including the first-order gas-to-particle approximation based on uptake coefficients (UPTAKE) and a hybrid method that combines the former with an equilibrium model (HYB), significantly overpredict the nitrate uptake by aerosols especially that by coarse particles, resulting in total nitrate aerosol burdens higher than that in DYN by +106% and +47%, respectively. Thus, nitrate aerosol in the coarse mode calculated by HYB is 0.18 Tg N, a factor of 2 more than that in DYN (0.086 Tg N). Excessive formation of the coarse-mode nitrate in HYB leads to near surface nitrate concentrations in the fine mode lower than that in DYN by up to 50% over continents. In addition, near-surface HNO{sub 3} and NO{sub x} concentrations are underpredicted by HYB by up to 90% and 5%, respectively. UPTAKE overpredicts the NO{sub x} burden by 56% and near

  8. Electrically Driven Technologies for Radioactive Aerosol Abatement

    Energy Technology Data Exchange (ETDEWEB)

    David W. DePaoli; Ofodike A. Ezekoye; Costas Tsouris; Valmor F. de Almeida

    2003-01-28

    The purpose of this research project was to develop an improved understanding of how electriexecy driven processes, including electrocoalescence, acoustic agglomeration, and electric filtration, may be employed to efficiently treat problems caused by the formation of aerosols during DOE waste treatment operations. The production of aerosols during treatment and retrieval operations in radioactive waste tanks and during thermal treatment operations such as calcination presents a significant problem of cost, worker exposure, potential for release, and increased waste volume.

  9. Semiconductor industry wafer fab exhaust management

    CERN Document Server

    Sherer, Michael J

    2005-01-01

    Given the myriad exhaust compounds and the corresponding problems that they can pose in an exhaust management system, the proper choice of such systems is a complex task. Presenting the fundamentals, technical details, and general solutions to real-world problems, Semiconductor Industry: Wafer Fab Exhaust Management offers practical guidance on selecting an appropriate system for a given application. Using examples that provide a clear understanding of the concepts discussed, Sherer covers facility layout, support facilities operations, and semiconductor process equipment, followed by exhaust types and challenges. He reviews exhaust point-of-use devices and exhaust line requirements needed between process equipment and the centralized exhaust system. The book includes information on wet scrubbers for a centralized acid exhaust system and a centralized ammonia exhaust system and on centralized equipment to control volatile organic compounds. It concludes with a chapter devoted to emergency releases and a separ...

  10. Aircraft specific exhaust emissions

    Energy Technology Data Exchange (ETDEWEB)

    Lecht, M.; Deidewig, F.; Doepelheuer, A. [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Koeln (Germany). Inst. fuer Antriebstechnik

    1997-12-01

    The objective of this work to calculate essential species of aircraft emissions has been approached by a combination of different tasks. First of all engine performance and emission correlation has been modelled taking sea level static measurements from the engine certification process as a reference. At second a flight simulation program has been modified to couple aircraft and engine performance along a flight mission profile. By this for a selected number of aircraft/engine combinations the emissions of NO{sub x}, CO and HC as well as fuel burn for short, medium and long haul flights have been calculated and finally adapted to a specified format of flight distance and altitude increments. Sensitivity studies of the change of emissions along the cruise section showed a 30% decrease of the NO{sub x} emission rate until the end of cruise. Differences of ambient air temperature from ISA conditions will have a substantial impact on NO{sub x}, CO and HC emissions rather than on mission fuel. (orig.) 144 figs., 42 tabs., 497 refs.

  11. Chemical processes in the turbine and exhaust nozzle

    Energy Technology Data Exchange (ETDEWEB)

    Lukachko, S.P.; Waitz, I.A. [Massachusetts Inst. of Tech., Cambridge, MA (United States). Aero-Environmental Lab.; Miake-Lye, R.C.; Brown, R.C.; Anderson, M.R. [Aerodyne Research, Inc., Billerica, MA (United States); Dawes, W.N. [University Engineering Dept., Cambridge (United Kingdom). Whittle Lab.

    1997-12-31

    The objective is to establish an understanding of primary pollutant, trace species, and aerosol chemical evolution as engine exhaust travels through the nonuniform, unsteady flow fields of the turbine and exhaust nozzle. An understanding of such processes is necessary to provide accurate inputs for plume-wake modeling efforts and is therefore a critical element in an assessment of the atmospheric effects of both current and future aircraft. To perform these studies, a numerical tool was developed combining the calculation of chemical kinetics and one-, two-, or three-dimensional (1-D, 2-D, 3-D) Reynolds-averaged flow equations. Using a chemistry model that includes HO{sub x}, NO{sub y}, SO{sub x}, and CO{sub x} reactions, several 1-D parametric analyses were conducted for the entire turbine and exhaust nozzle flow path of a typical advanced subsonic engine to understand the effects of various flow and chemistry uncertainties on a baseline 1-D result. These calculations were also used to determine parametric criteria for judging 1-D, 2-D, and 3-D modeling requirements as well as to provide information about chemical speciation at the nozzle exit plane. (author) 9 refs.

  12. Aerosol typing - key information from aerosol studies

    Science.gov (United States)

    Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  13. Sea Spray Aerosols

    DEFF Research Database (Denmark)

    Butcher, Andrew Charles

    Aerosols are important climactically. Their specific emissions are key to reducing the uncertainty in global climate models. Marine aerosols make up the largest source of primary aerosols to the Earth's atmosphere. Uncertainty in marine aerosol mass and number flux lies in separating primary emis...... with decreasing temperature. Unique surface images of bubble size distributions allow the investigation of temperature, bubble size, and particle production......Aerosols are important climactically. Their specific emissions are key to reducing the uncertainty in global climate models. Marine aerosols make up the largest source of primary aerosols to the Earth's atmosphere. Uncertainty in marine aerosol mass and number flux lies in separating primary...... entrainment may account for the large discrepancy in energy input for the two systems. In the third study, the temperature dependence of sea spray aerosol production is probed with the use of a highly stable temperature controlled plunging jet. Similar to previous studies, particle production increases...

  14. Change in global aerosol composition since preindustrial times

    Directory of Open Access Journals (Sweden)

    K. Tsigaridis

    2006-01-01

    Full Text Available To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=, ammonium (NH4+, nitrate (NO3−, black carbon (BC, sea-salt, dust, primary and secondary organics (POA and SOA with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD

  15. Aerosol droplets: Nucleation dynamics and photokinetics

    Science.gov (United States)

    Signorell, Ruth

    This talk addresses two fundamental aerosol processes that play a pivotal role in atmospheric processes: The formation dynamics of aerosol particles from neutral gas phase precursors and photochemical reactions in small aerosol droplets induced by ultraviolet and visible light. Nucleation is the rate determining step of aerosol particle formation. The idea behind nucleation is that supersaturation of a gas leads to the formation of a critical cluster, which quickly grows into larger aerosol particles. We discuss an experiment for studying the size and chemical composition of critical clusters at the molecular level. Much of the chemistry happening in planetary atmospheres is driven by sunlight. Photochemical reactions in small aerosol particles play a peculiar role in this context. Sunlight is strongly focused inside these particles which leads to a natural increase in the rates of photochemical reactions in small particles compared with the bulk. This ubiquitous phenomenon has been recognised but so far escaped direct observation and quantification. The development of a new experimental setup has finally made it possible to directly observe this nanofocusing effect in droplet photokinetics. This work was supported by the Swiss National Science Foundation (SNSF) and ETH Zurich.

  16. Exhaust Gas Scrubber Washwater Effluent

    Science.gov (United States)

    2011-11-01

    10 Sulfur Content of Certain Liquid Fuels Exhaust Gas Scrubber Washwater Effluent...diesel and gasoline components DIN Dissolved inorganic nitrogen THC Total hydrocarbon TKN Total Kjeldahl nitrogen HEM Hexane extractable...Benefit Analysis to support the impact assessment accompanying the revision of Directive 1999/32/EC on the sulfur content of certain liquid fuels

  17. Ship exhaust gas plume cooling

    NARCIS (Netherlands)

    Schleijpen, H.M.A.; Neele, P.P.

    2004-01-01

    The exhaust gas plume is an important and sometimes dominating contributor to the infrared signature of ships. Suppression of the infrared ship signatures has been studied by TNO for the Royal Netherlands Navy over considerable time. This study deals with the suppression effects, which can be

  18. Influence of crustal dust and sea spray supermicron particle concentrations and acidity on inorganic NO3- aerosol during the 2013 Southern Oxidant and Aerosol Study

    Science.gov (United States)

    Allen, H. M.; Draper, D. C.; Ayres, B. R.; Ault, A.; Bondy, A.; Takahama, S.; Modini, R. L.; Baumann, K.; Edgerton, E.; Knote, C.; Laskin, A.; Wang, B.; Fry, J. L.

    2015-09-01

    Inorganic aerosol composition was measured in the southeastern United States, a region that exhibits high aerosol mass loading during the summer, as part of the 2013 Southern Oxidant and Aerosol Study (SOAS) campaign. Measurements using a Monitor for AeRosols and GAses (MARGA) revealed two periods of high aerosol nitrate (NO3-) concentrations during the campaign. These periods of high nitrate were correlated with increased concentrations of supermicron crustal and sea spray aerosol species, particularly Na+ and Ca2+, and with a shift towards aerosol with larger (1 to 2.5 μm) diameters. We suggest this nitrate aerosol forms by multiphase reactions of HNO3 and particles, reactions that are facilitated by transport of crustal dust and sea spray aerosol from a source within the United States. The observed high aerosol acidity prevents the formation of NH4NO3, the inorganic nitrogen species often dominant in fine-mode aerosol at higher pH. Calculation of the rate of the heterogeneous uptake of HNO3 on mineral aerosol supports the conclusion that aerosol NO3- is produced primarily by this process, and is likely limited by the availability of mineral cation-containing aerosol surface area. Modeling of NO3- and HNO3 by thermodynamic equilibrium models (ISORROPIA II and E-AIM) reveals the importance of including mineral cations in the southeastern United States to accurately balance ion species and predict gas-aerosol phase partitioning.

  19. Evaluation of aerosol processes between roadside and neighbourhood scale

    Science.gov (United States)

    Karl, Matthias; Kukkonen, Jaakko; Pirjola, Liisa; Keuken, Menno P.

    2015-04-01

    Particle emissions from road transport include vehicle exhaust emissions, tire/brake wear and re-suspension of road dust. Vehicle exhaust emissions usually constitute the most significant source of ultrafine particles (UFP), i.e. particles with diameters air pollution legislation. UFP emitted from road traffic are subject to complex dilution and transformation processes in the urban environment. This model study evaluates the influence of aerosol processes on PN concentration on the spatial and temporal range between the roadside, typically represented by measurements at a traffic monitoring site, and the neighbourhood scale, extending from several hundred meters to several kilometres. Several dispersion scenarios for the cities Oslo, Helsinki and Rotterdam were simulated using the multicomponent aerosol dynamics process model MAFOR, approximating dilution by a power-law function. Aerosol processes considered in this study were condensation/evaporation of n-alkanes, coagulation and the dry deposition of particles. Under typical dispersion conditions dilution clearly dominated the change of total PN on the neighbourhood scale. Dry deposition and coagulation of particles were identified to be the most important aerosol dynamical processes controlling the removal of particles from emitted from vehicular exhaust on urban time scales. The effect of condensation/evaporation of organic vapours emitted by vehicles on particle numbers and on particle size distributions was examined. A simplified parameterization for the implementation of coagulation and dry deposition of particles in urban air quality models is presented. Further work is needed to validate size segregated PN concentration distributions modelled by the urban models.

