The statistical distribution of aerosol properties in sourthern West Africa

Science.gov (United States)

Haslett, Sophie; Taylor, Jonathan; Flynn, Michael; Bower, Keith; Dorsey, James; Crawford, Ian; Brito, Joel; Denjean, Cyrielle; Bourrianne, Thierry; Burnet, Frederic; Batenburg, Anneke; Schulz, Christiane; Schneider, Johannes; Borrmann, Stephan; Sauer, Daniel; Duplissy, Jonathan; Lee, James; Vaughan, Adam; Coe, Hugh

2017-04-01

The population and economy in southern West Africa have been growing at an exceptional rate in recent years and this trend is expected to continue, with the population projected to more than double to 800 million by 2050. This will result in a dramatic increase in anthropogenic pollutants, already estimated to have tripled between 1950 and 2000 (Lamarque et al., 2010). It is known that aerosols can modify the radiative properties of clouds. As such, the entrainment of anthropogenic aerosol into the large banks of clouds forming during the onset of the West African Monsoon could have a substantial impact on the region's response to climate change. Such projections, however, are greatly limited by the scarcity of observations in this part of the world. As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, three research aircraft were deployed, each carrying equipment capable of measuring aerosol properties in-situ. Instrumentation included Aerosol Mass Spectrometers (AMS), Single Particle Soot Photometers (SP2), Condensation Particle Counters (CPC) and Scanning Mobility Particle Sizers (SMPS). Throughout the intensive aircraft campaign, 155 hours of scientific flights covered an area including large parts of Benin, Togo, Ghana and parts of Côte D'Ivoire. Approximately 70 hours were dedicated to the measurement of cloud-aerosol interactions, with many other flights producing data contributing towards this objective. Using datasets collected during this campaign period, it is possible to build a robust statistical understanding of aerosol properties in this region for the first time, including size distributions and optical and chemical properties. Here, we describe preliminary results from aerosol measurements on board the three aircraft. These have been used to describe aerosol properties throughout the region and time period encompassed by the DACCIWA aircraft campaign. Such statistics will be invaluable for improving future

Light scattering and extinction measurements combined with laser-induced incandescence for the real-time determination of soot mass absorption cross section.

Science.gov (United States)

Wei, Yiyi; Ma, Lulu; Cao, Tingting; Zhang, Qing; Wu, Jun; Buseck, Peter R; Thompson, J E

2013-10-01

An aerosol albedometer was combined with laser-induced incandescence (LII) to achieve simultaneous measurements of aerosol scattering, extinction coefficient, and soot mass concentration. Frequency doubling of a Nd:YAG laser line resulted in a colinear beam of both λ = 532 and 1064 nm. The green beam was used to perform cavity ring-down spectroscopy (CRDS), with simultaneous measurements of scattering coefficient made through use of a reciprocal sphere nephelometer. The 1064 nm beam was selected and directed into a second integrating sphere and used for LII of light-absorbing kerosene lamp soot. Thermal denuder experiments showed the LII signals were not affected by the particle mixing state when laser peak power was 1.5-2.5 MW. The combined measurements of optical properties and soot mass concentration allowed determination of mass absorption cross section (M.A.C., m(2)/g) with 1 min time resolution when soot concentrations were in the low microgram per cubic meter range. Fresh kerosene nanosphere soot (ns-soot) exhibited a mean M.A.C and standard deviation of 9.3 ± 2.7 m(2)/g while limited measurements on dry ambient aerosol yielded an average of 8.2 ± 5.9 m(2)/g when soot was >0.25 μg/m(3). The method also detected increases in M.A.C. values associated with enhanced light absorption when polydisperse, laboratory-generated ns-soot particles were embedded within or coated with ammonium nitrate, ammonium sulfate, and glycerol. Glycerol coatings produced the largest fractional increase in M.A.C. (1.41-fold increase), while solid coatings of ammonium sulfate and ammonium nitrate produced increases of 1.10 and 1.06, respectively. Fresh, ns-soot did not exhibit increased M.A.C. at high relative humidity (RH); however, lab-generated soot coated with ammonium nitrate and held at 85% RH exhibited M.A.C. values nearly double the low-humidity case. The hybrid instrument for simultaneously tracking soot mass concentration and aerosol optical properties in real time is a

T-matrix modeling of linear depolarization by morphologically complex soot and soot-containing aerosols

Science.gov (United States)

Mishchenko, Michael I.; Liu, Li; Mackowski, Daniel W.

2013-07-01

We use state-of-the-art public-domain Fortran codes based on the T-matrix method to calculate orientation and ensemble averaged scattering matrix elements for a variety of morphologically complex black carbon (BC) and BC-containing aerosol particles, with a special emphasis on the linear depolarization ratio (LDR). We explain theoretically the quasi-Rayleigh LDR peak at side-scattering angles typical of low-density soot fractals and conclude that the measurement of this feature enables one to evaluate the compactness state of BC clusters and trace the evolution of low-density fluffy fractals into densely packed aggregates. We show that small backscattering LDRs measured with ground-based, airborne, and spaceborne lidars for fresh smoke generally agree with the values predicted theoretically for fluffy BC fractals and densely packed near-spheroidal BC aggregates. To reproduce higher lidar LDRs observed for aged smoke, one needs alternative particle models such as shape mixtures of BC spheroids or cylinders.

Fragmentation and bond strength of airborne diesel soot agglomerates

Directory of Open Access Journals (Sweden)

Messerer Armin

2008-06-01

Full Text Available Abstract Background The potential of diesel soot aerosol particles to break up into smaller units under mechanical stress was investigated by a direct impaction technique which measures the degree of fragmentation of individual agglomerates vs. impact energy. Diesel aerosol was generated by an idling diesel engine used for passenger vehicles. Both the aerosol emitted directly and aerosol that had undergone additional growth by Brownian coagulation ("aging" was investigated. Optionally a thermo-desoption technique at 280°C was used to remove all high-volatility and the majority of low-volatility HC adsorbates from the aerosol before aging. Results It was found that the primary soot agglomerates emitted directly from the engine could not be fragmented at all. Soot agglomerates permitted to grow additionally by Brownian coagulation of the primary emitted particles could be fragmented to a maximum of 75% and 60% respectively, depending on whether adsorbates were removed from their surface prior to aging or not. At most, these aged agglomerates could be broken down to roughly the size of the agglomerates from the primary emission. The energy required for a 50% fragmentation probability of all bonds within an agglomerate was reduced by roughly a factor of 2 when aging "dry" agglomerates. Average bond energies derived from the data were 0.52*10-16 and 1.2*10-16 J, respectively. This is about 2 orders of magnitude higher than estimates for pure van-der-Waals agglomerates, but agrees quite well with other observations. Conclusion Although direct conclusions regarding the behavior of inhaled diesel aerosol in contact with body fluids cannot be drawn from such measurements, the results imply that highly agglomerated soot aerosol particles are unlikely to break up into units smaller than roughly the size distribution emitted as tail pipe soot.

Fragmentation and bond strength of airborne diesel soot agglomerates

Science.gov (United States)

Rothenbacher, Sonja; Messerer, Armin; Kasper, Gerhard

2008-01-01

Background The potential of diesel soot aerosol particles to break up into smaller units under mechanical stress was investigated by a direct impaction technique which measures the degree of fragmentation of individual agglomerates vs. impact energy. Diesel aerosol was generated by an idling diesel engine used for passenger vehicles. Both the aerosol emitted directly and aerosol that had undergone additional growth by Brownian coagulation ("aging") was investigated. Optionally a thermo-desoption technique at 280°C was used to remove all high-volatility and the majority of low-volatility HC adsorbates from the aerosol before aging. Results It was found that the primary soot agglomerates emitted directly from the engine could not be fragmented at all. Soot agglomerates permitted to grow additionally by Brownian coagulation of the primary emitted particles could be fragmented to a maximum of 75% and 60% respectively, depending on whether adsorbates were removed from their surface prior to aging or not. At most, these aged agglomerates could be broken down to roughly the size of the agglomerates from the primary emission. The energy required for a 50% fragmentation probability of all bonds within an agglomerate was reduced by roughly a factor of 2 when aging "dry" agglomerates. Average bond energies derived from the data were 0.52*10-16 and 1.2*10-16 J, respectively. This is about 2 orders of magnitude higher than estimates for pure van-der-Waals agglomerates, but agrees quite well with other observations. Conclusion Although direct conclusions regarding the behavior of inhaled diesel aerosol in contact with body fluids cannot be drawn from such measurements, the results imply that highly agglomerated soot aerosol particles are unlikely to break up into units smaller than roughly the size distribution emitted as tail pipe soot. PMID:18533015

Aerosol Properties of the Atmospheres of Extrasolar Giant Planets

Energy Technology Data Exchange (ETDEWEB)

Lavvas, P. [Groupe de Spectrométrie Moléculaire et Atmosphérique, UMR CNRS 7331, Université de Reims Champagne Ardenne, Reims (France); Koskinen, T., E-mail: panayotis.lavvas@univ-reims.fr [Lunar and Planetary Laboratory, University of Arizona, Tucson, AZ (United States)

2017-09-20

We use a model of aerosol microphysics to investigate the impact of high-altitude photochemical aerosols on the transmission spectra and atmospheric properties of close-in exoplanets, such as HD 209458 b and HD 189733 b. The results depend strongly on the temperature profiles in the middle and upper atmospheres, which are poorly understood. Nevertheless, our model of HD 189733 b, based on the most recently inferred temperature profiles, produces an aerosol distribution that matches the observed transmission spectrum. We argue that the hotter temperature of HD 209458 b inhibits the production of high-altitude aerosols and leads to the appearance of a clearer atmosphere than on HD 189733 b. The aerosol distribution also depends on the particle composition, photochemical production, and atmospheric mixing. Due to degeneracies among these inputs, current data cannot constrain the aerosol properties in detail. Instead, our work highlights the role of different factors in controlling the aerosol distribution that will prove useful in understanding different observations, including those from future missions. For the atmospheric mixing efficiency suggested by general circulation models, we find that the aerosol particles are small (∼nm) and probably spherical. We further conclude that a composition based on complex hydrocarbons (soots) is the most likely candidate to survive the high temperatures in hot-Jupiter atmospheres. Such particles would have a significant impact on the energy balance of HD 189733 b’s atmosphere and should be incorporated in future studies of atmospheric structure. We also evaluate the contribution of external sources to photochemical aerosol formation and find that their spectral signature is not consistent with observations.

Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

OpenAIRE

Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

2014-01-01

Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as d...

Subsonic aircraft soot. A tracer documenting barriers to inter-hemispheric mixing

Energy Technology Data Exchange (ETDEWEB)

Pueschel, R F [NASA Ames Research Center, Moffett Field, CA (United States)

1998-12-31

Meridional observations of soot aerosols and radioactive {sup 14}C, and models of the geographic distribution of nuclear bomb-released {sup 14}C and aircraft-emitted NO{sub x}, all show strong gradients between the hemispheres. Reason for it are decade-long inter-hemispheric mixing times which are much in excess of yearlong stratospheric residence times of tracers. Vertical mixing of soot aerosol is not corroborated by {sup 14}C observations. The reason could be radiometric forces that act on strongly absorbing soot. (author) 10 refs.

Subsonic aircraft soot. A tracer documenting barriers to inter-hemispheric mixing

Energy Technology Data Exchange (ETDEWEB)

Pueschel, R.F. [NASA Ames Research Center, Moffett Field, CA (United States)

1997-12-31

Meridional observations of soot aerosols and radioactive {sup 14}C, and models of the geographic distribution of nuclear bomb-released {sup 14}C and aircraft-emitted NO{sub x}, all show strong gradients between the hemispheres. Reason for it are decade-long inter-hemispheric mixing times which are much in excess of yearlong stratospheric residence times of tracers. Vertical mixing of soot aerosol is not corroborated by {sup 14}C observations. The reason could be radiometric forces that act on strongly absorbing soot. (author) 10 refs.

Ambient Observations of Aerosols, Novel Aerosol Structures, And Their Engineering Applications

Science.gov (United States)

Beres, Nicholas D.

The role of atmospheric aerosols remains a crucial issue in understanding and mitigating climate change in our world today. These particles influence the Earth by altering the Earth's delicate radiation balance, human health, and visibility. In particular, black carbon particulate matter remains the key driver in positive radiative forcing (i.e., warming) due to aerosols. Produced from the incomplete combustion of hydrocarbons, these compounds can be found in many different forms around the globe. This thesis provides an overview of three research topics: (1) the ambient characterization of aerosols in the Northern Indian Ocean, measurement techniques used, and how these aerosols influence local, regional, and global climate; (2) the exploration of novel soot superaggregate particles collected in the Northern Indian Ocean and around the globe and how the properties of these particles relate to human health and climate forcing; and (3) how aerogelated soot can be produced in a novel, one-step method utilizing an inverted flame reactor and how this material could be used in industrial settings.

Mixing state of regionally transported soot particles and the coating effect on their size and shape at a mountain site in Japan

Science.gov (United States)

Adachi, Kouji; Zaizen, Yuji; Kajino, Mizuo; Igarashi, Yasuhito

2014-05-01

Soot particles influence the global climate through interactions with sunlight. A coating on soot particles increases their light absorption by increasing their absorption cross section and cloud condensation nuclei activity when mixed with other hygroscopic aerosol components. Therefore, it is important to understand how soot internally mixes with other materials to accurately simulate its effects in climate models. In this study, we used a transmission electron microscope (TEM) with an auto particle analysis system, which enables more particles to be analyzed than a conventional TEM. Using the TEM, soot particle size and shape (shape factor) were determined with and without coating from samples collected at a remote mountain site in Japan. The results indicate that ~10% of aerosol particles between 60 and 350 nm in aerodynamic diameters contain or consist of soot particles and ~75% of soot particles were internally mixed with nonvolatile ammonium sulfate or other materials. In contrast to an assumption that coatings change soot shape, both internally and externally mixed soot particles had similar shape and size distributions. Larger aerosol particles had higher soot mixing ratios, i.e., more than 40% of aerosol particles with diameters >1 µm had soot inclusions, whereas <20% of aerosol particles with diameters <1 µm included soot. Our results suggest that climate models may use the same size distributions and shapes for both internally and externally mixed soot; however, changing the soot mixing ratios in the different aerosol size bins is necessary.

Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

Science.gov (United States)

Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

2004-01-01

matter, and dust found for the ACE Asia aerosol are comparable to values estimated for ACE 1, Aerosols99, and INDOEX. Unique to the ACE Asia aerosol was the large mass fractions of dust, the dominance of dust in controlling the aerosol optical properties, and the interaction of dust with soot aerosol.

Absorbing Aerosols: Field and Laboratory Studies of Black Carbon and Dust

Science.gov (United States)

Aiken, A. C.; Flowers, B. A.; Dubey, M. K.

2011-12-01

Currently, absorbing aerosols are thought to be the most uncertain factor in atmospheric climate models (~0.4-1.2 W/m2), and the 2nd most important factor after CO2 in global warming (1.6 W/m2; Ramanathan and Carmichael, Nature Geoscience, 2008; Myhre, Science, 2009). While most well-recognized atmospheric aerosols, e.g., sulfate from power-plants, have a cooling effect on the atmosphere by scattering solar radiation, black carbon (BC or soot) absorbs sunlight strongly which results in a warming of the atmosphere. Dust particles are also present globally and can absorb radiation, contributing to a warmer and drier atmosphere. Direct on-line measurements of BC and hematite, an absorbing dust aerosol, can be made with the Single Particle Soot Photometer (SP2), which measures the mass of the particles by incandescence on an individual particle basis. Measurements from the SP2 are combined with absorption measurements from the three-wavelength photoacoustic soot spectrometer (PASS-3) at 405, 532, and 781 nm and the ultraviolet photoacoustic soot spectrometer (PASS-UV) at 375 nm to determine wavelength-dependent mass absorption coefficients (MACs). Laboratory aerosol samples include flame-generated soot, fullerene soot, Aquadag, hematite, and hematite-containing dusts. Measured BC MAC's compare well with published values, and hematite MAC's are an order of magnitude less than BC. Absorbing aerosols measured in the laboratory are compared with those from ambient aerosols measured during the Las Conchas fire and BEACHON-RoMBAS. The Las Conchas fire was a wildfire in the Jemez Mountains of New Mexico that burned over 100,000 acres during the Summer of 2011, and BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study) is a field campaign focusing on biogenic aerosols at the Manitou Forest Observatory near Colorado Springs, CO in Summer 2011. Optical properties and size

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.

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

1998-12-31

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.

Small particles big effect? - Investigating ice nucleation abilities of soot particles

Science.gov (United States)

Mahrt, Fabian; David, Robert O.; Lohmann, Ulrike; Stopford, Chris; Wu, Zhijun; Kanji, Zamin A.

2017-04-01

emissions. Collected particles will be re-suspended and aerosolized using an atomizer (TSI, model 3076) and dried by a diffusion drier prior to ice nucleation experiments. A Particle Phase Discriminator (PPD) coupled to HINC will allow discrimination of size-resolved liquid and ice hydrometeors formed on the atmospheric soot particles injected into the CFDC. This will allow to more precisely quantify the microphysical properties of these particles in cloud processes for the conditions tested. To our knowledge this is the first time such a coupling is done for atmospheric soot particles. Results show different activation behavior of the soot over the temperature range investigated. While CAST-brown soot needs conditions above water saturation to show any freezing, some of the commercial soot samples show heterogeneous ice nucleation well below water saturation for the cirrus conditions. For the mixed-phase cloud conditions all soot types show droplet activation for high water supersaturation.

Numerical simulations on the effect of aerosols on tropospheric chemistry and range of sight; Numerische Simulationen zur Wirkung des Aerosols auf die troposphaerische Chemie und die Sichtweite

Energy Technology Data Exchange (ETDEWEB)

Riemer, N.

2002-05-01

In this study the mesoscale KAMM/DRAS model system was extended by an MADE aerosol module with a view to studying tropospheric aerosols in terms of composition and size distribution in the greatest possible detail. In particular, the MADE aerosol module was supplemented by a routine for soot. This routine involves the parameterisation of the ageing process of soot through coagulation of soot particles with soluble particles and condensation of sulphuric acid on the soot particles. This transforms the soot from an external into an internal mixture and changes its hygroscopic properties. Thus extended the model system was used to study two aspects of the effects of aerosols on the physical and chemical environment of the troposphere. The first of these two tasks was to quantify the influence of heterogeneous hydrolysis of dinitrogen pentoxide (N{sub 2}O{sub 5}) on tropospheric chemistry under summer smog conditions. The second was to study the optical properties of aerosols. The paper shows a way of deriving extinction coefficients from the calculated aerosol distributions. This is then used as a starting point for developing a method for determining range of sight. [German] Das mesoskalige Modellsystem KAMM/DRAIS wird im Rahmen dieser Arbeit um das Aerosolmodul MADE erweitert, um das troposphaerische Aerosol sowohl bezueglich seiner Zusammensetzung als auch bezueglich seiner Groessenverteilung moeglichst detailliert zu behandeln. Insbesondere wird das Aerosolmodul MADE um die Behandlung der Substanz Russ ergaenzt. Hierbei wird der Alterungsprozess von Russ durch Koagulation der Russteilchen mit loeslichen Partikeln und durch Kondensation von Schwefelsaeure auf den Russpartikeln, wodurch der Russ von einer externen in eine interne Mischung uebergeht und seine hygroskopischen Eigenschaften aendert, parametrisiert. Mit dem so erweiterten Modellsystem wird fuer zwei Themenschwerpunkte die Wirkung des Aerosols auf die physikalischen und chemischen Bedingungen in der

Single-particle coherent diffractive imaging with a soft x-ray free electron laser: towards soot aerosol morphology

Science.gov (United States)

Bogan, Michael J.; Starodub, Dmitri; Hampton, Christina Y.; Sierra, Raymond G.

2010-10-01

The first of its kind, the Free electron LASer facility in Hamburg, FLASH, produces soft x-ray pulses with unprecedented properties (10 fs, 6.8-47 nm, 1012 photons per pulse, 20 µm diameter). One of the seminal FLASH experiments is single-pulse coherent x-ray diffractive imaging (CXDI). CXDI utilizes the ultrafast and ultrabright pulses to overcome resolution limitations in x-ray microscopy imposed by x-ray-induced damage to the sample by 'diffracting before destroying' the sample on sub-picosecond timescales. For many lensless imaging algorithms used for CXDI it is convenient when the data satisfy an oversampling constraint that requires the sample to be an isolated object, i.e. an individual 'free-standing' portion of disordered matter delivered to the centre of the x-ray focus. By definition, this type of matter is an aerosol. This paper will describe the role of aerosol science methodologies used for the validation of the 'diffract before destroy' hypothesis and the execution of the first single-particle CXDI experiments being developed for biological imaging. FLASH CXDI now enables the highest resolution imaging of single micron-sized or smaller airborne particulate matter to date while preserving the native substrate-free state of the aerosol. Electron microscopy offers higher resolution for single-particle analysis but the aerosol must be captured on a substrate, potentially modifying the particle morphology. Thus, FLASH is poised to contribute significant advancements in our knowledge of aerosol morphology and dynamics. As an example, we simulate CXDI of combustion particle (soot) morphology and introduce the concept of extracting radius of gyration of fractal aggregates from single-pulse x-ray diffraction data. Future upgrades to FLASH will enable higher spatially and temporally resolved single-particle aerosol dynamics studies, filling a critical technological need in aerosol science and nanotechnology. Many of the methodologies described for FLASH will

Single-particle coherent diffractive imaging with a soft x-ray free electron laser: towards soot aerosol morphology

International Nuclear Information System (INIS)

Bogan, Michael J; Starodub, Dmitri; Hampton, Christina Y; Sierra, Raymond G

2010-01-01

The first of its kind, the Free electron LASer facility in Hamburg, FLASH, produces soft x-ray pulses with unprecedented properties (10 fs, 6.8-47 nm, 10 12 photons per pulse, 20 μm diameter). One of the seminal FLASH experiments is single-pulse coherent x-ray diffractive imaging (CXDI). CXDI utilizes the ultrafast and ultrabright pulses to overcome resolution limitations in x-ray microscopy imposed by x-ray-induced damage to the sample by 'diffracting before destroying' the sample on sub-picosecond timescales. For many lensless imaging algorithms used for CXDI it is convenient when the data satisfy an oversampling constraint that requires the sample to be an isolated object, i.e. an individual 'free-standing' portion of disordered matter delivered to the centre of the x-ray focus. By definition, this type of matter is an aerosol. This paper will describe the role of aerosol science methodologies used for the validation of the 'diffract before destroy' hypothesis and the execution of the first single-particle CXDI experiments being developed for biological imaging. FLASH CXDI now enables the highest resolution imaging of single micron-sized or smaller airborne particulate matter to date while preserving the native substrate-free state of the aerosol. Electron microscopy offers higher resolution for single-particle analysis but the aerosol must be captured on a substrate, potentially modifying the particle morphology. Thus, FLASH is poised to contribute significant advancements in our knowledge of aerosol morphology and dynamics. As an example, we simulate CXDI of combustion particle (soot) morphology and introduce the concept of extracting radius of gyration of fractal aggregates from single-pulse x-ray diffraction data. Future upgrades to FLASH will enable higher spatially and temporally resolved single-particle aerosol dynamics studies, filling a critical technological need in aerosol science and nanotechnology. Many of the methodologies described for FLASH will

Laboratory Experiments and Instrument Development for the Study of Atmospheric Aerosols

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul

2011-12-10

Soot particles are generated by incomplete combustion of fossil and biomass fuels. Through direct effects clear air aerosols containing black carbon (BC) such as soot aerosols, absorb incoming light heating the atmosphere, while most other aerosols scatter light and produce cooling. Even though BC represents only 1-2% of the total annual emissions of particulate mass to the atmosphere, it has been estimated that the direct radiative effect of BC is the second-most important contributor to global warming after absorption by CO2. Ongoing studies continue to underscore the climate forcing importance of black carbon. However, estimates of the radiative effects of black carbon on climate remain highly uncertain due to the complexity of particles containing black carbon. Quantitative measurement of BC is challenging because BC often occurs in highly non-spherical soot particles of complex morphology. Freshly emitted soot particles are typically fractal hydrophobic aggregates. The aggregates consist of black carbon spherules with diameters typically in the range of about 15-40 nm, and they are usually coated by adsorbed polyaromatic hydrocarbons (PAHs) produced during combustion. Diesel-generated soot particles are often emitted with an organic coating composed primarily of lubricating oil and unburned fuel, as well as well as PAH compounds. Sulfuric acid has also been detected in diesel and aircraft-emitted soot particles. In the course of aging, these particle coatings may be substantially altered by chemical reactions and/or the deposition of other materials. Such processes transform the optical and CCN properties of the soot aerosols in ways that are not yet well understood. Our work over the past seven years consisted of laboratory research, instrument development and characterization, and field studies with the central focus of improving our understanding of the black carbon aerosol climate impacts. During the sixth year as well as during this seventh year (no

Effects of Large Polycyclic Aromatic Hydrocarbons on the Soot Formation in Ethylene-Air Nonpremixed Flames

KAUST Repository

Prabhu, S.; Arias, P.G.; Wang, Y.; Gao, Y.; Park, S.; Im, Hong G.; Sarathy, Mani; Chung, Suk-Ho; Lu, T.