  20. Microphysical processing of aerosol particles in orographic clouds

    Directory of Open Access Journals (Sweden)

    S. Pousse-Nottelmann

    2015-08-01

    aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener–Bergeron–Findeisen (WBF process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number

  1. Recent advances in investigations of toxicity of automotive exhaust

    Science.gov (United States)

    Stupfel, Maurice

    1976-01-01

    The influence of auto exhaust on man's health is difficult to gauge considering the intricacy of human environmental urban stresses and particularly of other air polluting (industrial, domestic) emissions. Epidemiological surveys made in road tunnel employees and in traffic officers have not demonstrated specific effects and have often been complicated by cigarette smoking as a factor. Long-term animal experiments run mostly on small rodents give evidence of little effect of the pathological actions of dilutions such as those encountered in high polluted cities. However the acute toxicity of gasoline exhaust emission is well known and mostly due to carbon monoxide. Considering the different types of cycles and operating conditions of vehicles (gasoline and diesel), auto exhaust gases constitute no more a chemical entity than they show, a definite toxicity. A great number of substances that they contain (nitrogen oxides, aldehydes, antiknock additives, heavy metals, possible catalysts are highly toxic as shown by in vivo and in vitro (mutagenic) tests. Interactions of the components are for the moment ignored or poorly understood. Besides, the evolution of the physicochemical properties and natures of the auto exhaust emission in the gaseous biotope of man under determined conditions of ultraviolet irradiation, temperature, and hygrometry provoke the formation of secondary products such as oxidants and ozone. Several experiments show clearly that irradiation increases the toxicity of auto exhaust significantly. For these reasons, geographical, meteorological, and chronological (circadian and seasonal) factors should be taken into consideration, especially with regard to emission standards. PMID:67944

  2. Aerosol mobility size spectrometer

    Science.gov (United States)

    Wang, Jian; Kulkarni, Pramod

    2007-11-20

    A device for measuring aerosol size distribution within a sample containing aerosol particles. The device generally includes a spectrometer housing defining an interior chamber and a camera for recording aerosol size streams exiting the chamber. The housing includes an inlet for introducing a flow medium into the chamber in a flow direction, an aerosol injection port adjacent the inlet for introducing a charged aerosol sample into the chamber, a separation section for applying an electric field to the aerosol sample across the flow direction and an outlet opposite the inlet. In the separation section, the aerosol sample becomes entrained in the flow medium and the aerosol particles within the aerosol sample are separated by size into a plurality of aerosol flow streams under the influence of the electric field. The camera is disposed adjacent the housing outlet for optically detecting a relative position of at least one aerosol flow stream exiting the outlet and for optically detecting the number of aerosol particles within the at least one aerosol flow stream.

  3. Los Angeles Summer Midday Particulate Carbon: Primary and Secondary Aerosol

    OpenAIRE

    Turpin, Barbara J.; Huntzicker, James J.; Larson, Susan M.; Cass, Glen R.

    1991-01-01

    Aerosol sampling during photochemically active times across the Los Angeles Basin has provided evidence of secondary formation of organic aerosol from gas-phase precursors at midday. Ambient organic carbon/elemental carbon ratios exceeded the estimated ratio of organic carbon/elemental carbon in primary source emissions on most sampling days at all sites. The concentration of secondary organic aerosol was calculated by using ambient data and estimates of the organic ca...

  4. Characteristics of inorganic aerosol formation over ammonia-poor and ammonia-rich areas in the Pearl River Delta region, China

    Science.gov (United States)

    Yin, Shasha; Huang, Zhijiong; Zheng, Junyu; Huang, Xiaobo; Chen, Duohong; Tan, Haobo

    2018-03-01

    A well-evaluated Comprehensive Air quality Model with extensions (CAMx) was used to simulate concentrations of secondary inorganic aerosols in fine particulate matter (PM2.5) over Pearl River Delta (PRD) region during two separate months (April and October) in 2013. An indicator of adjusted gas ratio (AdjGR) was used to characterize PM chemistry under both NH3-poor (NP) and NH3-rich (NR) conditions as well as to identify their respective spatiotemporal patterns at different PM2.5 levels. The results were as follows: (1) Based on both observed molar ratio of [NH4+]/[SO42-] and modeled AdjGR, NR and NP conditions exhibited diurnal, daily, and seasonal variations. (2) A larger area in PRD had NP conditions over the two months when pollution was apparent; this NP region tended to occur downwind of PRD in October and the central region of PRD in April, with high PM2.5 concentrations in both. (3) This wider NP distribution could be related to higher nitrogen oxidation ratio (NOR), with more NOx converting to nitrate. Under conditions of higher pollution, there were relative lower degree of sulfate neutralization (DSN) and particle neutralization ratio (PNR). This supports the claim that NH3 may not be fully neutralized by SO42-. (4) Modeled AdjGR displayed clear hourly variations, with the lowest levels occurring in the afternoon. Reducing NH3 emission is not as efficient as NOx at increasing evening nitrate concentrations. (5) To mitigate PM2.5 pollution even further, a greater reduction of NH3 should be suggested in chemical regions transiting to NR condition when there are lower SO2 and NOx emissions.

  5. Exhaust System Reinforced by Jet Flow

    DEFF Research Database (Denmark)

    Pedersen, Lars Germann; Nielsen, Peter V.

    Since 1985 the University of Aalborg and Nordfab A/S have been working on an exhaust principle which is quite different from traditional exhaust systems. The REEXS principle (Reinforced Exhaust System), which originally was designed for the agricultural sector, is particularly well......-suited for industrial ventilation purposes. With the REEXS principle it is possible to create a flow pattern in front of the exhaust opening which will have a considerable influence on the general flow in a given room....

  6. Aerosol Angstrom Absorption Coefficient Comparisons during MILAGRO.

    Science.gov (United States)

    Marley, N. A.; Marchany-Rivera, A.; Kelley, K. L.; Mangu, A.; Gaffney, J. S.

    2007-12-01

    Measurements of aerosol absorption were obtained as part of the MAX-Mex component of the MILAGRO field campaign at site T0 (Instituto Mexicano de Petroleo in Mexico City) by using a 7-channel aethalometer (Thermo- Anderson) during the month of March, 2006. The absorption measurements obtained in the field at 370, 470, 520, 590, 660, 880, and 950 nm were used to determine the aerosol Angstrom absorption exponents by linear regression. Since, unlike other absorbing aerosol species (e.g. humic like substances, nitrated PAHs), black carbon absorption is relatively constant from the ultraviolet to the infrared with an Angstrom absorption exponent of -1 (1), a comparison of the Angstrom exponents can indicate the presence of aerosol components with an enhanced UV absorption over that expected from BC content alone. The Angstrom exponents determined from the aerosol absorption measurements obtained in the field varied from - 0.7 to - 1.3 during the study and was generally lower in the afternoon than the morning hours, indicating an increase in secondary aerosol formation and photochemically generated UV absorbing species in the afternoon. Twelve-hour integrated samples of fine atmospheric aerosols (Petroleo (IMP) and CENICA.

  7. Toxicity of aged gasoline exhaust particles to normal and diseased airway epithelia.

    Science.gov (United States)

    Künzi, Lisa; Krapf, Manuel; Daher, Nancy; Dommen, Josef; Jeannet, Natalie; Schneider, Sarah; Platt, Stephen; Slowik, Jay G; Baumlin, Nathalie; Salathe, Matthias; Prévôt, André S H; Kalberer, Markus; Strähl, Christof; Dümbgen, Lutz; Sioutas, Constantinos; Baltensperger, Urs; Geiser, Marianne

    2015-06-29

    Particulate matter (PM) pollution is a leading cause of premature death, particularly in those with pre-existing lung disease. A causative link between particle properties and adverse health effects remains unestablished mainly due to complex and variable physico-chemical PM parameters. Controlled laboratory experiments are required. Generating atmospherically realistic aerosols and performing cell-exposure studies at relevant particle-doses are challenging. Here we examine gasoline-exhaust particle toxicity from a Euro-5 passenger car in a uniquely realistic exposure scenario, combining a smog chamber simulating atmospheric ageing, an aerosol enrichment system varying particle number concentration independent of particle chemistry, and an aerosol deposition chamber physiologically delivering particles on air-liquid interface (ALI) cultures reproducing normal and susceptible health status. Gasoline-exhaust is an important PM source with largely unknown health effects. We investigated acute responses of fully-differentiated normal, distressed (antibiotics-treated) normal, and cystic fibrosis human bronchial epithelia (HBE), and a proliferating, single-cell type bronchial epithelial cell-line (BEAS-2B). We show that a single, short-term exposure to realistic doses of atmospherically-aged gasoline-exhaust particles impairs epithelial key-defence mechanisms, rendering it more vulnerable to subsequent hazards. We establish dose-response curves at realistic particle-concentration levels. Significant differences between cell models suggest the use of fully-differentiated HBE is most appropriate in future toxicity studies.

  8. High Temperature Resistant Exhaust Valve Spindle

    DEFF Research Database (Denmark)

    Bihlet, Uffe Ditlev

    of the engine, new high temperature alloys are required for a specific engine component, the exhaust valve spindle. Two alloys are used for an exhaust valve spindle; one for the bottom of the spindle, and one for the spindle seat. Being placed in the exhaust gas stream, combustion products such as V2O5 and Na2...

  9. The Chemical Composition and Mixing State of Sea Spray Aerosol and Organic Aerosol in the Winter-Spring Arctic

    Science.gov (United States)

    Kirpes, R.; Bondy, A. L.; Bonanno, D.; Moffet, R.; Wang, B.; Laskin, A.; Ault, A. P.; Pratt, K.

    2016-12-01

    The Arctic region is undergoing rapid transformations and loss of sea ice due to climate change. With increased sea ice fracturing resulting in greater open ocean surface, winter emissions of sea spray aerosol (SSA) are expected to be increasing. Additionally, during the winter-spring transition, Arctic haze contributes to the Arctic aerosol budget. The magnitude of aerosol climate effects depends on the aerosol composition and mixing state (distribution of chemical species within and between particles). However, few studies of aerosol chemistry have been conducted in the winter Arctic, despite it being a time when aerosol impacts on clouds are expected to be significant. To study aerosol composition and mixing state in the winter Arctic, atmospheric particles were collected near Barrow, Alaska in January and February 2014 for off-line individual particle chemical analysis. SSA was the most prevalent particle type observed. Sulfate and nitrate were observed to be internally mixed with SSA and organic aerosol. Greater than 98% of observed SSA particles contained organic content, with 15-35% organic volume fraction on average for individual particles. The SSA organic compounds consisted of carbohydrates, lipids, and fatty acids found in the seawater surface microlayer. SSA was determined to be emitted from open leads, while transported sulfate and nitrate contributed to aging of SSA and organic aerosol. Determining the aerosol chemical composition and mixing state in the winter Arctic will further the understanding of how individual aerosol particles impact climate through radiative effects and cloud formation.

  10. Aerosols and Climate

    Indian Academy of Sciences (India)

    How do Aerosols Influence Climate? Although making up only one part in a billion of the mass of the atmosphere, aerosols have the potential to significantly influ- ence the climate. The global impact of aerosol is assessed as the change imposed on planetary radiation measured in Wm-2, which alters the global temperature ...

  11. Aerosols and Climate

    Indian Academy of Sciences (India)

    Aerosols and Climate · Slide 2 · Slide 3 · Slide 4 · Slide 5 · Slide 6 · Principal efforts in improving the understanding of Climate impact of aerosols - · Slide 8 · Observations of Aerosol – from space (Spatial variation) · AOD around Indian region from AVHRR · Dust absorption efficiency over Great Indian Desert from Satellite ...