2015-01-01

This study presents updated comprehensive gas-phase kinetic mechanism and aerosol models to predict soot formation characteristics in ethylene-air nonpremixed flames. A main objective is to investigate the sensitivity of the soot formation rate to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph (DRG) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames of pure ethylene at low strain rate sooting conditions are considered, for which the sensitivity of soot formation characteristics with respect to hetrogeneous nucleation is investigated. Results show that higher PAH concentrations result in higher soot nucleation rate, and that the average size of the particles are in good agreement with experimental results. It is found that the nucleation processes (i.e., soot inception) from higher PAH precursors, coronene in particular, is critical for accurate prediction of the overall soot formation.

Effects of Large Polycyclic Aromatic Hydrocarbons on the Soot Formation in Ethylene-Air Nonpremixed Flames

KAUST Repository

Prabhu, S.

2015-03-30

This study presents updated comprehensive gas-phase kinetic mechanism and aerosol models to predict soot formation characteristics in ethylene-air nonpremixed flames. A main objective is to investigate the sensitivity of the soot formation rate to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph (DRG) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames of pure ethylene at low strain rate sooting conditions are considered, for which the sensitivity of soot formation characteristics with respect to hetrogeneous nucleation is investigated. Results show that higher PAH concentrations result in higher soot nucleation rate, and that the average size of the particles are in good agreement with experimental results. It is found that the nucleation processes (i.e., soot inception) from higher PAH precursors, coronene in particular, is critical for accurate prediction of the overall soot formation.

Impact of morphology on the radiative properties of fractal soot aggregates

International Nuclear Information System (INIS)

Doner, Nimeti; Liu, Fengshan

2017-01-01

The impact of morphology on the radiative properties of fractal soot aggregates was investigated using the discrete dipole approximation (DDA). The optical properties of four different types of aggregates of freshly emitted soot with a fractal dimension D f =1.65 and a fractal pre-factor k f =1.76 were calculated. The four types of aggregates investigated are formed by uniform primary particles in point-touch, by uniform but overlapping primary particles, by uniform but enlarged primary particles in point-touch, and formed by point-touch and polydisperse primary particles. The radiative properties of aggregates consisting of N=20, 56 and 103 primary particles were numerically evaluated for a given refractive index at 0.532 and 1.064 μm. The radiative properties of soot aggregates vary strongly with the volume equivalent radius a eff and wavelength. The accuracy of DDA was evaluated in the first and fourth cases against the generalized multi-sphere Mie (GMM) solution in terms of the vertical–vertical differential scattering cross section (C vv ). The model predicted the average relative deviations from the base case to be within 15–25% for C vv , depending on the number of particles for the aggregate. The scattering cross sections are only slightly affected by the overlapping but more significantly influenced by primary particle polydispersity. It was also found that the enlargement of primary particles by 20% has a strong effect on soot aggregate radiative properties. - Highlights: • The radiative properties of aggregates of N=20, 56 and 103 primary particles were investigated. • Four different cases, formed by point-touch, overlapping, aggregate expansion and polydispersion, were studied. • The effects of overlapping and aggregate expansion on morphology are found to be the same.

A review of optical measurements at the aerosol and cloud chamber AIDA

International Nuclear Information System (INIS)

Wagner, Robert; Linke, Claudia; Naumann, Karl-Heinz; Schnaiter, Martin; Vragel, Marlen; Gangl, Martin; Horvath, Helmuth

2009-01-01

This paper provides a survey of recent studies on the optical properties of aerosol and cloud particles that have been conducted at the AIDA facility of Forschungszentrum Karlsruhe (Aerosol Interactions and Dynamics in the Atmosphere). Reflecting the broad accessible temperature range of the AIDA chamber which extends from ambient temperature down to 183 K, the investigations feature a broad diversity of research topics, such as the wavelength-dependence of the specific absorption cross sections of soot and mineral dust aerosols at room temperature, depolarization and infrared extinction measurements of ice crystal clouds generated at temperatures below 235 K, and the optical properties of polar stratospheric cloud constituents whose formation was studied in chamber experiments at temperatures well below 200 K. After reviewing the AIDA research activity of the past decade and introducing the optical instrumentation of the AIDA facility, this paper presents illustrative examples of ongoing and already published work on optical measurements of soot aerosols, mineral dust particles, and ice crystal clouds.

Black carbon aerosol properties measured by a single particle soot photometer in emissions from biomass burning in the laboratory and field

Science.gov (United States)

G. R. McMeeking; J. W. Taylor; A. P. Sullivan; M. J. Flynn; S. K. Akagi; C. M. Carrico; J. L. Collett; E. Fortner; T. B. Onasch; S. M. Kreidenweis; R. J. Yokelson; C. Hennigan; A. L. Robinson; H. Coe

2010-01-01

We present SP2 observations of BC mass, size distributions and mixing state in emissions from laboratory and field biomass fires in California, USA. Biomass burning is the primary global black carbon (BC) source, but understanding of the amount emitted and its physical properties at and following emission are limited. The single particle soot photometer (SP2) uses a...

Sooting turbulent jet flame: characterization and quantitative soot measurements

Science.gov (United States)

Köhler, M.; Geigle, K. P.; Meier, W.; Crosland, B. M.; Thomson, K. A.; Smallwood, G. J.

2011-08-01

Computational fluid dynamics (CFD) modelers require high-quality experimental data sets for validation of their numerical tools. Preferred features for numerical simulations of a sooting, turbulent test case flame are simplicity (no pilot flame), well-defined boundary conditions, and sufficient soot production. This paper proposes a non-premixed C2H4/air turbulent jet flame to fill this role and presents an extensive database for soot model validation. The sooting turbulent jet flame has a total visible flame length of approximately 400 mm and a fuel-jet Reynolds number of 10,000. The flame has a measured lift-off height of 26 mm which acts as a sensitive marker for CFD model validation, while this novel compiled experimental database of soot properties, temperature and velocity maps are useful for the validation of kinetic soot models and numerical flame simulations. Due to the relatively simple burner design which produces a flame with sufficient soot concentration while meeting modelers' needs with respect to boundary conditions and flame specifications as well as the present lack of a sooting "standard flame", this flame is suggested as a new reference turbulent sooting flame. The flame characterization presented here involved a variety of optical diagnostics including quantitative 2D laser-induced incandescence (2D-LII), shifted-vibrational coherent anti-Stokes Raman spectroscopy (SV-CARS), and particle image velocimetry (PIV). Producing an accurate and comprehensive characterization of a transient sooting flame was challenging and required optimization of these diagnostics. In this respect, we present the first simultaneous, instantaneous PIV, and LII measurements in a heavily sooting flame environment. Simultaneous soot and flow field measurements can provide new insights into the interaction between a turbulent vortex and flame chemistry, especially since soot structures in turbulent flames are known to be small and often treated in a statistical manner.

Technical Note: The single particle soot photometer fails to reliably detect PALAS soot nanoparticles

Directory of Open Access Journals (Sweden)

M. Gysel

2012-12-01

Full Text Available The single particle soot photometer (SP2 uses laser-induced incandescence (LII for the measurement of atmospheric black carbon (BC particles. The BC mass concentration is obtained by combining quantitative detection of BC mass in single particles with a counting efficiency of 100% above its lower detection limit. It is commonly accepted that a particle must contain at least several tenths of a femtogram BC in order to be detected by the SP2.

Here we show the result that most BC particles from a PALAS spark discharge soot generator remain undetected by the SP2, even if their BC mass, as independently determined with an aerosol particle mass analyser (APM, is clearly above the typical lower detection limit of the SP2. Comparison of counting efficiency and effective density data of PALAS soot with flame generated soot (combustion aerosol standard burner, CAST, fullerene soot and carbon black particles (Cabot Regal 400R reveals that particle morphology can affect the SP2's lower detection limit. PALAS soot particles are fractal-like agglomerates of very small primary particles with a low fractal dimension, resulting in a very low effective density. Such loosely packed particles behave like "the sum of individual primary particles" in the SP2's laser. Accordingly, most PALAS soot particles remain undetected as the SP2's laser intensity is insufficient to heat the primary particles to their vaporisation temperature because of their small size (D_pp ≈ 5–10 nm. Previous knowledge from pulsed laser-induced incandescence indicated that particle morphology might have an effect on the SP2's lower detection limit, however, an increase of the lower detection limit by a factor of ∼5–10, as reported here for PALAS soot, was not expected.

In conclusion, the SP2's lower detection limit at a certain laser power depends primarily on the total BC mass per particle for compact particles with sufficiently high effective

Cavity Ring-Down Measurement of Aerosol Optical Properties During the Asian Dust Above Monterey Experiment and DOE Aerosol Intensive Operating Period

Science.gov (United States)

Ricci, K.; Strawa, A. W.; Provencal, R.; Castaneda, R.; Bucholtz, A.; Schmid, B.

2004-01-01

Large uncertainties in the effects of aerosols on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This paper describes preliminary results from Cadenza, a new continuous wave cavity ring-down (CW-CRD) instrument designed to address these uncertainties. Cadenza measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. In the past year Cadenza was deployed in the Asian Dust Above Monterey (ADAM) and DOE Aerosol Intensive Operating Period (IOP) field projects. During these flights Cadenza produced measurements of aerosol extinction in the range from 0.2 to 300/Mm with an estimated precision of 0.1/Mm for 1550 nm light and 0.2/Mm for 675 nm light. Cadenza data from the ADAM and Aerosol IOP missions compared favorably with data from the other instruments aboard the CIRPAS Twin Otter aircraft and participating in those projects. We present comparisons between the Cadenza measurements and those from a TSI nephelometer, Particle Soot Absorption Photometer (PSAP), and the AATS 14 sun-photometer. Measurements of the optical properties of smoke and dust plumes sampled during these campaigns are presented and estimates of heating rates due to these plumes are made.

Estimating soot emissions from an elevated flare

Science.gov (United States)

Almanza, Victor; Sosa, Gustavo

2009-11-01

Combustion aerosols are one of the major concerns in flaring operations, due to both health and environmental hazards. Preliminary results are presented for a 2D transient simulation of soot formation in a reacting jet with exit velocity of 130 m/s under a 5 m/s crossflow released from a 50 m high elevated flare and a 50 cm nozzle. Combustion dynamics was simulated with OpenFOAM. Gas-phase non-premixed combustion was modeled with the Chalmers PaSR approach and a κ-ɛ turbulence model. For soot formation, Moss model was used and the ISAT algorithm for solving the chemistry. Sulfur chemistry was considered to account for the sourness of the fuel. Gas composition is 10 % H2S and 90 % C2H4. A simplified Glassman reaction mechanism was used for this purpose. Results show that soot levels are sensitive to the sulfur present in the fuel, since it was observed a slight decrease in the soot volume fraction. NSC is the current oxidation model for soot formation. Predicted temperature is high (about 2390 K), perhaps due to soot-radiation interaction is not considered yet, but a radiation model implementation is on progress, as well as an oxidation mechanism that accounts for OH radical. Flame length is about 50 m.

Minor and Trace Element Chemistry of Urban NS-Soot from the Central Valley of CA, USA

Science.gov (United States)

Kleich, S. J.; Hooper, R.