  12. Aerosol distribution apparatus

    Science.gov (United States)

    Hanson, W.D.

    An apparatus for uniformly distributing an aerosol to a plurality of filters mounted in a plenum, wherein the aerosol and air are forced through a manifold system by means of a jet pump and released into the plenum through orifices in the manifold. The apparatus allows for the simultaneous aerosol-testing of all the filters in the plenum.

  13. Numerical modelling of the internal mixing by coagulation of black carbon particles in aircraft exhaust

    Energy Technology Data Exchange (ETDEWEB)

    Ohlsson, S.; Stroem, J. [Stockholm Univ. (Sweden). Dept. of Meteorology

    1997-12-31

    When exhaust gases from an aircraft engine mix with ambient air the humidity may reach water saturation and water droplets will form on the available cloud condensation nuclei (CCN). It is still not resolved if the CCN, on which the cloud droplets form, are mainly particles present in the ambient air or particles emitted by the aircraft. It the exhaust from a jet engine the particles are believed to consist mainly of black carbon (BC) and sulfate. The aim is to study, with the help of a numerical model, how a two-component aerosol (i.e. BC and sulfate) in an exhaust trail may be transformed in terms of hygroscopicity by coagulation mixing and how this may depend on the sulfur content in the fuel. (R.P.) 15 refs.

  14. Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China

    Science.gov (United States)

    Zheng, B.; Zhang, Q.; Zhang, Y.; He, K. B.; Wang, K.; Zheng, G. J.; Duan, F. K.; Ma, Y. L.; Kimoto, T.

    2015-02-01

    Severe regional haze pollution events occurred in eastern and central China in January 2013, which had adverse effects on the environment and public health. Extremely high levels of particulate matter with aerodynamic diameter of 2.5 μm or less (PM2.5) with dominant components of sulfate and nitrate are responsible for the haze pollution. Although heterogeneous chemistry is thought to play an important role in the production of sulfate and nitrate during haze episodes, few studies have comprehensively evaluated the effect of heterogeneous chemistry on haze formation in China by using the 3-D models due to of a lack of treatments for heterogeneous reactions in most climate and chemical transport models. In this work, the WRF-CMAQ model with newly added heterogeneous reactions is applied to East Asia to evaluate the impacts of heterogeneous chemistry and the meteorological anomaly during January 2013 on regional haze formation. As the parameterization of heterogeneous reactions on different types of particles is not well established yet, we arbitrarily selected the uptake coefficients from reactions on dust particles and then conducted several sensitivity runs to find the value that can best match observations. The revised CMAQ with heterogeneous chemistry not only captures the magnitude and temporal variation of sulfate and nitrate, but also reproduces the enhancement of relative contribution of sulfate and nitrate to PM2.5 mass from clean days to polluted haze days. These results indicate the significant role of heterogeneous chemistry in regional haze formation and improve the understanding of the haze formation mechanisms during the January 2013 episode.

  15. Electrophysiologic Study of Exhaustive Exercise

    Directory of Open Access Journals (Sweden)

    MA Babaee Bigi

    2010-12-01

    Full Text Available Background: Exhaustive exercise is well known to pose a variety ofhealth hazards, such as sudden cardiac death reported in ultra-marathon runners.Depressed parasympathetic tone is associated with increased risk of suddencardiac death, thus parasympathetic withdrawal in post-exercise phase may be ahigh risk period for sudden death. To date, the effect on cardiacelectrophysiology after exhaustive strenuous exercise has not been described.The aim of this study was to evaluate the impact of severe exhaustive exerciseon cardiac electrophysiology.Methods: The subjects in ranger training were invited to participatein this prospective study. The parameters measured consisted of PR interval, QRSduration, and macro T wave alternans as well as corrected QT, QTc dispersion,Tpeak –Tend interval and Tpeak –Tend dispersion.Results: The study group consisted of 40 consecutive male rangers whocompleted training and the control group (22 healthy age and height matched malesubjects. In regard to electrocardiographic criteria, no differences were foundbetween rangers before and after training program. In respect of therepolarization markers, there were no significant differences between therangers before and after training program.

  16. Model of optical response of marine aerosols to Forbush decreases

    DEFF Research Database (Denmark)

    Bondo, Torsten; Enghoff, Martin Andreas Bødker; Svensmark, Henrik

    2010-01-01

    In order to elucidate the effect of galactic cosmic rays on cloud formation, we investigate the optical response of marine aerosols to Forbush decreases - abrupt decreases in galactic cosmic rays - by means of modeling. We vary the nucleation rate of new aerosols, in a sectional coagulation...

  17. Marine aerosol production: a review of the current knowledge

    NARCIS (Netherlands)

    O'Dowd, C.D.; Leeuw, G. de

    2007-01-01

    The current knowledge in primary and secondary marine aerosol formation is reviewed. For primary marine aerosol source functions, recent source functions have demonstrated a significant flux of submicrometre particles down to radii of 20 nm. Moreover, the source functions derived from different

  18. Role of ammonium ion and transition metals in the formation of secondary organic aerosol and metallo-organic complex within fog processed ambient deliquescent submicron particles collected in central part of Indo-Gangetic Plain.

    Science.gov (United States)

    Singh, Dharmendra Kumar; Gupta, Tarun

    2017-08-01

    In this study we observed the role of ammonium ion (NH4+) and transition metals (Fe, Mn, Cr, and Cu) present in ambient submicron particles in stabilizing and enhancing the yield of water soluble organic carbon (WSOC). A good correlation of WSOC with transition metals and NH4+ was found (R2 = 0.87 and 0.71), respectively within foggy episode collected ambient PM1 (particles having aerodynamic diameter ≤1.0 μm) suggesting plausibleness of alternate oxidation (primarily various carbonyls into their respective organic acids, esters and other derivatives.) and aging mechanisms. Molar concentration of ammonium ion was observed to be exceeded over and above to require in neutralizing the sulphate and nitrate which further hints its role in the neutralization, stabilization and enhancement of subset of WSOC such as water soluble organic acids. Transition metals were further apportioned using enrichment factor analysis. The source of Fe, Mn, and Cr was found to be crustal and Cu was tagged to anthropogenic origin. This study also described the plausible role of significant predictors (Fe and Cu) in the secondary organic aerosol (SOA) formation through effect of Fenton chemistry. Mass-to-charge ratio of identified oxalic acid from our published recent field study (carried out from same sampling location) was used for understanding the possible metallo-organic complex with Fe supports the substantial role of Fe in SOA formation in the deliquescent submicron particles facilitated by aqueous-phase chemistry. Copyright © 2017 Elsevier Ltd. All rights reserved.

  19. Atmospheric Degradation Initiated by OH Radicals of the Potential Foam Expansion Agent, CF3(CF2)2CH═CH2 (HFC-1447fz): Kinetics and Formation of Gaseous Products and Secondary Organic Aerosols.

    Science.gov (United States)

    Jiménez, Elena; González, Sergio; Cazaunau, Mathieu; Chen, Hui; Ballesteros, Bernabé; Daële, Véronique; Albaladejo, José; Mellouki, Abdelwahid

    2016-02-02

    The assessment of the atmospheric impact of the potential foam expansion agent, CF3(CF2)2CH═CH2 (HFC-1447fz), requires the knowledge of its degradation routes, oxidation products, and radiative properties. In this paper, the gas-phase reactivity of HFC-1447fz with OH radicals is presented as a function of temperature, obtaining kOH (T = 263-358 K) = (7.4 ± 0.4) × 10(-13)exp{(161 ± 16)/T} (cm(3)·molecule(-1)·s(-1)) (uncertainties: ±2σ). The formation of gaseous oxidation products and secondary organic aerosols (SOAs) from the OH + HFC-1447fz reaction was investigated in the presence of NOx at 298 K. CF3(CF2)2CHO was observed at low- and high-NOx conditions. Evidence of SOA formation (ultrafine particles in the range 10-100 nm) is reported with yields ranging from 0.12 to 1.79%. In addition, the absolute UV (190-368 nm) and IR (500-4000 cm(-1)) absorption cross-sections of HFC-1447fz were determined at room temperature. No appreciable absorption in the solar actinic region (λ > 290 nm) was observed, leaving the removal by OH radicals as the main atmospheric loss process for HFC-1447fz. The major contribution of the atmospheric loss of HFC-1447fz is due to OH reaction (84%), followed by ozone (10%) and chlorine atoms (6%). Correction of the instantaneous radiative efficiency (0.36 W m(-2)·ppbv(-1)) with the relatively short lifetime of HFC-1447fz (ca. 8 days) implies that its global warming potential at a time horizon of 100 year is negligible (0.19) compared to that of HCFC-141b (782) and to that of modern foam-expansion blowing agents (148, 882, and 804 for HFC-152a, HFC-245fa and HFC-365mfc, respectively).

  20. Fractionation of Stable Isotopes in Atmospheric Aerosol Reactions

    DEFF Research Database (Denmark)

    Meusinger, Carl

    Aerosols - particles suspended in air - are the single largest uncertainty in our current understanding of Earth's climate. They also affect human health, infrastructure and ecosystems. Aerosols are emitted either directly into the atmosphere or are formed there for instance in response to chemical...... reactions and undergo complex chemical and physical changes during their lifetimes. In order to assess processes that form and alter aerosols, information provided by stable isotopes can be used to help constrain estimates on the strength of aerosol sources and sinks. This thesis studies (mass......-independent) fractionation processes of stable isotopes of C, N, O and S in order to investigate three different systems related to aerosols: 1. Post-depositional processes of nitrate in snow that obscure nitrate ice core records 2. Formation and aging of secondary organic aerosol generated by ozonolysis of X...

  1. Protection of air in premises and environment against beryllium aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Bitkolov, N.Z.; Vishnevsky, E.P.; Krupkin, A.V. [Research Inst. of Industrial and Marine Medicine, St. Petersburg (Russian Federation)

    1998-01-01

    First and foremost, the danger of beryllium aerosols concerns a possibility of their inhalation. The situation is aggravated with high biological activity of the beryllium in a human lung. The small allowable beryllium aerosols` concentration in air poses a rather complex and expensive problem of the pollution prevention and clearing up of air. The delivery and transportation of beryllium aerosols from sites of their formation are defined by the circuit of ventilation, that forms aerodynamics of air flows in premises, and aerodynamic links between premises. The causes of aerosols release in air of premises from hoods, isolated and hermetically sealed vessels can be vibrations, as well as pulses of temperature and pressure. Furthermore, it is possible the redispersion of aerosols from dirty surfaces. The effective protection of air against beryllium aerosols at industrial plants is provided by a complex of hygienic measures: from individual means of breath protection up to collective means of the prevention of air pollution. (J.P.N.)

  2. Homologous series of low molecular weight (C1-C10) monocarboxylic acids, benzoic acid and hydroxyacids in fine-mode (PM2.5) aerosols over the Bay of Bengal: Influence of heterogeneity in air masses and formation pathways

    Science.gov (United States)

    Boreddy, Suresh K. R.; Mochizuki, Tomoki; Kawamura, Kimitaka; Bikkina, Srinivas; Sarin, M. M.