2017-12-01

During a recent study of metal transport in the Central Valley of California, it was noted that ns-soot (soot) occurred as complex clusters of graphene-like spheres admixed with other aerosols and were usually the dominant component of PM2.5 air particulates. These soot clusters contained a wide variety of metals of environmental concern such as As,Pb,Cr, and Ni. This study reports semi-quantitative results for 20 minor and trace elements (calibrated with Smithsonian microbeam standards) using a 200kV Transmission Electron Microscope, EDS, and SAED. This study also examined the mineralogy and crystallinity of admixed aerosols within composite soot clusters. Samples selected represent three contrasting urban settings in the Central Valley: Woodland, on the western side of the valley (Interstate highway to the east); Stockton, an inland sea-port and land transportation corridor in the center of the valley; and Roseville, a major rail-transport hub to the east. The wet/dry Mediterranean climate of California resulted in pronounced seasonal variations in total metal content. Soot cluster chemistry is highly variable however certain patterns emerged. Soot collected during the wet season is generally more aciniform, less structurally complex, and had lower sulfur (sulfate) concentrations but still had significant levels of transition metals (V,Cr,Mn,Fe,Ni,Zn and Pb) . Dry season soot was predominantly admixed with sulfate aerosols, and enriched in alkalis and alkaline earth metals. Stockton (wet-season) soot had up to 6000ppm of Pb. There is appreciable Pb (210ppm-2600ppm) in 38% of samples from Roseville but no Pb greater than 200ppm in Woodland. The highest overall total metals were found in Roseville soot with appreciable As(670ppm), V(100ppm), Pb(2600ppm), Zn(4000 ppm), Cr(90ppm), and Ni(300ppm). Heavy transport (road/rail/port) correlates with higher metal contents regardless of climate.

Smog chamber study on aging of combustion soot in isoprene/SO2/NOx system: Changes of mass, size, effective density, morphology and mixing state

Science.gov (United States)

Li, Kangwei; Chen, Linghong; Han, Ke; Lv, Biao; Bao, Kaiji; Wu, Xuecheng; Gao, Xiang; Cen, Kefa

2017-02-01

Atmospheric soot aging process is always accompanied by secondary particle formation, which is a comprehensive environmental issue that deserves great attention. On one hand, aging of primary soot could change its own physicochemical properties; on the other hand, complex air pollution caused by pollutant emission from various sources (e.g., vehicle exhausts, coal-fired flue gases and biogenic VOCs emission) may contribute to secondary particle formation onto primary particle surface. In this study, aging of combustion soot in isoprene/SO2/NOx system was investigated under controlled laboratory conditions in several smog chamber experiments. During the evolution of soot, several physical properties such as mass, size, effective density, morphology and mixing state were determined simultaneously by an integrated aerosol analytical system of Scanning Mobility Particle Sizer (SMPS), Differential Mobility Analyzer-Aerosol Particle Mass Analyzer-Condensation Particle Counter (DMA-APM-CPC) and Transmission Electron Microscopy coupled with Energy-dispersive X-ray Spectrometry (TEM/EDX) techniques. Here, based on the experimental results of soot aging under different gas-phase composition and relative humidity (RH), we firstly proposed possible aging pathways of soot in isoprene/SO2/NOx system. A synergetic effect was speculated to exist between SO2 and isoprene on soot aging process, which led to more secondary particle formation. At the same time, TEM/EDX analysis showed that a competitive mechanism between H2SO4(g) and isoprene oxidation vapor may exist: H2SO4(g) firstly condensed onto fresh soot, then an acceleration of isoprene oxidation products formed onto H2SO4 pre-coated soot. In isoprene/SO2/NOx system, high RH conditions could contribute to soot aging and new particle formation. The changes of effective density and dynamic shape factor of soot also indicated that high RH conditions could accelerate soot aging process, and led chain-like soot into more spherical

A computational study of ethylene–air sooting flames: Effects of large polycyclic aromatic hydrocarbons

KAUST Repository

Selvaraj, Prabhu

2015-11-05

An updated reduced gas-phase kinetic mechanism was developed and integrated with aerosol models to predict soot formation characteristics in ethylene nonpremixed and premixed flames. A primary objective is to investigate the sensitivity of the soot formation to various chemical pathways for large polycyclic aromatic hydrocarbons (PAH). The gas-phase chemical mechanism adopted the KAUST-Aramco PAH Mech 1.0, which utilized the AramcoMech 1.3 for gas-phase reactions validated for up to C2 fuels. In addition, PAH species up to coronene (C24H12 or A7) were included to describe the detailed formation pathways of soot precursors. In this study, the detailed chemical mechanism was reduced from 397 to 99 species using directed relation graph with expert knowledge (DRG-X) and sensitivity analysis. The method of moments with interpolative closure (MOMIC) was employed for the soot aerosol model. Counterflow nonpremixed flames at low strain rate sooting conditions were considered, for which the sensitivity of soot formation characteristics to different nucleation pathways were investigated. Premixed flame experiment data at different equivalence ratios were also used for validation. The findings show that higher PAH concentrations result in a higher soot nucleation rate, and that the total soot volume and average size of the particles are predicted in good agreement with experimental results. Subsequently, the effects of different pathways, with respect to pyrene- or coronene-based nucleation models, on the net soot formation rate were analyzed. It was found that the nucleation processes (i.e., soot inception) are sensitive to the choice of PAH precursors, and consideration of higher PAH species beyond pyrene is critical for accurate prediction of the overall soot formation.

Soot in the air may have serious climatic consequences

International Nuclear Information System (INIS)

Seip, Hans Martin

2002-01-01

Emissions of soot in China and India may be an important cause of changed summer weather in China, with increasing floods in the south-east and increasing droughts in the north-east. In addition to the greenhouse gases, the particulate matter (aerosols) in the air has an important effect on the climate. Most particles have a cooling effect since they reflect solar radiation. However, some particles are dark as they contain soot ('black carbon'). Such particles, which are formed by incomplete combustion of coal, oil and biomass, absorb solar radiation and thus have a warming effect, even if they reduce the solar irradiation on the ground. Soot particles do not have quite the same effect as the greenhouse gases. The soot particles absorb solar radiation, while the greenhouse gases absorb terrestrial heat radiation. In addition, the residence time of the soot particles in the atmosphere is shorter than that of, say, carbon dioxide. The concentration is therefore much higher in areas close to emission sources than elsewhere

How do the optical properties of Asian aerosols change when they cross the Pacific?

Science.gov (United States)

Fischer, E. V.; Jaffe, D. A.

2009-12-01

Primary and secondary aerosols from Asia may have important climate implications. These aerosols are emitted locally, but can then be lofted into the free troposphere and advected across the Pacific. In this analysis we used observations from the Mount Bachelor Observatory (MBO) in conjunction with satellite data to identify the dominant aerosol types in specific Asian plumes that crossed the Pacific. In situ data from MBO is used to understand the observed changes in radiative properties. A suite of gas phase and aerosol measurements were made during spring 2008 and spring 2009 at MBO (2763 masl), located in central Oregon. Here we focus on observations of dry sub-μm aerosol scattering (σsp) and absorption (σap), made with an integrating nephelometer and a particle soot absorption photometer (PSAP). Using a combination of backward trajectory calculations and satellite observations, we identified 7 well defined plumes of Asian origin. These plumes included the highest σsp (34.8 Mm-1 hourly average) and σap (4.8 Mm-1 hourly average) observed at MBO over the 2008 and 2009 spring campaigns. Of interest in this analysis is 1) whether the intensive optical properties differ between these 7 Asian events, 2) whether these differences can be linked to differences in composition, and 3) whether the intensive optical properties differ from those observed closer to the Asian source region. Preliminary results show that the plumes clustered in terms of their optical properties; plumes hypothesized to contain a large fraction of mineral dust were the most distinct. We also observed larger variability in the average scattering Ångstrom exponent of the plumes and a higher average single scatter albedo than observations closer to the Asian coast. This work will be extended to compare observations at MBO with the most recent observations from Asia as they become available.

A study of radiative properties of fractal soot aggregates using the superposition T-matrix method

International Nuclear Information System (INIS)

Li Liu; Mishchenko, Michael I.; Patrick Arnott, W.

2008-01-01

We employ the numerically exact superposition T-matrix method to perform extensive computations of scattering and absorption properties of soot aggregates with varying state of compactness and size. The fractal dimension, D f , is used to quantify the geometrical mass dispersion of the clusters. The optical properties of soot aggregates for a given fractal dimension are complex functions of the refractive index of the material m, the number of monomers N S , and the monomer radius a. It is shown that for smaller values of a, the absorption cross section tends to be relatively constant when D f f >2. However, a systematic reduction in light absorption with D f is observed for clusters with sufficiently large N S , m, and a. The scattering cross section and single-scattering albedo increase monotonically as fractals evolve from chain-like to more densely packed morphologies, which is a strong manifestation of the increasing importance of scattering interaction among spherules. Overall, the results for soot fractals differ profoundly from those calculated for the respective volume-equivalent soot spheres as well as for the respective external mixtures of soot monomers under the assumption that there are no electromagnetic interactions between the monomers. The climate-research implications of our results are discussed

Stratospheric Aerosol Measurements

Science.gov (United States)

Pueschel, Rudolf, F.; Gore, Warren J. (Technical Monitor)

1998-01-01

Stratospheric aerosols affect the atmospheric energy balance by scattering and absorbing solar and terrestrial radiation. They also can alter stratospheric chemical cycles by catalyzing heterogeneous reactions which markedly perturb odd nitrogen, chlorine and ozone levels. Aerosol measurements by satellites began in NASA in 1975 with the Stratospheric Aerosol Measurement (SAM) program, to be followed by the Stratospheric Aerosol and Gas Experiment (SAGE) starting in 1979. Both programs employ the solar occultation, or Earth limb extinction, techniques. Major results of these activities include the discovery of polar stratospheric clouds (PSCs) in both hemispheres in winter, illustrations of the impacts of major (El Chichon 1982 and Pinatubo 1991) eruptions, and detection of a negative global trend in lower stratospheric/upper tropospheric aerosol extinction. This latter result can be considered a triumph of successful worldwide sulfur emission controls. The SAGE record will be continued and improved by SAGE III, currently scheduled for multiple launches beginning in 2000 as part of the Earth Observing System (EOS). The satellite program has been supplemented by in situ measurements aboard the ER-2 (20 km ceiling) since 1974, and from the DC-8 (13 km ceiling) aircraft beginning in 1989. Collection by wire impactors and subsequent electron microscopic and X-ray energy-dispersive analyses, and optical particle spectrometry have been the principle techniques. Major findings are: (1) The stratospheric background aerosol consists of dilute sulfuric acid droplets of around 0.1 micrometer modal diameter at concentration of tens to hundreds of monograms per cubic meter; (2) Soot from aircraft amounts to a fraction of one percent of the background total aerosol; (3) Volcanic eruptions perturb the sulfuric acid, but not the soot, aerosol abundance by several orders of magnitude; (4) PSCs contain nitric acid at temperatures below 195K, supporting chemical hypotheses

Aerosol and Cloud Properties during the Cloud Cheju ABC Plume -Asian Monsoon Experiment (CAPMEX) 2008: Linking between Ground-based and UAV Measurements

Science.gov (United States)

Kim, S.; Yoon, S.; Venkata Ramana, M.; Ramanathan, V.; Nguyen, H.; Park, S.; Kim, M.

2009-12-01

Cheju Atmospheric Brown Cloud (ABC) Plume-Monsoon Experiment (CAPMEX), comprehsensive ground-based measurements and a series of data-gathering flights by specially equipped autonomous unmanned aerial vehicles (AUAVs) for aerosol and cloud, had conducted at Jeju (formerly, Cheju), South Korea during August-September 2008, to improve our understanding of how the reduction of anthropogenic emissions in China (so-called “great shutdown” ) during and after the Summer Beijing Olympic Games 2008 effcts on the air quliaty and radiation budgets and how atmospheric brown clouds (ABCs) influences solar radiation budget off Asian continent. Large numbers of in-situ and remote sensing instruments at the Gosan ABC observatory and miniaturized instruments on the aircraft measure a range of properties such as the quantity of soot, size-segregated aerosol particle numbers, total particle numbers, size-segregated cloud droplet numbers (only AUAV), aerosol scattering properties (only ground), aerosol vertical distribution, column-integrated aerosol properties, and meteorological variables. By integrating ground-level and high-elevation AUAV measurements with NASA-satellite observations (e.g., MODIS, CALIPSO), we investigate the long range transport of aerosols, the impact of ABCs on clouds, and the role of biogenic and anthropogenic aerosols on cloud condensation nuclei (CCN). In this talk, we will present the results from CAPMEX focusing on: (1) the characteristics of aerosol optical, physical and chemical properties at Gosan observatory, (2) aerosol solar heating calculated from the ground-based micro-pulse lidar and AERONET sun/sky radiometer synergy, and comparison with direct measurements from UAV, and (3) aerosol-cloud interactions in conjunction with measurements by satellites and Gosan observatory.