    2017-10-01

    Low molecular weight monocarboxylic acids (LMW monoacids) are most abundant volatile organic compounds (VOCs) in the atmosphere and often act as important contributors to the acidity of precipitation in addition to inorganic acids. However, there is a large uncertainty in the sources and secondary formations of these acids in the atmosphere. This study reports homologous series of LMW monoacids, including normal (C1-C10), branched chain (iC4-iC6), aromatic (benzoic acid) and hydroxyacids (lactic and glycolic acids) in the fine-mode (PM2.5) aerosols collected over the Bay of Bengal (BoB) during a winter cruise (December 2008 to January 2009). The samples were associated with two distinct continental air masses arriving from the Indo-Gangetic Plain (IGP-outflow) and Southeast Asia (SEA-outflow). The molecular distributions of organic acids are characterized by the dominance of formic acid (C1) followed by acetic acid (C2) and nonanoic acid (C9) in the IGP-outflow, whereas dominance of C1 or C9 was observed in the SEA-outflow followed by C2. Formic-to-acetic acid (C1/C2) ratios were higher than unity (mean: 1.3 ± 0.3) in the IGP-outflow, whereas they were less than unity (0.9 ± 0.5) in the SEA-outflow. These results suggest that secondary formation of organic acids is largely important in the IGP-outflow whereas primary emission is a major source of organic acids in the SEA-outflow. Based on the correlation coefficient matrix analysis and C1/C2 and C4/C3 ratios, we consider that the sources of C1 are probably associated with the secondary formation via the oxidation of biogenic VOCs, while C2 has both primary and secondary formations associated with anthropogenic sources in the IGP-outflow. On the other hand, C1 and C2 have similar sources (both primary and secondary) originated from biomass burning and bacterial activities via long-range atmospheric transport in the SEA-outflow, as inferred from the MODIS fire spot data, significant concentrations of isovaleric

  3. Hygroscopic growth of particles nebulized from water-soluble extracts of PM2.5 aerosols over the Bay of Bengal: Influence of heterogeneity in air masses and formation pathways.

    Science.gov (United States)

    Boreddy, S K R; Kawamura, Kimitaka; Bikkina, Srinivas; Sarin, M M

    2016-02-15

    Hygroscopic properties of water-soluble matter (WSM) extracted from fine-mode aerosols (PM2.5) in the marine atmospheric boundary layer of the Bay of Bengal (BoB) have been investigated during a cruise from 27th December 2008 to 30th January 2009. Hygroscopic growth factors were measured on particles generated from the WSM using an H-TDMA system with an initial dry size of 100 nm in the range of 5-95% relative humidity (RH). The measured hygroscopic growth of WSM at 90% RH, g(90%)WSM, were ranged from 1.11 to 1.74 (mean: 1.43 ± 0.19) over the northern BoB and 1.12 to 1.38 (mean: 1.25 ± 0.09) over the southern BoB. A key finding is that distinct hygroscopic growth factors are associated with the air masses from the Indo-Gangetic plains (IGP), which are clearly distinguishable from those associated with air masses from Southeast Asia (SEA). We found higher (lower) g(90%)WSM over the northern (southern) BoB, which were associated with an IGP (SEA) air masses, probably due the formation of high hygroscopic salts such as (NH4)2SO4. On the other hand, biomass burning influenced SEA air masses confer the low hygroscopic salts such as K2SO4, MgSO4, and organic salts over the southern BoB. Interestingly, mass fractions of water-soluble organic matter (WSOM) showed negative and positive correlations with g(90%)WSM over the northern and southern BoB, respectively, suggesting that the mixing state of organic and inorganic fractions could play a major role on the g(90%)WSM over the BoB. Further, WSOM/SO4(2-) mass ratios suggest that SO4(2-) dominates the g(90%)WSM over the northern BoB whereas WSOM fractions were important over the southern BoB. The present study also suggests that aging process could significantly alter the hygroscopic growth of aerosol particles over the BoB, especially over the southern BoB. Copyright © 2015 Elsevier B.V. All rights reserved.

  4. 20 CFR 636.5 - Exhaustion of grantee level procedure.

    Science.gov (United States)

    2010-04-01

    ... 20 Employees' Benefits 3 2010-04-01 2010-04-01 false Exhaustion of grantee level procedure. 636.5..., INVESTIGATIONS AND HEARINGS § 636.5 Exhaustion of grantee level procedure. (a) Exhaustion required. No... have been exhausted. (b) Exhaustion exceptions. Complainants who have not exhausted the procedures at...

  5. Reactions between water-soluble organic acids and nitrates in atmospheric aerosols: Recycling of nitric acid and formation of organic salts

    Science.gov (United States)

    Wang, Bingbing; Laskin, Alexander

    2014-03-01

    Atmospheric particles often include a complex mixture of nitrate and secondary organic materials accumulated within the same individual particles. Nitrate as an important inorganic component can be chemically formed in the atmosphere. For instance, formation of sodium nitrate (NaNO3) and calcium nitrate (Ca(NO3)2) occurs when nitrogen oxides and nitric acid (HNO3) react with sea salt and calcite, respectively. Organic acids contribute a significant fraction of photochemically formed secondary organics that can condense on the preexisting nitrate-containing particles. Here we present a systematic microanalysis study on chemical composition of laboratory-generated particles composed of water-soluble organic acids and nitrates (i.e., NaNO3 and Ca(NO3)2) using computer-controlled scanning electron microscopy with energy-dispersive X-ray microanalysis and Fourier transform infrared microspectroscopy. The results show that water-soluble organic acids can react with nitrates and release gaseous HNO3 during the dehydration process. These reactions are attributed to acid displacement of nitrate with weak organic acids driven by the evaporation of HNO3 into gas phase because of its relatively high volatility. The reactions result in significant nitrate depletion and formation of organic salts in mixed organic acids/nitrate particles that, in turn, may affect their physical and chemical properties relevant to atmospheric environment and climate. Airborne nitrate concentrations are estimated by thermodynamic calculations corresponding to various nitrate depletions in selected organic acids of atmospheric relevance. The results indicate a potential mechanism of HNO3 recycling that may further affect concentrations of gas and condensed phase species in the atmosphere and the heterogeneous reaction chemistry between them.

  6. Simulation of the evolution of particle size distributions in a vehicle exhaust plume with unconfined dilution by ambient air.

    Science.gov (United States)

    Jiang, Pengzhi; Lignell, David O; Kelly, Kerry E; Lighty, JoAnn S; Sarofim, Adel F; Montgomery, Christopher J

    2005-04-01

    Over the past several years, numerous studies have linked ambient concentrations of particulate matter (PM) to adverse health effects, and more recent studies have identified PM size and surface area as important factors in determining the health effects of PM. This study contributes to a better understanding of the evolution of particle size distributions in exhaust plumes with unconfined dilution by ambient air. It combines computational fluid dynamics (CFD) with an aerosol dynamics model to examine the effects of different streamlines in an exhaust plume, ambient particle size distributions, and vehicle and wind speed on the particle size distribution in an exhaust plume. CFD was used to calculate the flow field and gas mixing for unconfined dilution of a vehicle exhaust plume, and the calculated dilution ratios were then used as input to the aerosol dynamics simulation. The results of the study show that vehicle speed affected the particle size distribution of an exhaust plume because increasing vehicle speed caused more rapid dilution and inhibited coagulation. Ambient particle size distributions had an effect on the smaller sized particles (approximately 10 nm range under some conditions) and larger sized particles (>2 microm) of the particle size distribution. The ambient air particle size distribution affects the larger sizes of the exhaust plume because vehicle exhaust typically contains few particles larger than 2 microm. Finally, the location of a streamline in the exhaust plume had little effect on the particle size distribution; the particle size distribution along any streamline at a distance x differed by less than 5% from the particle size distributions along any other streamline at distance x.

  7. A large source of low-volatility secondary organic aerosol

    DEFF Research Database (Denmark)

    Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard

    2014-01-01

    Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar...... the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form......-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air...

  8. Aerosols, clouds and their climatic impacts

    Energy Technology Data Exchange (ETDEWEB)

    Kulmala, M.; Laaksonen, A.; Korhonen, P. [Helsinki Univ. (Finland). Dept. of Physics

    1995-12-31

    The increasing atmospheric concentrations of greenhouse gases such as carbon dioxide and methane may drive a significant warming of the earth`s climate. However, a topic of more recent attention is the possibility that increased atmospheric concentrations of aerosol particles might drive a cooling of the planet. There are two distinct cooling mechanisms related to the enhanced concentrations of aerosol particles: the increase in the direct reflection of solar radiation (the direct effect), and the increase in cloud reflectivity caused by greater numbers of cloud condensation nuclei available (the indirect effect). Aerosols and clouds play a major role in the scattering and absorption of radiation in the Earth`s atmosphere. Locally the net effect can vary because of different kinds of surfaces. But according to measurements, the global net effect of clouds (and aerosols) on the atmosphere is net cooling and thus in opposition to the effect of greenhouse gases. The prediction of the future evolution of the climate involves substantial uncertainties. Clouds have a major effect on the radiation balance of the Earth and the prediction of amount and radiative properties of clouds is very difficult. Also the formation mechanisms and residence times of aerosol particles in the atmosphere involve large uncertainties. Thus the most serious difficulties arise in the area of the physics of clouds and aerosols

  9. Imaging aerosol viscosity

    Science.gov (United States)

    Pope, Francis; Athanasiadis, Thanos; Botchway, Stan; Davdison, Nicholas; Fitzgerald, Clare; Gallimore, Peter; Hosny, Neveen; Kalberer, Markus; Kuimova, Marina; Vysniauskas, Aurimas; Ward, Andy

    2017-04-01

    Organic aerosol particles play major roles in atmospheric chemistry, climate, and public health. Aerosol particle viscosity is important since it can determine the ability of chemical species such as oxidants, organics or water to diffuse into the particle bulk. Recent measurements indicate that OA may be present in highly viscous states; however, diffusion rates of small molecules such as water appear not to be limited by these high viscosities. We have developed a technique for measuring viscosity that allows for the imaging of aerosol viscosity in micron sized aerosols through use of fluorescence lifetime imaging of viscosity sensitive dyes which are also known as 'molecular rotors'. These rotors can be introduced into laboratory generated aerosol by adding minute quantities of the rotor to aerosol precursor prior to aerosolization. Real world aerosols can also be studied by doping them in situ with the rotors. The doping is achieved through generation of ultrafine aerosol particles that contain the rotors; the ultrafine aerosol particles deliver the rotors to the aerosol of interest via impaction and coagulation. This work has been conducted both on aerosols deposited on microscope coverslips and on particles that are levitated in their true aerosol phase through the use of a bespoke optical trap developed at the Central Laser Facility. The technique allows for the direct observation of kinetic barriers caused by high viscosity and low diffusivity in aerosol particles. The technique is non-destructive thereby allowing for multiple experiments to be carried out on the same sample. It can dynamically quantify and track viscosity changes during atmospherically relevant processes such oxidation and hygroscopic growth (1). This presentation will focus on the oxidation of aerosol particles composed of unsaturated and saturated organic species. It will discuss how the type of oxidant, oxidation rate and the composition of the oxidized products affect the time

  10. T Cell Exhaustion During Persistent Viral Infections

    Science.gov (United States)

    Kahan, Shannon M.; Wherry, E. John; Zajac, Allan J.

    2015-01-01

    Although robust and highly effective anti-viral T cells contribute to the clearance of many acute infections, viral persistence is associated with the development of functionally inferior, exhausted, T cell responses. Exhaustion develops in a step-wise and progressive manner, ranges in severity, and can culminate in the deletion of the anti-viral T cells. This disarming of the response is consequential as it compromises viral control and potentially serves to dampen immune-mediated damage. Exhausted T cells are unable to elaborate typical anti-viral effector functions. They are characterized by the sustained upregulation of inhibitory receptors and display a gene expression profile that distinguishes them from prototypic effector and memory T cell populations. In this review we discuss the properties of exhausted T cells; the virological and immunological conditions that favor their development; the cellular and molecular signals that sustain the exhausted state; and strategies for preventing and reversing exhaustion to favor viral control. PMID:25620767

  11. Desulphurization of exhaust gases in chemical processes

    Energy Technology Data Exchange (ETDEWEB)

    Asperger, K.; Wischnewski, W.