Laboratory and modeling studies on the effects of water and soot emissions and ambient conditions on the properties of contrail ice particles in the jet regime

Directory of Open Access Journals (Sweden)

H.-W. Wong

2013-10-01

Full Text Available Contrails and contrail-induced cirrus clouds are identified as the most uncertain components in determining aviation impacts on global climate change. Parameters affecting contrail ice particle formation immediately after the engine exit plane (< 5 s in plume age may be critical to ice particle properties used in large-scale models predicting contrail radiative forcing. Despite this, detailed understanding of these parametric effects is still limited. In this paper, we present results from recent laboratory and modeling studies conducted to investigate the effects of water and soot emissions and ambient conditions on near-field formation of contrail ice particles and ice particle properties. The Particle Aerosol Laboratory (PAL at the NASA Glenn Research Center and the Aerodyne microphysical parcel model for contrail ice particle formation were employed. Our studies show that exhaust water concentration has a significant impact on contrail ice particle formation and properties. When soot particles were introduced, ice particle formation was observed only when exhaust water concentration was above a critical level. When no soot or sulfuric acid was introduced, no ice particle formation was observed, suggesting that ice particle formation from homogeneous nucleation followed by homogeneous freezing of liquid water was unfavorable. Soot particles were found to compete for water vapor condensation, and higher soot concentrations emitted into the chamber resulted in smaller ice particles being formed. Chamber conditions corresponding to higher cruising altitudes were found to favor ice particle formation. The microphysical model captures trends of particle extinction measurements well, but discrepancies between the model and the optical particle counter measurements exist as the model predicts narrower ice particle size distributions and ice particle sizes nearly a factor of two larger than measured. These discrepancies are likely due to particle

Evolution of biomass burning aerosol over the Amazon: airborne measurements of aerosol chemical composition, microphysical properties, mixing state and optical properties during SAMBBA

Science.gov (United States)

Morgan, W.; Allan, J. D.; Flynn, M.; Darbyshire, E.; Hodgson, A.; Liu, D.; O'Shea, S.; Bauguitte, S.; Szpek, K.; Johnson, B.; Haywood, J.; Longo, K.; Artaxo, P.; Coe, H.

2013-12-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. On regional scales, the impacts are substantial, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated in the Cerrado. This led to significant differences in aerosol chemical composition, particularly in terms of the BC content, with BC being enhanced in the Cerrado

Dynamics of flow–soot interaction in wrinkled non-premixed ethylene–air flames

KAUST Repository

Arias, Paul G.

2015-08-17

A two-dimensional simulation of a non-premixed ethylene–air flame was conducted by employing a detailed gas-phase reaction mechanism considering polycyclic aromatic hydrocarbons, an aerosol-dynamics-based soot model using a method of moments with interpolative closure, and a grey gas and soot radiation model using the discrete transfer method. Interaction of the sooting flame with a prescribed decaying random velocity field was investigated, with a primary interest in the effects of velocity fluctuations on the flame structure and the associated soot formation process for a fuel-strip configuration and a composition with mature soot growth. The temporally evolving simulation revealed a multi-layered soot formation process within the flame, at a level of detail not properly described by previous studies based on simplified soot models utilizing acetylene or naphthalene precursors for initial soot inception. The overall effect of the flame topology on the soot formation was found to be consistent with previous experimental studies, while a unique behaviour of localised strong oxidation was also noted. The imposed velocity fluctuations led to an increase of the scalar dissipation rate in the sooting zone, causing a net suppression in the soot production rate. Considering the complex structure of the soot formation layer, the effects of the imposed fluctuations vary depending on the individual soot reactions. For the conditions under study, the soot oxidation reaction was identified as the most sensitive to the fluctuations and was mainly responsible for the local suppression of the net soot production. © 2015 Taylor & Francis

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

Directory of Open Access Journals (Sweden)

J. Wang

2016-07-01

Full Text Available In this work, the Aerodyne soot particle – aerosol mass spectrometer (SP-AMS was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD of China, for online characterization of the submicron aerosols (PM1. The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics. The average PM1 concentration was found to be 28.2 µg m−3, with organics (45 % as the most abundant component, following by sulfate (19.3 %, nitrate (13.6 %, ammonium (11.1 %, rBC (9.7 %, and chloride (1.3 %. These PM1 species together can reconstruct ∼ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (< 100 nm vacuum aerodynamic diameter were dominated by organics and rBC, while large particles had significant contributions from secondary inorganic species. Source apportionment of organic aerosols (OA yielded four OA subcomponents, including hydrocarbon-like OA (HOA, cooking-related OA (COA, semi-volatile oxygenated OA (SV-OOA, and low-volatility oxygenated OA (LV-OOA. Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA dominated the total OA mass (55.5 %, but primary organic aerosol (POA, equal to the sum of HOA and COA can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand

Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

Science.gov (United States)

Wang, Junfeng; Ge, Xinlei; Chen, Yanfang; Shen, Yafei; Zhang, Qi; Sun, Yele; Xu, Jianzhong; Ge, Shun; Yu, Huan; Chen, Mindong

2016-07-01

In this work, the Aerodyne soot particle - aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m-3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ˜ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (cooking-related OA (COA), semi-volatile oxygenated OA (SV-OOA), and low-volatility oxygenated OA (LV-OOA). Overall, secondary organic aerosol (SOA, equal to the sum of SV-OOA and LV-OOA) dominated the total OA mass (55.5 %), but primary organic aerosol (POA, equal to the sum of HOA and COA) can outweigh SOA in the early morning and evening due to enhanced human activities. High OA concentrations were often associated with high mass fractions of POA and rBC, indicating the important role of anthropogenic emissions during heavy pollution events. The diurnal cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species, sulfate, and LV-OOA concentrations increased in the afternoon, and showed no positive correlations with relative humidity (RH), likely indicating the contribution from photochemical oxidation is dominant over that of aqueous-phase processing for their formations. The

Dynamics of flow–soot interaction in wrinkled non-premixed ethylene–air flames

KAUST Repository

Arias, Paul G.; Lecoustre, Vivien R.; Roy, Somesh; Luo, Zhaoyu; Haworth, Daniel C.; Lu, Tianfeng; Trouvé , Arnaud; Im, Hong G.

2015-01-01

A two-dimensional simulation of a non-premixed ethylene–air flame was conducted by employing a detailed gas-phase reaction mechanism considering polycyclic aromatic hydrocarbons, an aerosol-dynamics-based soot model using a method of moments

Development of high fidelity soot aerosol dynamics models using method of moments with interpolative closure

KAUST Repository

Roy, Subrata P.

2014-01-28

The method of moments with interpolative closure (MOMIC) for soot formation and growth provides a detailed modeling framework maintaining a good balance in generality, accuracy, robustness, and computational efficiency. This study presents several computational issues in the development and implementation of the MOMIC-based soot modeling for direct numerical simulations (DNS). The issues of concern include a wide dynamic range of numbers, choice of normalization, high effective Schmidt number of soot particles, and realizability of the soot particle size distribution function (PSDF). These problems are not unique to DNS, but they are often exacerbated by the high-order numerical schemes used in DNS. Four specific issues are discussed in this article: the treatment of soot diffusion, choice of interpolation scheme for MOMIC, an approach to deal with strongly oxidizing environments, and realizability of the PSDF. General, robust, and stable approaches are sought to address these issues, minimizing the use of ad hoc treatments such as clipping. The solutions proposed and demonstrated here are being applied to generate new physical insight into complex turbulence-chemistry-soot-radiation interactions in turbulent reacting flows using DNS. © 2014 Copyright Taylor and Francis Group, LLC.

Incipient Soot Formation in Rich Partially Premixed Flames under High Pressure Conditions of Relevance to Compression-Ignition Engines

Science.gov (United States)

2017-09-09

a Laminar Premixed Flame, Aerosol Reaction Engineering , Center for Aerosol science and Engineering (CASE) Workshop 2016, Saint Louis, Missouri, May...Publication Type: Conference Paper or Presentation Conference Name: Aerosol Reaction Engineering , Center for Aerosol science and Engineering (CASE...measurements of critical soot precursors up to 3-ring aromatics is available online to modelers to improve the chemical reaction mechanism [24]. To give a

Effect of Coatings on the Uptake Rate and HONO Yield in Heterogeneous Reaction of Soot with NO2

Science.gov (United States)

Cruz-Quiñones, M.; Khalizov, A. F.; Zhang, R.

2009-12-01

Heterogeneous reaction of nitrogen dioxide on carbon soot aerosols has been suggested as a possible source of nighttime nitrous acid (HONO) in atmosphere boundary layer. Available laboratory data show significant variability in the measured reaction probabilities and HONO yields, making it difficult to asses the atmospheric significance of this process. Moreover, little is known of how aging of soot aerosol through internal mixing with other atmospheric trace constituents will affect the heterogeneous reactivity and HONO production. In this work, the heterogeneous reaction of NO2 on fresh and aged soot films leading to HONO formation was studied through a series of kinetic uptake experiments and HONO yield measurements. Soot samples were prepared by incomplete combustion of propane and kerosene fuels under lean and rich flame conditions. Experiments were performed in a low-pressure, fast-flow reactor coupled to a chemical ionization mass spectrometer (CIMS), using atmospheric-level NO2 concentrations. Heterogeneous uptake coefficients, γ(geom) and γ(BET), were calculated using geometric and internal BET soot surface areas, respectively. The uptake coefficient and the HONO yield depend on the type of fuel and combustion regime and are the highest for soot samples prepared using rich kerosene flame. Although, the internal surface area of soot measured by BET method is a factor of 50 to 500 larger than the geometric surface area, only the top soot layers are involved in heterogeneous reaction with NO2 as follows from the observed weak dependence of γ(geom) and decrease in γ(BET) with increasing sample mass. Heating the soot samples before exposure to NO2 increases the BET surface area, the HONO yield, and the NO2 uptake coefficient due to the removal of the organic fraction from the soot backbone that unblocks active sites and makes them accessible for physical adsorption and chemical reactions. Our results support the oxidation-reduction mechanism involving

Experimental determination of soot refractive index in the infrared

International Nuclear Information System (INIS)

Ouf, F.X.; Vendel, J.; Ouf, F.X.; Coppalle, A.; Weil, M.E.; Yon, J.

2007-01-01

The study of physical properties of soot particles produced during combustion is a complex subject but of a great interest within the framework of the study of the safety of an installation, with respect to the fire hazard. These characteristics are, in this case, particularly useful in order to predict the behaviour of containment barriers in situation of fire, but also in order to estimate the contribution of these particles to radiative transfers. The aim of this study is to determine the radiative properties of soot particles produced during combustion. A specific device, which establishes extinction and vertical-vertical scattering coefficients, has been developed and has allowed to determine the refractive index of soot particles in the infrared. This determination also needed the establishment of size distribution and morphological properties of soot aggregates. We present in this document the experimental device developed, and the validation of this device on latex spheres which optical properties are well known. First results of extinction coefficients will be presented and will underline the similar optical behaviour of different soot aggregates. Values of refractive index will be detailed and discussed, and a direct application of these values will be carried out in order to determine the soot volume fraction. A comparison with reference method will underline the efficiency of our method. We will conclude on the validity of the information brought by this device and on the prospects of this study. A discussion is included, on the utility of mean values of refractive index and on the determination of total emissivity of soot particles. (authors)

Modelling heterogeneous ice nucleation on mineral dust and soot with parameterizations based on laboratory experiments

Science.gov (United States)

Hoose, C.; Hande, L. B.; Mohler, O.; Niemand, M.; Paukert, M.; Reichardt, I.; Ullrich, R.

2016-12-01

Between 0 and -37°C, ice formation in clouds is triggered by aerosol particles acting as heterogeneous ice nuclei. At lower temperatures, heterogeneous ice nucleation on aerosols can occur at lower supersaturations than homogeneous freezing of solutes. In laboratory experiments, the ability of different aerosol species (e.g. desert dusts, soot, biological particles) has been studied in detail and quantified via various theoretical or empirical parameterization approaches. For experiments in the AIDA cloud chamber, we have quantified the ice nucleation efficiency via a temperature- and supersaturation dependent ice nucleation active site density. Here we present a new empirical parameterization scheme for immersion and deposition ice nucleation on desert dust and soot based on these experimental data. The application of this parameterization to the simulation of cirrus clouds, deep convective clouds and orographic clouds will be shown, including the extension of the scheme to the treatment of freezing of rain drops. The results are compared to other heterogeneous ice nucleation schemes. Furthermore, an aerosol-dependent parameterization of contact ice nucleation is presented.

Lanthanum-promoted copper-based hydrotalcites derived mixed oxides for NO{sub x} adsorption, soot combustion and simultaneous NO{sub x}-soot removal

Energy Technology Data Exchange (ETDEWEB)

Wang, Zhongpeng [School of Resources and Environment, University of Jinan, 106 Jiwei Road, Jinan 250022 (China); Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, Oxford OX1 3QR (United Kingdom); Yan, Xiaotong; Bi, Xinlin; Wang, Liguo [School of Resources and Environment, University of Jinan, 106 Jiwei Road, Jinan 250022 (China); Zhang, Zhaoliang, E-mail: chm_zhangzl@ujn.edu.cn [School of Resources and Environment, University of Jinan, 106 Jiwei Road, Jinan 250022 (China); Jiang, Zheng; Xiao, Tiancun [Inorganic Chemistry Laboratory, University of Oxford, South Parks Road, Oxford OX1 3QR (United Kingdom); Umar, Ahmad [Department of Chemistry, College of Science and Arts, Najran University, P.O. Box 1988, Najran 11001 (Saudi Arabia); Promising Centre for Sensors and Electronic Devices (PCSED), Najran University, P.O. Box 1988, Najran 11001 (Saudi Arabia); Wang, Qiang, E-mail: qiang.wang.ox@gmail.com [College of Environmental Science and Engineering, Beijing Forestry University, 35 Tsinghua East Road, Beijing 100083 (China)

2014-03-01

Graphical abstract: - Highlights: • The addition of La in Cu-based oxides increased the types of active oxygen. • NO{sub x} adsorption, soot oxidation and simultaneous NO{sub x}-soot removal were enhanced. • The possible catalytic mechanism was studied via in situ FTIR analysis. • Soot oxidation was promoted by the NO{sub 2} intermediate. - Abstract: La-promoted Cu-based hydrotalcites derived mixed oxides were prepared and their catalytic activities for NO{sub x} adsorption, soot oxidation, and simultaneous NO{sub x}-soot removal were investigated. The catalysts were characterized by XRD, DTG, BET, FTIR, H2-TPR, TPD and TPO techniques. The oxides catalysts exhibited mesoporous properties with specific surface area of 45–160 m{sup 2}/g. The incorporation of La and Cu decreased the amount of basic sites due to the large decrease in surface areas. Under O{sub 2} atmosphere, La incorporation is dominant for soot oxidation activity, while Cu favors high selectivity to CO{sub 2} formation. A synergetic effect between La and Cu for catalyzed soot oxidation lies in the improved redox property and suitable basicity. The presence of NO in O{sub 2} significantly promoted soot oxidation on the catalysts with the ignition temperature decreased to about 300 °C. In O{sub 2}/NO atmosphere, NO{sub 2} acts as an intermediate which oxidizes soot to CO{sub 2} at a lower temperature with itself reduced to NO or N{sub 2}, contributing to the high catalytic performance in simultaneous removal of NO{sub x} and soot.

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

New Nanotech from an Ancient Material: Chemistry Demonstrations Involving Carbon-Based Soot

Science.gov (United States)

Campbell, Dean J.; Andrews, Mark J.; Stevenson, Keith J.

2012-01-01

Carbon soot has been known since antiquity, but has recently been finding new uses as a robust, inexpensive nanomaterial. This paper describes the superhydrophobic properties of carbon soot films prepared by combustion of candle wax or propane gas and introduces some of the optical absorption and fluorescence properties of carbon soot particles.…

Experiments and Model Development for the Investigation of Sooting and Radiation Effects in Microgravity Droplet Combustion

Science.gov (United States)

Choi, Mun Young; Yozgatligil, Ahmet; Dryer, Frederick L.; Kazakov, Andrei; Dobashi, Ritsu

2001-01-01

Today, despite efforts to develop and utilize natural gas and renewable energy sources, nearly 97% of the energy used for transportation is derived from combustion of liquid fuels, principally derived from petroleum. While society continues to rely on liquid petroleum-based fuels as a major energy source in spite of their finite supply, it is of paramount importance to maximize the efficiency and minimize the environmental impact of the devices that burn these fuels. The development of improved energy conversion systems, having higher efficiencies and lower emissions, is central to meeting both local and regional air quality standards. This development requires improvements in computational design tools for applied energy conversion systems, which in turn requires more robust sub-model components for combustion chemistry, transport, energy transport (including radiation), and pollutant emissions (soot formation and burnout). The study of isolated droplet burning as a unidimensional, time dependent model diffusion flame system facilitates extensions of these mechanisms to include fuel molecular sizes and pollutants typical of conventional and alternative liquid fuels used in the transportation sector. Because of the simplified geometry, sub-model components from the most detailed to those reduced to sizes compatible for use in multi-dimensional, time dependent applied models can be developed, compared and validated against experimental diffusion flame processes, and tested against one another. Based on observations in microgravity experiments on droplet combustion, it appears that the formation and lingering presence of soot within the fuel-rich region of isolated droplets can modify the burning rate, flame structure and extinction, soot aerosol properties, and the effective thermophysical properties. These observations led to the belief that perhaps one of the most important outstanding contributions of microgravity droplet combustion is the observation that in the

Effect of soot on oil properties and wear of engine components

International Nuclear Information System (INIS)

Green, D A; Lewis, R

2007-01-01

The objective of the work outlined in this paper was to increase the understanding of the wear mechanisms that occur within a soot contaminated contact zone, to help in future development of a predictive wear model to assist in the automotive engine valve train design process. The paper builds on previous work by the author, through testing of different lubricants and increased levels of soot contamination. Wear testing has been carried out using specimens operating under realistic engine conditions, using a reciprocating test-rig specifically designed for this application, where a steel disc is held in a heated bath of oil and a steel ball is attached to a reciprocating arm (replicating a sliding elephant's foot valve train contact). Detailed analysis of the test specimens has been performed using scanning electron microscopy to identify wear features relating to the proposed wear mechanisms. Analysis of worn engine components from durability engine tests has also been carried out for a comparison between specimen tests and engine testing. To assist the understanding of the wear test results obtained, the physical properties of contaminated lubricants were investigated, through viscosity, traction and friction measurements. The results have revealed how varying lubrication conditions change the wear rate of engine components and determine the wear mechanism that dominates in specific situations. Testing has also shown the positive effects of advanced engine lubricants to reduce the amount of wear produced with soot present

Application of a robust and efficient Lagrangian particle scheme to soot transport in turbulent flames

KAUST Repository

Attili, Antonio

2013-09-01

A Lagrangian particle scheme is applied to the solution of soot dynamics in turbulent nonpremixed flames. Soot particulate is described using a method of moments and the resulting set of continuum advection-reaction equations is solved using the Lagrangian particle scheme. The key property of the approach is the independence between advection, described by the movement of Lagrangian notional particles along pathlines, and internal aerosol processes, evolving on each notional particle via source terms. Consequently, the method overcomes the issues in Eulerian grid-based schemes for the advection of moments: errors in the advective fluxes pollute the moments compromising their realizability and the stiffness of source terms weakens the stability of the method. The proposed scheme exhibits superior properties with respect to conventional Eulerian schemes in terms of stability, accuracy, and grid convergence. Taking into account the quality of the solution, the Lagrangian approach can be computationally more economical than commonly used Eulerian schemes as it allows the resolution requirements dictated by the different physical phenomena to be independently optimized. Finally, the scheme posseses excellent scalability on massively parallel computers. © 2013 Elsevier Ltd.

Aerosol effects on UV radiation

International Nuclear Information System (INIS)

Koepke, P.; Reuder, J.; Schwander, H.

2000-01-01

The reduction of erythemally weighted UV-irradiance (given as UV index, UVI) due to aerosols is analyzed by variation of the tropospheric particles in a wide, but realistic range. Varied are amount and composition of the particles and relative humidity and thickness of the mixing layer. The reduction of UVI increases with aerosol optical depth and the UV change is around 10% for a change aerosol optical depth from 0.25 to 0.1 and 0.4 respectively. Since both aerosol absorption and scattering are of relevance, the aerosol effect depends besides total aerosol amount on relative amount of soot and on relative humidity

NATO Workshop on Soot in Combustion Systems

CERN Document Server

Prado, G

1983-01-01

Our interest in Mulhouse for carbon black and soot began some 30 years ago when J.B. Donnet developed the concept of surface chemistry of carbon and its involvement in interactions with gas, liquid and solid phases. In the late sixties, we began to study soot formation in pyrolytic systems and later on in flames. The idea of organ1z1ng a meeting on soot formation originated some four or five years ago, through discussions among Professor J.B. Howard, Dr. A. D'Alessio and ourselves. At that time the scientific community was becoming aware of the necessity to strictly control soot formation and emission. Being involved in the study of surface properties of carbon black as well as of formation of soot, we realized that the combustion community was not always fully aware of the progress made by the physical-chemists on carbon black. Reciprocally, the carbon specialists were often ignoring the research carried out on soot in flames. One objective of this workshop was to stimulate discussions between these two scie...

The immersion freezing behavior of size-segregated soot and kaolinite particles

Science.gov (United States)

Hartmann, S.; Augustin, S.; Clauss, T.; Niedermeier, D.; Raddatz, M.; Wex, H.; Shaw, R. A.; Stratmann, F.

2011-12-01

Heterogeneous ice nucleation plays a crucial role for ice formation in mixed-phase and cirrus clouds and has an important impact on precipitation formation, global radiation balances, and therefore Earth's climate (Cantrell and Heymsfield, 2005). Mineral dust and soot particles are found to be a major component of ice crystal residues (e.g., Pratt et al., 2009) so these substances are potential sources of atmospheric ice nuclei (IN). Experimental studies investigating the immersion freezing behavior of size-segregated soot and kaolinite particles conducted at the Leipzig Aerosol Cloud Interaction Simulator (LACIS) are presented. In our measurements only one aerosol particle is immersed in an air suspended water droplet which can trigger ice nucleation. The method facilitates very precise examinations with respect to temperature, ice nucleation time and ice nucleus size. Considering laboratory studies, the picture of the IN ability of soot particles is quite heterogeneous. Our studies show that submicron flame, spark soot particles and optionally coated with sulfuric acid to simulate chemically aging do not act as IN at temperatures higher than homogeneous freezing taking place. Therefore soot particles might not be an important source of IN for immersion freezing in the atmosphere. In contrast, kaolinite being representative for natural mineral dust with a well known composition and structure is found to be very active in forming ice for all freezing modes (e.g., Mason and Maybank, 1958). Analyzing the immersion freezing behavior of different sized kaolinite particles (300, 500 and 700 nm in diameter) the size effect was clearly observed, i.e. the ice fraction (number of frozen droplets per total number) scales with particle surface, i.e. the larger the ice nucleus surface the higher the ice fraction. The slope of the logarithm of the ice fraction as function of temperature is similar for all particle sizes investigated and fits very well with the results of L�

NAA of an iridium tracer to determine soot exposure of students commuting on Baltimore`s buses

Energy Technology Data Exchange (ETDEWEB)

Ondov, J.M.; Wu, C.C.; Lin, Zhibo; Kidwell, C.B. [Univ. of Maryland, College Park, MD (United States)

1997-12-01

Epidemiologic studies suggest that short-term increases in indices of particulate air pollution are associated with increased mortality and morbidity from respiratory and cardiovascular diseases. An important component of urban aerosol, diesel soot, is a known respiratory irritant and contains mutagenic and carcinogenic organic compounds. In the United States, motor vehicles are thought to be the largest single source of atmospheric soot and account for {approximately}36% of the annual anthropogenic emission of toxic polynuclear aromatic hydrocarbons (PAH). Much of the motor-vehicle-derived PAH originates from diesel-powered vehicles because their PAH emissions are up to 50-fold greater than those from gasoline engines. In Baltimore, city high school students take public buses to school and, often, must stand at bus stops while many diesel buses pass or stop before their own buses arrive. To estimate student exposures to soot emitted from public diesel buses (MTA) during commutes to city high schools, the Baltimore municipal fuel supply was tagged with an iridium tracer, and exposure was monitored during commutes with personal aerosol monitors as a part of the Baltimore Environmental Justice Project.

In-Situ Measurements of Aerosol Optical Properties using New Cavity Ring-Down and Photoacoustics Instruments and Comparison with more Traditional Techniques

Science.gov (United States)

Strawa, A. W.; Arnott, P.; Covert, D.; Elleman, R.; Ferrare, R.; Hallar, A. G.; Jonsson, H.; Kirchstetter, T. W.; Luu, A. P.; Ogren, J.