    1981-01-01

    The sulfur content of exhaust gases can be reduced by: desulphurization of fuels; modification of processes; or treatment of resultant gases. In this paper a few selected examples from the chemical industry in the German Democratic Republic are presented. Using modified processes and treating the resultant gases, the sulphuric content of exhaust gases is effectively reduced. Methods to reduce the sulfur content of exhaust gases are described in the field of production of: sulphuric acid; viscose; fertilizers; and paraffin.

  12. Emotionally exhausting factors in general practitioners? work

    OpenAIRE

    Torppa, M.A.; Kuikka, L.; Nevalainen, M.; Pitk?l?, K.H.

    2015-01-01

    Background. Emotional exhaustion is central in burnout syndrome and signals its development. General practitioners? (GP) work is emotionally challenging but research on these aspects is lacking. Objective. To study the prevalence of emotional exhaustion among GPs and to evaluate how their characteristics and work experiences are associated with emotional exhaustion. Design and methods. A questionnaire survey was carried out among GPs in Finland in 2011 in which questions were posed regarding ...

  13. Whitecaps, sea-salt aerosols, and climate

    Science.gov (United States)

    Anguelova, Magdalena Dimitrova

    Oceanic whitecaps are the major source of sea-salt aerosols. Because these aerosols are dominant in remote marine air, they control the radiative properties of the clean background atmosphere by scattering sunlight, changing cloud properties and lifetime, and providing media for chemical reactions. Including sea-salt effects in climate models improves predictions, but simulating their generation is first necessary. To make the sea-salt generation function currently used in climate models more relevant for aerosol investigations, this study proposes two modifications. First, the conventional relation between whitecap coverage, W, and the 10-meter wind speed, U10, used in typical generation functions is expanded to include additional factors that affect whitecaps and sea-salt aerosol formation. Second, the sea-salt generation function is extended to smaller sizes; sea-salt aerosol with initial radii from 0.4 to 20 mum can now be modeled. To achieve these goals, this thesis develops a new method for estimating whitecap coverage on a global scale using satellite measurements of the brightness temperature of the ocean surface. Whitecap coverage evaluated with this method incorporates the effects of atmospheric stability, sea-surface temperature, salinity, wind fetch, wind duration, and the amount of surface-active material. Assimilating satellite-derived values for whitecap coverage in the sea-salt generation function incorporates the effects of all environmental factors on sea-salt production and predicts realistic sea-salt aerosol loadings into the atmosphere. An extensive database of whitecap coverage and sea-salt aerosol fluxes has been compiled with the new method and is used to investigate their spatial and temporal characteristics. The composite effect of all environmental factors suggests a more uniform latitudinal distribution of whitecaps and sea-salt aerosols than that predicted from wind speed alone. The effect of sea-surface temperature, TS, is

  14. Role of snow and cold environment in the fate and effects of nanoparticles and select organic pollutants from gasoline engine exhaust.

    Science.gov (United States)

    Nazarenko, Yevgen; Kurien, Uday; Nepotchatykh, Oleg; Rangel-Alvarado, Rodrigo B; Ariya, Parisa A

    2016-02-01

    Exposure to vehicle exhaust can drive up to 70 % of excess lifetime cancer incidences due to air pollution in urban environments. Little is known about how exhaust-derived particles and organic pollutants, implicated in adverse health effects, are affected by freezing ambient temperatures and the presence of snow. Airborne particles and (semi)volatile organic constituents in dilute exhaust were studied in a novel low-temperature environmental chamber system containing natural urban snow under controlled cold environmental conditions. The presence of snow altered the aerosol size distributions of dilute exhaust in the 10 nm to 10 μm range and decreased the number density of the nanoparticulate (pollutant content in snow, has potential to alter health effects of human exposure to vehicle exhaust.

  15. Aerosols Science and Technology

    CERN Document Server

    Agranovski, Igor

    2011-01-01

    This self-contained handbook and ready reference examines aerosol science and technology in depth, providing a detailed insight into this progressive field. As such, it covers fundamental concepts, experimental methods, and a wide variety of applications, ranging from aerosol filtration to biological aerosols, and from the synthesis of carbon nanotubes to aerosol reactors.Written by a host of internationally renowned experts in the field, this is an essential resource for chemists and engineers in the chemical and materials disciplines across multiple industries, as well as ideal supplementary

  16. Literature review supporting assessment of potential radionuclides in the 291-Z exhaust ventilation

    Energy Technology Data Exchange (ETDEWEB)

    Mahoney, L.A.; Ballinger, M.Y.; Jette, S.J.; Thomas, L.M. Glissmeyer, J.A. [Pacific Northwest Lab., Richland, WA (United States); Davis, W.E. [Westinghouse Hanford Co., Richland, WA (United States)

    1994-08-01

    This literature review was prepared to support a study conducted by Pacific Northwest Laboratory to assess the potential deposition and resuspension of radionuclides in the 291-Z ventilation exhaust building located in the 200 West Area of the US Department of Energy`s Hanford Project near Richland, Washington. The filtered ventilation air from three of the facilities at the Plutonium Finishing Plant (PFP) complex are combined together in the 291-Z building before discharge through a common stack. These three facilities contributing filtered exhaust air to the discharge stream are (1) the PFP, also known as the Z-Plant or 234-5Z, (2) the Plutonium Reclamation Facility (PRF or 236-Z), and (3), the Waste Incinerator Building (WIB or 232-Z). The 291-Z building houses the exhaust fans that pull air from the 291-Z central collection plenum and exhausts the air to the stack. Section 2.0 of this report is a description of the physical characteristic of the ventilation system from the High Efficiency Particulate Air (HEPA) filters to the exhaust stack. A description of the processes performed in the facilities that are vented through 291-Z is given in Section 3.0. The description focuses on the chemical and physical forms of potential aerosols given off from the unit operations. A timeline of the operations and events that may have affected the deposition of material in the ventilation system is shown. Aerosol and radiation measurements taken in previous studies are also discussed. Section 4.0 discusses the factors that influence particle deposition and adhesion. Mechanisms of attachment and resuspension are covered with specific attention to the PFP ducts. Conclusions and recommendations are given in Section 5.0.

  17. Exhaust gas bypass valve control for thermoelectric generator

    Science.gov (United States)

    Reynolds, Michael G; Yang, Jihui; Meisner, Greogry P.; Stabler, Francis R.; De Bock, Hendrik Pieter Jacobus; Anderson, Todd Alan

    2012-09-04

    A method of controlling engine exhaust flow through at least one of an exhaust bypass and a thermoelectric device via a bypass valve is provided. The method includes: determining a mass flow of exhaust exiting an engine; determining a desired exhaust pressure based on the mass flow of exhaust; comparing the desired exhaust pressure to a determined exhaust pressure; and determining a bypass valve control value based on the comparing, wherein the bypass valve control value is used to control the bypass valve.

  18. T cell exhaustion and immune-mediated disease-the potential for therapeutic exhaustion.

    Science.gov (United States)

    McKinney, Eoin F; Smith, Kenneth Gc

    2016-12-01

    T cell exhaustion represents a continuous spectrum of cellular dysfunction induced during chronic viral infection, facilitating viral persistence and associating with poor clinical outcome. Modulation of T cell exhaustion can restore function in exhausted CD8 T cells, promoting viral clearance. Exhaustion has also been implicated as playing an important role in anti-tumour responses, whereby exhausted tumour-infiltrating lymphocytes fail to control tumour progression. More recently exhaustion has been linked to long-term clinical outcome in multiple autoimmune diseases but, in contrast to cancer or infection, it is associated with a favourable clinical outcome characterised by fewer relapses. An increasing understanding of key inhibitory signals promoting exhaustion has led to advances in therapy for chronic infection and cancer. An increasing understanding of this biology may facilitate novel treatment approaches for autoimmunity through the therapeutic induction of exhaustion. Copyright © 2016. Published by Elsevier Ltd.

  19. Field and laboratory measurements of biomass burning and vehicle exhaust using a PTR-MS

    Science.gov (United States)

    VanderSchelden, Graham Samuel

    The Proton Transfer Reaction Mass Spectrometer (PTR-MS) is a powerful tool for analyzing organic compounds in air and has been applied in field and laboratory applications to assess emissions from biomass burning and vehicles. Biomass burning is an important source of air pollution globally in the form of wild fires, burning of crop stubble, and combustion of organic material for home energy. In the United States, residential wood combustion combined with low inversion heights in winter time has caused air quality problems. Through field deployment of the PTR-MS in Xi'an China during August of 2011, it was determined that 27%, 16%, 26%, and 12% of ambient carbon monoxide (CO), acetaldehyde, benzene, and toluene could be attributed to biomass burning. The PTR-MS was also deployed to Yakima, Washington in January of 2013, finding that residential wood combustion was a substantial source of air toxics and PM. Residential wood combustion contributed 100%, 73%, 69%, 55%, 36%, 19%, 19%, and 17% of organic PM1, formaldehyde, acetaldehyde, black carbon, benzene, toluene, C2-alkylbenzenes, and CO respectively. Diesel vehicles are becoming a larger fraction of the vehicle fleet and can be held responsible for a substantial fraction of air pollution emissions from on and off road mobile sources. Diesel engines are a source of low volatility products that are difficult to measure and are thought to be important in the formation of secondary organic aerosol (SOA). This work focuses on measuring important diesel exhaust compounds with the PTR-MS and assessing oxidation processes of these compounds. When the PTR-MS was deployed to the field along with a thermal desorption pre-concentration system, we estimated that diesel vehicles were about 3-15% of the vehicle activity influencing our study site in Yakima, WA using the ratio of m/z 157 to m/z 129. SOA yields of diesel exhaust compounds were assessed and about 48% of the SOA was attributed to compounds measured by the PTR

  20. Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

    Directory of Open Access Journals (Sweden)

    M. Elser

    2016-06-01

    Full Text Available Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero  ≤  2.5 µm in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC and several trace gases including carbon monoxide (CO, carbon dioxide (CO2, and methane (CH4 were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF: hydrocarbon-like OA (HOA, from traffic emissions, biomass burning OA (BBOA, from biomass combustion, residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning, and oxygenated OA (OOA, related to secondary aerosol formation. OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded

  1. Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

    Science.gov (United States)

    Elser, Miriam; Bozzetti, Carlo; El-Haddad, Imad; Maasikmets, Marek; Teinemaa, Erik; Richter, Rene; Wolf, Robert; Slowik, Jay G.; Baltensperger, Urs; Prévôt, André S. H.

    2016-06-01

    Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero ≤ 2.5 µm) in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR)-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning), and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded regional background

  2. Some results of an experimental study of the atmospheric aerosol in Tomsk: A combined approach

    Energy Technology Data Exchange (ETDEWEB)

    Zuev, V.V. [Institute of Atmospheric Optics, Tomsk (Russian Federation)

    1996-04-01

    As widely accepted, aerosols strongly contribute to the formation of the earth`s radiation balance through the absorption and scattering of solar radiation. In addition, aerosols, being active condensation nuclei, also have a role in the cloud formation process. In this paper, results are presented of aerosol studies undertaken at the field measurement sites of the Institute of Atmospheric Optics in Tomsk and the Tomsk region.

  3. Assessment of the global impact of aerosols on tropospheric oxidants

    Science.gov (United States)

    Tie, Xuexi; Madronich, Sasha; Walters, Stacy; Edwards, David P.; Ginoux, Paul; Mahowald, Natalie; Zhang, Renyi; Lou, Chao; Brasseur, Guy

    2005-02-01

    We present here a fully coupled global aerosol and chemistry model for the troposphere. The model is used to assess the interactions between aerosols and chemical oxidants in the troposphere, including (1) the conversion from gas-phase oxidants into the condensed phase during the formation of aerosols, (2) the heterogeneous reactions occurring on the surface of aerosols, and (3) the effect of aerosols on ultraviolet radiation and photolysis rates. The present study uses the global three-dimensional chemical/transport model, Model for Ozone and Related Chemical Tracers, version 2 (MOZART-2), in which aerosols are coupled with the model. The model accounts for the presence of sulfate, soot, primary organic carbon, ammonium nitrate, secondary organic carbon, sea salt, and mineral dust particles. The simulated global distributions of the aerosols are analyzed and evaluated using satellite measurements (Moderate-Resolution Imaging Spectroradiometer (MODIS)) and surface measurements. The results suggest that in northern continental regions the tropospheric aerosol loading is highest in Europe, North America, and east Asia. Sulfate, organic carbon, black carbon, and ammonium nitrate are major contributions for the high aerosol loading in these regions. Aerosol loading is also high in the Amazon and in Africa. In these areas the aerosols consist primarily of organic carbon and black carbon. Over the southern high-latitude ocean (around 60°S), high concentrations of sea-salt aerosol are predicted. The concentration of mineral dust is highest over the Sahara and, as a result of transport, spread out into adjacent regions. The model and MODIS show similar geographical distributions of aerosol particles. However, the model overestimates the sulfate and carbonaceous aerosol in the eastern United States, Europe, and east Asia. In the region where aerosol loading is high, aerosols have important impacts on tropospheric ozone and other oxidants. The model suggests that

  4. Increase in upper tropospheric and lower stratospheric aerosol levels and its potential connection with Asian pollution

    Science.gov (United States)

    Vernier, J.-P.; Fairlie, T. D.; Natarajan, M.; Wienhold, F. G.; Bian, J.; Martinsson, B. G.; Crumeyrolle, S.; Thomason, L. W.; Bedka, K. M.

    2015-02-01

    Satellite observations have shown that the Asian Summer Monsoon strongly influences the upper troposphere and lower stratosphere (UTLS) aerosol morphology through its role in the formation of the Asian Tropopause Aerosol Layer (ATAL). Stratospheric Aerosol and Gas Experiment II solar occultation and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar observations show that summertime UTLS Aerosol Optical Depth (AOD) between 13 and 18 km over Asia has increased by three times since the late 1990s. Here we present the first in situ balloon measurements of aerosol backscatter in the UTLS from Western China, which confirm high aerosol levels observed by CALIPSO since 2006. Aircraft in situ measurements suggest that aerosols at lower altitudes of the ATAL are largely composed of carbonaceous and sulfate materials (carbon/sulfur elemental ratio ranging from 2 to 10). Back trajectory analysis from Cloud-Aerosol Lidar with Orthogonal Polarization observations indicates that deep convection over the Indian subcontinent supplies the ATAL through the transport of pollution into the UTLS. Time series of deep convection occurrence, carbon monoxide, aerosol, temperature, and relative humidity suggest that secondary aerosol formation and growth in a cold, moist convective environment could play an important role in the formation of ATAL. Finally, radiative calculations show that the ATAL layer has exerted a short-term regional forcing at the top of the atmosphere of -0.1 W/m2 in the past 18 years.

  5. Local Exhaust Optimization and Worker Exposure

    DEFF Research Database (Denmark)

    Heiselberg, Per; Pedersen, Morten; Plath, Thomas

    This paper describes a process of optimisation of exhaust efficiency and of minimisation of worker exposure at a semiautomatic printing machine at a printing office.......This paper describes a process of optimisation of exhaust efficiency and of minimisation of worker exposure at a semiautomatic printing machine at a printing office....

  6. Vital exhaustion and risk for cancer

    DEFF Research Database (Denmark)

    Bergelt, Corinna; Christensen, Jane Hvarregaard; Prescott, Eva

    2005-01-01

    Vital exhaustion, defined as feelings of depression and fatigue, has previously been investigated mainly as a risk factor for cardiovascular disease. The authors investigated the association between depressive feelings and fatigue as covered by the concept of vital exhaustion and the risk...

  7. 49 CFR 393.83 - Exhaust systems.

    Science.gov (United States)

    2010-10-01

    ... 49 Transportation 5 2010-10-01 2010-10-01 false Exhaust systems. 393.83 Section 393.83... NECESSARY FOR SAFE OPERATION Miscellaneous Parts and Accessories § 393.83 Exhaust systems. (a) Every motor... shall have a system to direct the discharge of such fumes. No part shall be located where its location...

  8. Effect of exhaustive exercise on myocardial performance.

    Science.gov (United States)

    Grimditch, G K; Barnard, R J; Duncan, H W

    1981-11-01

    Several investigators have reported ultrastructural changes in hearts of animals exercised to exhaustion. The present study was designed to determine whether functional changes occur in the intact heart at exhaustion. Adult mongrel dogs (n = 8) were chronically instrumented to measure cardiac output, coronary blood flow, aortic blood pressure, left ventricular pressure, +dP/dtmax, and -dP/dtmax. After recovery, the dogs were run to exhaustion at a constant work load, eliciting approximately 70% of maximum heart rate. The exhaustive bouts were terminated when the animals either refused or were unable to continue running, at which time their rectal temperatures approaches 42.2 degree C. The mean exhaustion time was 76.7 +/- 11.8 min. All parameters increased from rest to steady state with the exception of stroke volume (23.2 +/- 4.9 vs. 20.5 +/- 1.6 ml), which remained constant. In the transition from steady state to exhaustion, only +dP/dtmax (6,652 +/- 291 vs. 7,689 +/- 479 Torr/s) and -dP/dtmax (4,110 +/- 227 vs. 4,890 +/- 215 Torr/s) increased significantly; all other values exhibited no significant change. Similarly, when maximum cardiovascular parameters were measured before and after exhaustion, no significant changes were found. These data show that cardiac contractile function is not depressed in dogs as a result of exhaustive exercise.

  9. Method for removing soot from exhaust gases

    Energy Technology Data Exchange (ETDEWEB)

    Suib, Steven L.; Dharmarathna, D. A. Saminda; Pahalagedara, Lakshitha R.

    2018-01-16

    A method for oxidizing soot from diesel exhaust gas from a diesel engine. The method involves providing a diesel particulate filter for receiving the diesel exhaust gas; coating a catalyst composition on the diesel particulate filter; and contacting the soot from the diesel exhaust gas with the catalyst coated diesel particulate filter at a temperature sufficient to oxidize the soot to carbon dioxide. The catalyst composition is a doped or undoped manganese oxide octahedral molecular sieve (OMS-2) material. A diesel exhaust gas treatment system that includes a diesel particulate filter for receiving diesel exhaust gas from a diesel engine and collecting soot; and a catalyst composition coated on the diesel particulate filter. The catalyst composition is a doped or undoped manganese oxide octahedral molecular sieve (OMS-2).

  10. Sensitivity of aerosol direct radiative forcing to aerosol vertical profile

    Directory of Open Access Journals (Sweden)

    Jung-Ok Choi

    2014-05-01

    Full Text Available Aerosol vertical profile significantly affects the aerosol direct radiative forcing at the TOA level. The degree to which the aerosol profile impacts the aerosol forcing depends on many factors such as presence of cloud, surface albedo and aerosol single scattering albedo (SSA. Using a radiation model, we show that for absorbing aerosols (with an SSA of 0.7–0.8 whether aerosols are located above cloud or below induces at least one order of magnitude larger changes of the aerosol forcing than how aerosols are vertically distributed in clear skies, above cloud or below cloud. To see if this finding also holds for the global average aerosol direct radiative effect, we use realistic AOD distribution by integrating MODIS, MISR and AERONET observations, SSA from AERONET and cloud data from various satellite observations. It is found that whether aerosols are above cloud or below controls about 70–80% of the effect of aerosol vertical profile on the global aerosol radiative effect. Aerosols below cloud contribute as much to the global aerosol radiative effect as aerosols above cloud.

  11. Emotionally exhausting factors in general practitioners’ work

    Science.gov (United States)

    Torppa, M.A.; Kuikka, L.; Nevalainen, M.; Pitkälä, K.H.

    2015-01-01

    Background. Emotional exhaustion is central in burnout syndrome and signals its development. General practitioners’ (GP) work is emotionally challenging but research on these aspects is lacking. Objective. To study the prevalence of emotional exhaustion among GPs and to evaluate how their characteristics and work experiences are associated with emotional exhaustion. Design and methods. A questionnaire survey was carried out among GPs in Finland in 2011 in which questions were posed regarding their experience of emotional exhaustion and items related to their work experiences and professional identity. A statement “I feel burnt out from my job” (never, seldom, sometimes, quite often, or often) enquired about emotional exhaustion. Those responding quite often or often were categorized as emotionally exhausted. Results. Among the GPs, 68% responded (165/244). Of the respondents, 18% were emotionally exhausted. Emotional exhaustion was associated with older age, longer working history, experiences of having too much work, fear and reports of having committed a medical error, low tolerance of uncertainty in their work, and feeling alone at work. No differences in positive work experiences were found. In logistic regression analysis working experience > 5 years (OR 4.1, 95% CI 1.6–10.8; p = 0.0036) and feeling alone at work (OR 2.9, 95% CI 1.2–7.1; p = 0.020) predicted emotional exhaustion, having committed a medical error in the past three months predicted it marginally significantly (OR 2.4, 95% CI 1.0–5.9, p = 0.057), whereas tolerating uncertainty well protected against it (OR 0.2, 95% CI 0.09–0.7; p = 0.0098). Conclusions. Emotional exhaustion among GPs was common and associated with longer working history, having committed a medical error, and feelings of isolation at work. GPs should receive more support throughout their careers. PMID:26311207

  12. CADS:Cantera Aerosol Dynamics Simulator.

    Energy Technology Data Exchange (ETDEWEB)

    Moffat, Harry K.

    2007-07-01

    This manual describes a library for aerosol kinetics and transport, called CADS (Cantera Aerosol Dynamics Simulator), which employs a section-based approach for describing the particle size distributions. CADS is based upon Cantera, a set of C++ libraries and applications that handles gas phase species transport and reactions. The method uses a discontinuous Galerkin formulation to represent the particle distributions within each section and to solve for changes to the aerosol particle distributions due to condensation, coagulation, and nucleation processes. CADS conserves particles, elements, and total enthalpy up to numerical round-off error, in all of its formulations. Both 0-D time dependent and 1-D steady state applications (an opposing-flow flame application) have been developed with CADS, with the initial emphasis on developing fundamental mechanisms for soot formation within fires. This report also describes the 0-D application, TDcads, which models a time-dependent perfectly stirred reactor.