2004-01-01

Carbonaceous species (BC and OC) are responsible for most of the absorption associated with aerosol particles. The amount of radiant energy an aerosol absorbs has profound effects on climate and air quality. It is ironic that aerosol absorption coefficient is one of the most difficult aerosol properties to measure. A new cavity ring-down (CRD) instrument, called Cadenza (NASA-ARC), measures the aerosol extinction coefficient for 675 nm and 1550 nm light, and simultaneously measures the scattering coefficient at 675 nm. Absorption coefficient is obtained from the difference of measured extinction and scattering within the instrument. Aerosol absorption coefficient is also measured by a photoacoustic (PA) instrument (DRI) that was operated on an aircraft for the first time during the DOE Aerosol Intensive Operating Period (IOP). This paper will report on measurements made with this new instrument and other in-situ instruments during two field recent field studies. The first field study was an airborne cam;oaign, the DOE Aerosol Intensive Operating Period flown in May, 2003 over northern Oklahoma. One of the main purposes of the IOP was to assess our ability to measure extinction and absorption coefficient in situ. This paper compares measurements of these aerosol optical properties made by the CRD, PA, nephelometer, and Particle Soot Absorption Photometer (PSAP) aboard the CIRPAS Twin-Otter. During the IOP, several significant aerosol layers were sampled aloft. These layers are identified in the remote (AATS-14) as well as in situ measurements. Extinction profiles measured by Cadenza are compared to those derived from the Ames Airborne Tracking Sunphotometer (AATS-14, NASA-ARC). The regional radiative impact of these layers is assessed by using the measured aerosol optical properties in a radiative transfer model. The second study was conducted in the Caldecott Tunnel, a heavily-used tunnel located north of San Francisco, Ca. The aerosol sampled in this study was

Photoacoustic Soot Spectrometer (PASS) Instrument Handbook

Energy Technology Data Exchange (ETDEWEB)

Dubey, M [Los Alamos National Laboratory; Springston, S [Brookhaven National Laboratory; Koontz, A [Pacific Northwest National Laboratory; Aiken, A [Los Alamos National Laboratory

2013-01-17

The photoacoustic soot spectrometer (PASS) measures light absorption by aerosol particles. As the particles pass through a laser beam, the absorbed energy heats the particles and in turn the surrounding air, which sets off a pressure wave that can be detected by a microphone. The PASS instruments deployed by ARM can also simultaneously measure the scattered laser light at three wavelengths and therefore provide a direct measure of the single-scattering albedo. The Operator Manual for the PASS-3100 is included here with the permission of Droplet Measurement Technologies, the instrument’s manufacturer.

Properties of Arctic Aerosol Particles and Residuals of Warm Clouds: Cloud Activation Efficiency and the Aerosol Indirect Effect

Science.gov (United States)

Zelenyuk, A.; Imre, D. G.; Leaitch, R.; Ovchinnikov, M.; Liu, P.; Macdonald, A.; Strapp, W.; Ghan, S. J.; Earle, M. E.

2012-12-01

Single particle mass spectrometer, SPLAT II, was used to characterize the size, composition, number concentration, density, and shape of individual Arctic spring aerosol. Background particles, particles above and below the cloud, cloud droplet residuals, and interstitial particles were characterized with goal to identify the properties that separate cloud condensation nuclei (CCN) from background aerosol particles. The analysis offers a comparison between warm clouds formed on clean and polluted days, with clean days having maximum particle concentrations (Na) lower than ~250 cm-3, as compared with polluted days, in which maximum concentration was tenfold higher. On clean days, particles were composed of organics, organics mixed with sulfates, biomass burning (BB), sea salt (SS), and few soot and dust particles. On polluted days, BB, organics associated with BB, and their mixtures with sulfate dominated particle compositions. Based on the measured compositions and size distributions of cloud droplet residuals, background aerosols, and interstitial particles, we conclude that these three particle types had virtually the same compositions, which means that cloud activation probabilities were surprisingly nearly composition independent. Moreover, these conclusions hold in cases in which less than 20% or more than 90% of background particles got activated. We concluded that for the warm clouds interrogated in this study particle size played a more important factor on aerosol CCN activity. Comparative analysis of all studied clouds reveals that aerosol activation efficiency strongly depends on the aerosol concentrations, such that at Na <200 cm-3, nearly all particles activate, and at higher concentrations the activation efficiency is lower. For example, when Na was greater than 1500 cm-3, less than ~30% of particles activated. The data suggest that as the number of nucleated droplets increases, condensation on existing droplets effectively competes with particle

Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

Science.gov (United States)

Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

2014-12-01

Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could

Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

Energy Technology Data Exchange (ETDEWEB)

Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

2007-09-30

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

Biomass burning aerosol over the Amazon during SAMBBA: impact of chemical composition on radiative properties

Science.gov (United States)

Morgan, William; Allan, James; Flynn, Michael; Darbyshire, Eoghan; Hodgson, Amy; Liu, Dantong; O'shea, Sebastian; Bauguitte, Stephane; Szpek, Kate; Langridge, Justin; Johnson, Ben; Haywood, Jim; Longo, Karla; Artaxo, Paulo; Coe, Hugh

2014-05-01

Biomass burning represents one of the largest sources of particulate matter to the atmosphere, resulting in a significant perturbation to the Earth's radiative balance coupled with serious impacts on public health. Globally, biomass burning aerosols are thought to exert a small warming effect but with the uncertainty being 4 times greater than the central estimate. On regional scales, the impact is substantially greater, particularly in areas such as the Amazon Basin where large, intense and frequent burning occurs on an annual basis for several months. Absorption by atmospheric aerosols is underestimated by models over South America, which points to significant uncertainties relating to Black Carbon (BC) aerosol properties. Initial results from the South American Biomass Burning Analysis (SAMBBA) field experiment, which took place during September and October 2012 over Brazil on-board the UK Facility for Airborne Atmospheric Measurement (FAAM) BAe-146 research aircraft, are presented here. Aerosol chemical composition was measured by an Aerodyne Aerosol Mass Spectrometer (AMS) and a DMT Single Particle Soot Photometer (SP2). The physical, chemical and optical properties of the aerosols across the region will be characterized in order to establish the impact of biomass burning on regional air quality, weather and climate. The aircraft sampled a range of conditions including sampling of pristine Rainforest, fresh biomass burning plumes, regional haze and elevated biomass burning layers within the free troposphere. The aircraft sampled biomass burning aerosol across the southern Amazon in the states of Rondonia and Mato Grosso, as well as in a Cerrado (Savannah-like) region in Tocantins state. This presented a range of fire conditions, both in terms of their number, intensity, vegetation-type and their combustion efficiencies. Near-source sampling of fires in Rainforest environments suggested that smouldering combustion dominated, while flaming combustion dominated

Effect of strain rate on sooting limits in counterflow diffusion flames of gaseous hydrocarbon fuels: Sooting temperature index and sooting sensitivity index

KAUST Repository

Wang, Yu

2014-05-01

The effect of the strain rate on the sooting limits in counterflow diffusion flames was investigated in various gaseous hydrocarbon fuels by varying the nitrogen dilution in the fuel and oxidizer streams. The sooting limit was defined as the critical fuel and oxygen mole fraction at which soot started to appear in the elastic light scattering signal. The sooting region for normal alkane fuels at a specified strain rate, in terms of the fuel and oxygen mole fraction, expanded as the number of carbon atoms increased. The alkene fuels (ethylene, propene) tested had a higher propensity for sooting as compared with alkane fuels with the same carbon numbers (ethane, propane). Branched iso-butane had a higher propensity for sooting than did n-butane. An increase in the strain rate reduced the tendency for sooting in all the fuels tested. The sensitivity of the sooting limit to the strain rate was more pronounced for less sooting fuels. When plotted in terms of calculated flame temperature, the critical oxygen mole fraction exhibited an Arrhenius form under sooting limit conditions, which can be utilized to significantly reduce the effort required to determine sooting limits at different strain rates. We found that the limiting temperatures of soot formation flames are viable sooting metrics for quantitatively rating the sooting tendency of various fuels, based on comparisons with threshold soot index and normalized smoke point data. We also introduce a sooting temperature index and a sooting sensitivity index, two quantitative measures to describe sooting propensity and its dependence on strain rate. © 2013 The Combustion Institute.

Steady State Investigations of DPF Soot Burn Rates and DPF Modeling

DEFF Research Database (Denmark)

Cordtz, Rasmus Lage; Ivarsson, Anders; Schramm, Jesper

2011-01-01

and soot mass concentrations are used as model boundary conditions. An in-house developed raw exhaust gas sampling technique is used to measure the soot concentration upstream the DPF which is also needed to find the DPF soot burn rate. The soot concentration is measured basically by filtering the soot...... characteristics are used to fit model constants of soot and filter properties. Measured DPF gas conversions and soot burn rates are used to fit model activation energies of four DPF regeneration reactions using O2 and NO2 as reactants. Modeled DPF pressure drops and soot burn rates are compared to the steady...... state DPF experiments in the temperature range between 260 and 480 °C. The model widely reproduces the experimental results. Especially the exponential soot burn rate versus temperature is accurately reproduced by the model....

The Effect of Aerosol Hygroscopicity and Volatility on Aerosol Optical Properties During Southern Oxidant and Aerosol Study

Science.gov (United States)

Khlystov, A.; Grieshop, A. P.; Saha, P.; Subramanian, R.

2014-12-01

Secondary organic aerosol (SOA) from biogenic sources can influence optical properties of ambient aerosol by altering its hygroscopicity and contributing to light absorption directly via formation of brown carbon and indirectly by enhancing light absorption by black carbon ("lensing effect"). The magnitude of these effects remains highly uncertain. A set of state-of-the-art instruments was deployed at the SEARCH site near Centerville, AL during the Southern Oxidant and Aerosol Study (SOAS) campaign in summer 2013 to measure the effect of relative humidity and temperature on aerosol size distribution, composition and optical properties. Light scattering and absorption by temperature- and humidity-conditioned aerosols was measured using three photo-acoustic extinctiometers (PAX) at three wavelengths (405 nm, 532 nm, and 870 nm). The sample-conditioning system provided measurements at ambient RH, 10%RH ("dry"), 85%RH ("wet"), and 200 C ("TD"). In parallel to these measurements, a long residence time temperature-stepping thermodenuder (TD) and a variable residence time constant temperature TD in combination with three SMPS systems and an Aerosol Chemical Speciation Monitor (ACSM) were used to assess aerosol volatility and kinetics of aerosol evaporation. We will present results of the on-going analysis of the collected data set. We will show that both temperature and relative humidity have a strong effect on aerosol optical properties. SOA appears to increase aerosol light absorption by about 10%. TD measurements suggest that aerosol equilibrated fairly quickly, within 2 s. Evaporation varied substantially with ambient aerosol loading and composition and meteorology.

AIP1OGREN: Aerosol Observing Station Intensive Properties Value-Added Product

Energy Technology Data Exchange (ETDEWEB)

Koontz, Annette [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Flynn, Connor [Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

2017-09-15

The aip1ogren value-added product (VAP) computes several aerosol intensive properties. It requires as input calibrated, corrected, aerosol extensive properties (scattering and absorption coefficients, primarily) from the Aerosol Observing Station (AOS). Aerosol extensive properties depend on both the nature of the aerosol and the amount of the aerosol. We compute several properties as relationships between the various extensive properties. These intensive properties are independent of aerosol amount and instead relate to intrinsic properties of the aerosol itself. Along with the original extensive properties we report aerosol single-scattering albedo, hemispheric backscatter fraction, asymmetry parameter, and Ångström exponent for scattering and absorption with one-minute averaging. An hourly averaged file is produced from the 1-minute files that includes all extensive and intensive properties as well as submicron scattering and submicron absorption fractions. Finally, in both the minutely and hourly files the aerosol radiative forcing efficiency is provided.

Correlations between Optical, Chemical and Physical Properties ofBiomass Burn Aerosols

Energy Technology Data Exchange (ETDEWEB)

Hopkins, Rebecca J.; Lewis, K.; Desyaterik, Yury; Wang, Z.; Tivanski, Alexei V.; Arnott, W.P.; Laskin, Alexander; Gilles, M.K.

2008-01-29

Aerosols generated from burning different plant fuels were characterized to determine relationships between chemical, optical and physical properties. Single scattering albedo ({omega}) and Angstrom absorption coefficients ({alpha}{sub ap}) were measured using a photoacoustic technique combined with a reciprocal nephelometer. Carbon-to-oxygen atomic ratios, sp{sup 2} hybridization, elemental composition and morphology of individual particles were measured using scanning transmission X-ray microscopy coupled with near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) and scanning electron microscopy with energy dispersion of X-rays (SEM/EDX). Particles were grouped into three categories based on sp2 hybridization and chemical composition. Measured {omega} (0.4-1.0 at 405 nm) and {alpha}{sub ap} (1.0-3.5) values displayed a fuel dependence. The category with sp{sup 2} hybridization >80% had values of {omega} (<0.5) and {alpha}{sub ap} ({approx}1.25) characteristic of light absorbing soot. Other categories with lower sp2 hybridization (20 to 60%) exhibited higher {omega} (>0.8) and {alpha}{sub ap} (1.0 to 3.5) values, indicating increased absorption spectral selectivity.