  13. Combustion aerosols from potassium-containing fuels

    Energy Technology Data Exchange (ETDEWEB)

    Balzer Nielsen, Lars

    1998-12-31

    The scope of the work presented in this thesis is the formation and evolution of aerosol particles in the submicron range during combustion processes, in particular where biomass is used alone or co-fired with coal. An introduction to the formation processes of fly ash in general and submicron aerosol in particular during combustion is presented, along with some known problems related to combustion of biomass for power generation. The work falls in two parts. The first is the design of a laboratory setup for investigation of homogeneous nucleation and particle dynamics at high temperature. The central unit of the setup is a laminar flow aerosol condenser (LFAC), which essentially is a 173 cm long tubular furnace with an externally cooled wall. A mathematical model is presented which describes the formation and evolution of the aerosol in the LFAC, where the rate of formation of new nuclei is calculated using the so-called classical theory. The model includes mass and energy conservation equations and an expression for the description of particle growth by diffusion. The resulting set of nonlinear second-order partial differential equations are solved numerically using the method of orthogonal collocation. The model is implemented in the FORTRAN code MONAERO. The second part of this thesis describes a comprehensive investigation of submicron aerosol formation during co-firing of coal and straw carried out at a 380 MW{sub Th} pulverized coal unit at Studstrup Power Plant, Aarhus. Three types of coal are used, and total boiler load and straw input is varied systematically. Straw contains large amounts of potassium, which is released during combustion. Submicron aerosol is sampled between the two banks of the economizer at a flue gas temperature of 350 deg. C using a novel ejector probe. The aerosol is characterized using the SMPS system and a Berner-type low pressure impactor. The chemical composition of the particles collected in the impactor is determined using

  14. Composition of Secondary Organic Aerosol from the Photolysis of 1-Nitronaphthalene

    Science.gov (United States)

    Wenger, J.; Healy, R.; Chen, Y.; Kalberer, M.; Kourtchev, I.

    2012-12-01

    Nitro-substituted polycyclic aromatic hydrocarbons are of interest due to their associated mutagenic and carcinogenic effects. 1-Nitronaphthalene is emitted directly from combustion processes such as vehicle exhaust, but is also formed through the reaction of naphthalene with the hydroxyl or nitrate radical in the presence of NOx. Photolysis has previously been demonstrated to be the major degradation pathway for 1-nitronaphthalene in the troposphere. In this study, a series of simulation chamber experiments has been performed to investigate the chemical composition of secondary organic aerosol (SOA) formed through the direct photolysis of 1-nitronaphthalene using an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS, TSI). SOA forms rapidly with a yield of up to 50% depending on precursor concentration and photolysis rate. Along with expected products such as naphthoquinone and nitronaphthol, condensed species exhibiting mass spectra consistent with the presence of four aromatic rings were also observed. It is proposed that these species may be formed through dimerization of naphthoxy radicals generated during the photolysis process. Further evidence to support this mechanism was obtained when 1-nitronaphthalene was photolyzed in the presence of excess nitrobenzene. Dimers were then formed containing three aromatic rings, consistent with the reaction of phenoxy and naphthoxy radicals. The molecular formulae of the dimers were also confirmed by collecting SOA on filters and analysing the extracts off-line using an LTQ Orbitrap Velos mass spectrometer (Thermo-Fisher Scientific), fitted with a TriVersa NanoMate chip-based electrospray ionization source (Advion Biosystems). The rapid formation of condensable dimers through the self-reaction of naphthoxy radicals represents a previously unreported potential pathway to SOA formation. Analogous mechanisms may also be important for other nitrated polycyclic aromatic hydrocarbons.

  15. Nucleation and growth of sulfate aerosol in coal-fired power plant plumes: sensitivity to background aerosol and meteorology

    Directory of Open Access Journals (Sweden)

    R. G. Stevens

    2012-01-01

    Full Text Available New-particle formation in the plumes of coal-fired power plants and other anthropogenic sulfur sources may be an important source of particles in the atmosphere. It remains unclear, however, how best to reproduce this formation in global and regional aerosol models with grid-box lengths that are 10s of kilometers and larger. The predictive power of these models is thus limited by the resultant uncertainties in aerosol size distributions. In this paper, we focus on sub-grid sulfate aerosol processes within coal-fired power plant plumes: the sub-grid oxidation of SO2 with condensation of H2SO4 onto newly-formed and pre-existing particles. We have developed a modeling framework with aerosol microphysics in the System for Atmospheric Modelling (SAM, a Large-Eddy Simulation/Cloud-Resolving Model (LES/CRM. The model is evaluated against aircraft observations of new-particle formation in two different power-plant plumes and reproduces the major features of the observations. We show how the downwind plume aerosols can be greatly modified by both meteorological and background aerosol conditions. In general, new-particle formation and growth is greatly reduced during polluted conditions due to the large pre-existing aerosol surface area for H2SO4 condensation and particle coagulation. The new-particle formation and growth rates are also a strong function of the amount of sunlight and NOx since both control OH concentrations. The results of this study highlight the importance for improved sub-grid particle formation schemes in regional and global aerosol models.

  16. Health effects of exhaust particles

    Energy Technology Data Exchange (ETDEWEB)

    Pihlava, T.; Uuppo, M.; Niemi, S.

    2013-11-01

    This report introduces general information about diesel particles and their health effects. The purpose of this report is to introduce particulate matter pollution and present some recent studies made regarding the health effects of particulate matter. The aim is not to go very deeply into the science, but instead to keep the text understandable for the average layman. Particulate matter is a complex mixture of extremely small particles and liquid droplets. These small particles are made up of a number of components that include for example acids, such as nitrates and sulphates, as well as organic chemicals, metals and dust particles from the soil. Particulate matter comes from several sources, such as transportation emissions, industrial emissions, forest fires, cigarette smoke, volcanic ash and climate variations. Particles are divided into coarse particles with diameters less than 10 ..m, fine particles with diameters smaller than 2.5 ..m and ultra-fine particles with diameters less than 0.1 ..m. The particulate matter in diesel exhaust gas is a highly complex mixture of organic, inorganic, solid, volatile and partly volatile compounds. Many of these particles do not form until they reach the air. Many carcinogenic compounds have been found in diesel exhaust gas and it is considered carcinogenic to humans. Particulate matter can cause several health effects, such as premature death in persons with heart or lung disease, cancer, nonfatal heart attacks, irregular heartbeat, aggravated asthma, decreased lung function and an increase in respiratory symptoms, such as irritation of the airways, coughing or difficulty breathing. It is estimated that in Finland about 1300 people die prematurely due to particles and the economic loss in the EU due to the health effects of particles can be calculated in the billions. Ultra-fine particles are considered to be the most harmful to human health. Ultrafine particles usually make the most of their quantity and surface area

  17. Comparison of advanced offline and in situ techniques of organic aerosol composition measurement during the CalNex campaign

    NARCIS (Netherlands)

    Tsimkouski, I.|info:eu-repo/dai/nl/330541676; Dorst, T; Goldstein, AH; Oyama, B.S.; Holzinger, R.|info:eu-repo/dai/nl/337989338; Chan, AWH

    2015-01-01

    Our understanding of formation processes, physical properties, and climate/health effects of organic aerosols is still limited in part due to limited knowledge of organic aerosol composition. We present speciated measurements of organic aerosol composition by two methods: in situ thermaldesorption

  18. Atmosphere aerosol satellite project Aerosol-UA

    Science.gov (United States)

    Milinevsky, Gennadi; Yatskiv, Yaroslav; Syniavskyi, Ivan; Bovchaliuk, Andrii; Degtyaryov, Oleksandr; Sosonkin, Mikhail; Mishchenko, Michael; Danylevsky, Vassyl; Ivanov, Yury; Oberemok, Yevgeny; Masley, Volodymyr; Rosenbush, Vera; Moskalev, Sergii

    2017-04-01

    The experiment Aerosol-UA is Ukrainian space mission aimed to the terrestrial atmospheric aerosol spatial distribution and microphysics investigations. The experiment concept is based on idea of Glory/APS mission of precise orbital measurements of polarization and intensity of the sunlight scattered by the atmosphere, aerosol and the surface the multichannel Scanning Polarimeter (ScanPol) with narrow field-of-view. ScanPol measurements will be accompanied by the wide-angle MultiSpectral Imager-Polarimeter (MSIP). The ScanPol is designed to measure Stokes parameters I, Q, U within the spectral range from the UV to the SWIR in a wide range of phase angles along satellite ground path. Expected ScanPol polarimetric accuracy is 0.15%. A high accuracy measurement of the degree of linear polarization is provided by on-board calibration of the ScanPol polarimeter. On-board calibration is performed for each scan of the mirror scanning system. A set of calibrators is viewed during the part of the scan range when the ScanPol polarimeter looks in the direction opposite to the Earth's surface. These reference assemblies provide calibration of the zero of the polarimetric scale (unpolarized reference assembly) and the scale factor for the polarimetric scale (polarized reference assembly). The zero of the radiometric scale is provided by the dark reference assembly.The spectral channels of the ScanPol are used to estimate the tropospheric aerosol absorption, the aerosol over the ocean and the land surface, the signals from cirrus clouds, stratospheric aerosols caused by major volcanic eruptions, and the contribution of the Earth's surface. The imager-polarimeter MSIP will collect 60°x60° field-of-view images on the state of the atmosphere and surface in the area, where the ScanPol polarimeter will measure, to retrieve aerosol optical depth and polarization properties of aerosol by registration of three Stokes parameters simultaneously in three spectral channels. The two more

  19. DARE : Dedicated Aerosols Retrieval Experiment

    NARCIS (Netherlands)

    Smorenburg, K.; Courrèges-Lacoste, G.B.; Decae, R.; Court, A.J.; Leeuw, G. de; Visser, H.

    2004-01-01

    At present there is an increasing interest in remote sensing of aerosols from space because of the large impact of aerosols on climate, earth observation and health. TNO has performed a study aimed at improving aerosol characterisation using a space based instrument and state-of-the-art aerosol

  20. 40 CFR 90.407 - Engine inlet and exhaust systems.

    Science.gov (United States)

    2010-07-01

    ... exhaust emission compliance over the full range of air inlet filter systems and exhaust muffler systems. (b) The air inlet filter system and exhaust muffler system combination used on the test engine must...

  1. Exhaust gas recirculation system for an internal combustion engine

    Science.gov (United States)

    Wu, Ko-Jen

    2013-05-21

    An exhaust gas recirculation system for an internal combustion engine comprises an exhaust driven turbocharger having a low pressure turbine outlet in fluid communication with an exhaust gas conduit. The turbocharger also includes a low pressure compressor intake and a high pressure compressor outlet in communication with an intake air conduit. An exhaust gas recirculation conduit fluidly communicates with the exhaust gas conduit to divert a portion of exhaust gas to a low pressure exhaust gas recirculation branch extending between the exhaust gas recirculation conduit and an engine intake system for delivery of exhaust gas thereto. A high pressure exhaust gas recirculation branch extends between the exhaust gas recirculation conduit and the compressor intake and delivers exhaust gas to the compressor for mixing with a compressed intake charge for delivery to the intake system.

  2. An overview of aerosol particle sensors for size distribution measurement

    Directory of Open Access Journals (Sweden)

    Panich Intra

    2007-08-01

    Full Text Available Fine aerosols are generally referred to airborne particles of diameter in submicron or nanometer size range. Measurement capabilities are required to gain understanding of these particle dynamics. One of the most important physical and chemical parameters is the particle size distribution. The aim of this article is to give an overview of recent development of already existing sensors for particle size distribution measurement based on electrical mobility determination. Available instruments for particle size measurement include a scanning mobility particle sizer (SMPS, an electrical aerosol spectrometer (EAS, an engine exhaust particle sizer (EEPS, a bipolar charge aerosol classifier (BCAC, a fast aerosol spectrometer (FAS a differential mobility spectrometer (DMS, and a CMU electrical mobility spectrometer (EMS. The operating principles, as well as detailed physical characteristics of these instruments and their main components consisting of a particle charger, a mobility classifier, and a signal detector, are described. Typical measurements of aerosol from various sources by these instruments compared with an electrical low pressure impactor (ELPI are also presented.

  3. Aerosol-cirrus interactions: a number based phenomenon at all?

    Directory of Open Access Journals (Sweden)

    M. Seifert

    2004-01-01

    Full Text Available In situ measurements of the partitioning of aerosol particles within cirrus clouds were used to investigate aerosol-cloud interactions in ice clouds. The number density of interstitial aerosol particles (non-activated particles in between the cirrus crystals was compared to the number density of cirrus crystal residuals. The data was obtained during the two INCA (Interhemispheric Differences in Cirrus Properties from Anthropogenic Emissions campaigns, performed in the Southern Hemisphere (SH and Northern Hemisphere (NH midlatitudes. Different aerosol-cirrus interactions can be linked to the different stages of the cirrus lifecycle. Cloud formation is linked to positive correlations between the number density of interstitial aerosol (Nint and crystal residuals (Ncvi, whereas the correlations are smaller or even negative in a dissolving cloud. Unlike warm clouds, where the number density of cloud droplets is positively related to the aerosol number density, we observed a rather complex relationship when expressing Ncvi as a function of Nint for forming clouds. The data sets are similar in that they both show local maxima in the Nint range 100 to 200cm, where the SH- maximum is shifted towards the higher value. For lower number densities Nint and Ncvi are positively related. The slopes emerging from the data suggest that a tenfold increase in the aerosol number density corresponds to a 3 to 4 times increase in the crystal number density. As Nint increases beyond the ca. 100 to 200cm, the mean crystal number density decreases at about the same rate for both data sets. For much higher aerosol number densities, only present in the NH data set, the mean Ncvi remains low. The situation for dissolving clouds allows us to offer two possible, but at this point only speculative, alternative interactions between aerosols and cirrus: evaporating clouds might be associated with a source of aerosol particles, or air pollution (high aerosol number density might

  4. Comparative mutagenicity and genotoxicity of particles and aerosols emitted by the combustion of standard vs. rapeseed methyl ester supplemented bio-diesel fuels: impact of after treatment devices: oxidation catalyst and particulate filter.

    Science.gov (United States)

    André, V; Barraud, C; Capron, D; Preterre, D; Keravec, V; Vendeville, C; Cazier, F; Pottier, D; Morin, J P; Sichel, F

    2015-01-01

    Diesel exhausts are partly responsible for the deleterious effects on human health associated with urban pollution, including cardiovascular diseases, asthma, COPD, and possibly lung cancer. Particulate fraction has been incriminated and thus largely investigated for its genotoxic properties, based on exposure conditions that are, however, not relevant for human risk assessment. In this paper, original and more realistic protocols were used to investigate the hazards induced by exhausts emitted by the combustion of standard (DF0) vs. bio-diesel fuels (DF7 and DF30) and to assess the impact of exhaust treatment devices (DOC and DPF). Mutagenicity and genotoxicity were evaluated for (1) resuspended particles ("off line" exposure that takes into account the bioavailability of adsorbed chemicals) and for (2) the whole aerosols (particles+gas phase components) under continuous flow exposure ("on line" exposure). Native particles displayed mutagenic properties associated with nitroaromatic profiles (YG1041), whereas PAHs did not seem to be involved. After DOC treatment, the mutagenicity of particles was fully abolished. In contrast, the level of particle deposition was low under continuous flow exposure, and the observed mutagenicity in TA98 and TA102 was thus attributable to the gas phase. A bactericidal effect was also observed in TA102 after DOC treatment, and a weak but significant mutagenicity persisted after DPF treatment for bio-diesel fuels. No formation of bulky DNA-adducts was observed on A549 cells exposed to diesel exhaust, even in very drastic conditions (organic extracts corresponding to 500 μg equivalent particule/mL, 48 h exposure). Taken together, these data indicate that the exhausts issued from the bio-diesel fuels supplemented with rapseed methyl ester (RME), and generated by current diesel engines equipped with after treatment devices are less mutagenic than older ones. The residual mutagenicity is linked to the gas phase and could be due to pro

  5. The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite, Taiwan

    Science.gov (United States)

    Chang, Shih-Yu; Lee, Chung-Te; Chou, Charles C.-K.; Liu, Shaw-Chen; Wen, Tian-Xue

    The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas-aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl -, NO 2-, NO 3-, SO 42-, Na +, NH 4+, K +, Mg 2+ and Ca 2+). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m -3 for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.

  6. A large source of low-volatility secondary organic aerosol.

    Science.gov (United States)

    Ehn, Mikael; Thornton, Joel A; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B; Jørgensen, Solvejg; Kjaergaard, Henrik G; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R; Wildt, Jürgen; Mentel, Thomas F

    2014-02-27

    Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

  7. Exhaustion and the Pathologization of Modernity.

    Science.gov (United States)

    Schaffner, Anna Katharina

    2016-09-01

    This essay analyses six case studies of theories of exhaustion-related conditions from the early eighteenth century to the present day. It explores the ways in which George Cheyne, George Beard, Richard von Krafft-Ebing, Sigmund Freud, Alain Ehrenberg and Jonathan Crary use medical ideas about exhaustion as a starting point for more wide-ranging cultural critiques related to specific social and technological transformations. In these accounts, physical and psychological symptoms are associated with particular external developments, which are thus not just construed as pathology-generators but also pathologized. The essay challenges some of the persistently repeated claims about exhaustion and its unhappy relationship with modernity.

  8. Taxation of exhaustible resources. [Monograph

    Energy Technology Data Exchange (ETDEWEB)

    Dasgupta, P.; Heal, G.; Stiglitz, J.

    1980-01-01

    This paper analyzes the effect of taxation on the intertemporal allocation of an exhaustible resource. A general framework within which a large variety of taxes can be analyzed is developed and then applied to a number of specific taxes. It is shown that there exists a pattern of taxation which can generate essentially any desired pattern of resource usage. Many tax policies, however, have effects markedly different both from the effects that these policies would have in the case of produced commodities and from those which they are designed (or widely thought) to have. For instance, if extraction costs are zero, a depletion allowance at a constant rate (widely thought to encourage the extraction of resources) has absolutely no effect; its gradual removal (usually thought to be preferable to a sudden removal) leads to faster rates of depletion (and lower prices) now, but higher prices in the future; which its sudden and unanticipated removal has absolutely no distortionary effect on the pattern of extraction. More generally, it is shown that the effects of tax structure on the patterns of extraction are critically dependent on expectations concerning future taxation. The changes in tax structure that have occurred in the past fifty years are of the kind that, if they were anticipated, (or if similar further changes are expected to occur in the future) lead to excessively fast exploitation of natural resources. However, if it is believed that current tax policies (including rates) will persist indefinitely, the current tax structure would lead to excessive conservationism. Thus, whether in fact current tax policies have lead to excessive conservationism is a moot question.

  9. Development and Characterization of a Thermodenuder for Aerosol Volatility Measurements

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Timothy Onasch

    2009-09-09

    This SBIR Phase I project addressed the critical need for improved characterization of carbonaceous aerosol species in the atmosphere. The proposed work focused on the development of a thermodenuder (TD) system capable of systematically measuring volatility profiles of primary and secondary organic aerosol species and providing insight into the effects of absorbing and nonabsorbing organic coatings on particle absorption properties. This work provided the fundamental framework for the generation of essential information needed for improved predictions of ambient aerosol loadings and radiative properties by atmospheric chemistry models. As part of this work, Aerodyne Research, Inc. (ARI) continued to develop and test, with the final objective of commercialization, an improved thermodenuder system that can be used in series with any aerosol instrument or suite of instruments (e.g., aerosol mass spectrometers-AMS, scanning mobility particle sizers-SMPS, photoacoustic absorption spectrometers-PAS, etc.) to obtain aerosol chemical, physical, and optical properties as a function of particle volatility. In particular, we provided the proof of concept for the direct coupling of our improved TD design with a full microphysical model to obtain volatility profiles for different organic aerosol components and to allow for meaningful comparisons between different TD-derived aerosol measurements. In a TD, particles are passed through a heated zone and a denuding (activated charcoal) zone to remove semi-volatile material. Changes in particle size, number concentration, optical absorption, and chemical composition are subsequently detected with aerosol instrumentation. The aerosol volatility profiles provided by the TD will strengthen organic aerosol emission inventories, provide further insight into secondary aerosol formation mechanisms, and provide an important measure of particle absorption (including brown carbon contributions and identification, and absorption enhancements

  10. An Aerosol Physical Chemistry Model for the Upper Troposphere

    Science.gov (United States)

    Lin, Jin-Sheng

    2001-01-01

    This report is the final report for the Cooperative Agreement NCC2-1000. The tasks outlined in the various proposals are: (1) Development of an aerosol chemistry model; (2) Utilization of satellite measurements of trace gases along with analysis of temperatures and dynamic conditions to understand ice cloud formation, dehydration and sedimentation in the winter polar regions; (3) Comparison of the HALOE and SAGE II time dependencies of the Pinatubo aerosol decay. The publications are attached.

  11. An exploratory drilling exhaustion sequence plot program

    Science.gov (United States)

    Schuenemeyer, J.H.; Drew, L.J.

    1977-01-01

    The exhaustion sequence plot program computes the conditional area of influence for wells in a specified rectangular region with respect to a fixed-size deposit. The deposit is represented by an ellipse whose size is chosen by the user. The area of influence may be displayed on computer printer plots consisting of a maximum of 10,000 grid points. At each point, a symbol is presented that indicates the probability of that point being exhausted by nearby wells with respect to a fixed-size ellipse. This output gives a pictorial view of the manner in which oil fields are exhausted. In addition, the exhaustion data may be used to estimate the number of deposits remaining in a basin. ?? 1977.

  12. Two phase exhaust for internal combustion engine

    Science.gov (United States)

    Vuk, Carl T [Denver, IA

    2011-11-29

    An internal combustion engine having a reciprocating multi cylinder internal combustion engine with multiple valves. At least a pair of exhaust valves are provided and each supply a separate power extraction device. The first exhaust valves connect to a power turbine used to provide additional power to the engine either mechanically or electrically. The flow path from these exhaust valves is smaller in area and volume than a second flow path which is used to deliver products of combustion to a turbocharger turbine. The timing of the exhaust valve events is controlled to produce a higher grade of energy to the power turbine and enhance the ability to extract power from the combustion process.

  13. Exhaustivity and intonation: a unified theory

    NARCIS (Netherlands)

    Westera, M.

    2017-01-01

    This dissertation presents a precise, unified and explanatory theory of human conversation, centered on two broad phenomena: exhaustivity implications and intonational meaning. In a nutshell: (i) speakers have two types of communicative intentions, namely information sharing and attention sharing,

  14. Emergency Protection from Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Cristy, G.A.

    2001-11-13

    Expedient methods were developed that could be used by an average person, using only materials readily available, to protect himself and his family from injury by toxic (e.g., radioactive) aerosols. The most effective means of protection was the use of a household vacuum cleaner to maintain a small positive pressure on a closed house during passage of the aerosol cloud. Protection factors of 800 and above were achieved.

  15. Fuel consumption and exhaust emissions of aircrafts

    Energy Technology Data Exchange (ETDEWEB)

    Buechler, R. [Institute of Flightmechanics, Braunschweig (Germany)

    1997-12-31

    The reduction of contamination of sensitive atmospheric layers by improved flight planning steps, is investigated. Calculated results have shown, that a further development of flight track planning allows considerable improvements on fuel consumption and exhaust emissions. Even if air traffic will further increase, optimistic investigations forecast a reduction of the environmental damage by aircraft exhausts, if the effects of improved flight track arrangement and engine innovations will be combined. (R.P.) 4 refs.

  16. Jet Engine Exhaust Analysis by Subtractive Chromatography

    Science.gov (United States)

    1978-12-01

    hydrocarbon ( TII