Infrared remote sensing of atmospheric aerosols; Apports du sondage infrarouge a l'etude des aerosols atmospheriques

Energy Technology Data Exchange (ETDEWEB)

Pierangelo, C

2005-09-15

The 2001 report from the Intergovernmental Panel on Climate Change emphasized the very low level of understanding of atmospheric aerosol effects on climate. These particles originate either from natural sources (dust, volcanic aerosols...) or from anthropogenic sources (sulfates, soot...). They are one of the main sources of uncertainty on climate change, partly because they show a very high spatio-temporal variability. Observation from space, being global and quasi-continuous, is therefore a first importance tool for aerosol studies. Remote sensing in the visible domain has been widely used to obtain a better characterization of these particles and their effect on solar radiation. On the opposite, remote sensing of aerosols in the infrared domain still remains marginal. Yet, not only the knowledge of the effect of aerosols on terrestrial radiation is needed for the evaluation of their total radiative forcing, but also infrared remote sensing provides a way to retrieve other aerosol characteristics (observations are possible at night and day, over land and sea). In this PhD dissertation, we show that aerosol optical depth, altitude and size can be retrieved from infrared sounder observations. We first study the sensitivity of aerosol optical properties to their micro-physical properties, we then develop a radiative transfer code for scattering medium adapted to the very high spectral resolution of the new generation sounder NASA-Aqua/AIRS, and we finally focus on the inverse problem. The applications shown here deal with Pinatubo stratospheric volcanic aerosol, observed with NOAA/HIRS, and with the building of an 8 year climatology of dust over sea and land from this sounder. Finally, from AIRS observations, we retrieve the optical depth at 10 {mu}m, the average altitude and the coarse mode effective radius of mineral dust over sea. (author)

Soot Formation in Freely-Propagating Laminar Premixed Flames

Science.gov (United States)

Lin, K.-C.; Hassan, M. I.; Faeth, G. M.

1997-01-01

Soot formation within hydrocarbon-fueled flames is an important unresolved problem of combustion science. Thus, the present study is considering soot formation in freely-propagating laminar premixed flames, exploiting the microgravity environment to simplify measurements at the high-pressure conditions of interest for many practical applications. The findings of the investigation are relevant to reducing emissions of soot and continuum radiation from combustion processes, to improving terrestrial and spacecraft fire safety, and to developing methods of computational combustion, among others. Laminar premixed flames are attractive for studying soot formation because they are simple one-dimensional flows that are computationally tractable for detailed numerical simulations. Nevertheless, studying soot-containing burner-stabilized laminar premixed flames is problematical: spatial resolution and residence times are limited at the pressures of interest for practical applications, flame structure is sensitive to minor burner construction details so that experimental reproducibility is not very good, consistent burner behavior over the lengthy test programs needed to measure soot formation properties is hard to achieve, and burners have poor durability. Fortunately, many of these problems are mitigated for soot-containing, freely-propagating laminar premixed flames. The present investigation seeks to extend work in this laboratory for various soot processes in flames by observing soot formation in freely-propagating laminar premixed flames. Measurements are being made at both Normal Gravity (NG) and MicroGravity (MG), using a short-drop free-fall facility to provide MG conditions.

Physical and chemical characterization of urban winter-time aerosols by mobile measurements in Helsinki, Finland

Science.gov (United States)

Pirjola, Liisa; Niemi, Jarkko V.; Saarikoski, Sanna; Aurela, Minna; Enroth, Joonas; Carbone, Samara; Saarnio, Karri; Kuuluvainen, Heino; Kousa, Anu; Rönkkö, Topi; Hillamo, Risto

2017-06-01

A two-week measurement campaign by a mobile laboratory van was performed in urban environments in the Helsinki metropolitan area, Finland, in winter 2012, to obtain a comprehensive view on aerosol properties and sources. The abundances and physico-chemical properties of particles varied strongly in time and space, depending on the main sources of aerosols. Four major types of winter aerosol were recognized: 1) clean background aerosol with low particle number (Ntot) and lung deposited surface area (LDSA) concentrations due to marine air flows from the Atlantic Ocean; 2) long-range transported (LRT) pollution aerosol due to air flows from eastern Europe where the particles were characterized by the high contribution of oxygenated organic aerosol (OOA) and inorganic species, particularly sulphate, but low BC contribution, and their size distribution possessed an additional accumulation mode; 3) fresh smoke plumes from residential wood combustion in suburban small houses, these particles were characterized by high biomass burning organic aerosol (BBOA) and black carbon (BC) concentrations; and 4) fresh emissions from traffic while driving on busy streets in the city centre and on the highways during morning rush hours. This aerosol was characterized by high concentration of Ntot, LDSA, small particles in the nucleation mode, as well as high hydrocarbon-like organic aerosol (HOA) and BC concentrations. In general, secondary components (OOA, NO3, NH4, and SO4) dominated the PM1 chemical composition during the LRT episode accounting for 70-80% of the PM1 mass, whereas fresh primary emissions (BC, HOA and BBOA) dominated the local traffic and wood burning emissions. The major individual particle types observed with electron microscopy analysis (TEM/EDX) were mainly related to residential wood combustion (K/S/C-rich, soot, other C-rich particles), traffic (soot, Si/Al-rich, Fe-rich), heavy fuel oil combustion in heat plants or ships (S with V-Ni-Fe), LRT pollutants (S

Modification of Local Urban Aerosol Properties by Long-Range Transport of Biomass Burning Aerosol

Directory of Open Access Journals (Sweden)

Iwona S. Stachlewska

2018-03-01

Full Text Available During August 2016, a quasi-stationary high-pressure system spreading over Central and North-Eastern Europe, caused weather conditions that allowed for 24/7 observations of aerosol optical properties by using a complex multi-wavelength PollyXT lidar system with Raman, polarization and water vapour capabilities, based at the European Aerosol Research Lidar Network (EARLINET network urban site in Warsaw, Poland. During 24–30 August 2016, the lidar-derived products (boundary layer height, aerosol optical depth, Ångström exponent, lidar ratio, depolarization ratio were analysed in terms of air mass transport (HYSPLIT model, aerosol load (CAMS data and type (NAAPS model and confronted with active and passive remote sensing at the ground level (PolandAOD, AERONET, WIOS-AQ networks and aboard satellites (SEVIRI, MODIS, CATS sensors. Optical properties for less than a day-old fresh biomass burning aerosol, advected into Warsaw’s boundary layer from over Ukraine, were compared with the properties of long-range transported 3–5 day-old aged biomass burning aerosol detected in the free troposphere over Warsaw. Analyses of temporal changes of aerosol properties within the boundary layer, revealed an increase of aerosol optical depth and Ångström exponent accompanied by an increase of surface PM10 and PM2.5. Intrusions of advected biomass burning particles into the urban boundary layer seem to affect not only the optical properties observed but also the top height of the boundary layer, by moderating its increase.

Morphological transformation of soot: investigation of microphysical processes during the condensation of sulphuric acid and limonene ozonolysis products vapours

Science.gov (United States)

Pathak, R. K. P.; Pei, X.; Hallquist, M.; Pagels, J. H.

2017-12-01

Morphological transformation of soot particle by condensation of low volatility materials on it is a dominant atmospheric process with serious implications for its optical and hygroscopic properties, and atmospheric lifetime. In this study, the morphological transformation of soot agglomerate under the influence of condensation of vapours of sulphuric acid, and/or limonene ozonolysis products were investigated systematically using a Differential Mobility Analyser-Aerosol Particle Mass Analyser (DMA-APM) and the Tandem DMA techniques integrated with a laminar flow-tube system. We discovered that the morphology transformation of soot in general was a sequence of two-step process, i.e. (i) filling of void space within soot agglomerate; (ii) growth of particle diameter. These two steps followed and complimented each other. In the very beginning the filling was the dominant process followed by growth until it led to the accumulation of enough material that in turn exerted surface forces that eventually facilitated the further filling. The filling of void space was constrained by the initial morphology of fresh soot and the nature and amount of the material condensed. This process continued in several sequential steps until all void space within the soot agglomerate was filled completely and then growth of a spherical particle continued as long as mass was condensed on it. In this study, we developed a framework to quantify the microphysical transformation of soot upon the condensation of various materials. The framework utilized experimental data and hypothesis of ideal sphere growth and filling of voids to quantify the distribution of condensed materials in these two processes complimenting each other. Using this framework, we have quantified the percentage of material that went into processes of particle growth and void filling at each step. Using the same framework, we further estimated the fraction of internal voids and open voids and used this information to derive

Study on the propagation properties of laser in aerosol based on Monte Carlo simulation

Science.gov (United States)

Leng, Kun; Wu, Wenyuan; Zhang, Xi; Gong, Yanchun; Yang, Yuntao

2018-02-01

When laser propagate in the atmosphere, due to aerosol scattering and absorption, laser energy will continue to decline, affecting the effectiveness of the laser effect. Based on the Monte Carlo method, the relationship between the photon spatial energy distributions of the laser wavelengths of 10.6μm in marine, sand-type, water-soluble and soot aerosols ,and the propagation distance, visibility and the divergence angle were studied. The results show that for 10.6μm laser, the maximum number of attenuation of photons arriving at the receiving plane is sand-type aerosol, the minimal attenuation is water soluble aerosol; as the propagation distance increases, the number of photons arriving at the receiving plane decreases; as the visibility increases, the number of photons arriving at the receiving plane increases rapidly and then stabilizes; in the above cases, the photon energy distribution does not deviated from the Gaussian distribution; as the divergence angle increases, the number of photons arriving at the receiving plane is almost unchanged, but the photon energy distribution gradually deviates from the Gaussian distribution.

Infrared remote sensing of atmospheric aerosols; Apports du sondage infrarouge a l'etude des aerosols atmospheriques

Energy Technology Data Exchange (ETDEWEB)

Pierangelo, C.

2005-09-15

The 2001 report from the Intergovernmental Panel on Climate Change emphasized the very low level of understanding of atmospheric aerosol effects on climate. These particles originate either from natural sources (dust, volcanic aerosols...) or from anthropogenic sources (sulfates, soot...). They are one of the main sources of uncertainty on climate change, partly because they show a very high spatio-temporal variability. Observation from space, being global and quasi-continuous, is therefore a first importance tool for aerosol studies. Remote sensing in the visible domain has been widely used to obtain a better characterization of these particles and their effect on solar radiation. On the opposite, remote sensing of aerosols in the infrared domain still remains marginal. Yet, not only the knowledge of the effect of aerosols on terrestrial radiation is needed for the evaluation of their total radiative forcing, but also infrared remote sensing provides a way to retrieve other aerosol characteristics (observations are possible at night and day, over land and sea). In this PhD dissertation, we show that aerosol optical depth, altitude and size can be retrieved from infrared sounder observations. We first study the sensitivity of aerosol optical properties to their micro-physical properties, we then develop a radiative transfer code for scattering medium adapted to the very high spectral resolution of the new generation sounder NASA-Aqua/AIRS, and we finally focus on the inverse problem. The applications shown here deal with Pinatubo stratospheric volcanic aerosol, observed with NOAA/HIRS, and with the building of an 8 year climatology of dust over sea and land from this sounder. Finally, from AIRS observations, we retrieve the optical depth at 10 {mu}m, the average altitude and the coarse mode effective radius of mineral dust over sea. (author)

Effect of secondary organic aerosol coating thickness on the real-time detection and characterization of biomass-burning soot by two particle mass spectrometers

Directory of Open Access Journals (Sweden)

A. T. Ahern

2016-12-01

Full Text Available Biomass burning is a large source of light-absorbing refractory black carbon (rBC particles with a wide range of morphologies and sizes. The net radiative forcing from these particles is strongly dependent on the amount and composition of non-light-absorbing material internally mixed with the rBC and on the morphology of the mixed particles. Understanding how the mixing state and morphology of biomass-burning aerosol evolves in the atmosphere is critical for constraining the influence of these particles on radiative forcing and climate. We investigated the response of two commercial laser-based particle mass spectrometers, the vacuum ultraviolet (VUV ablation LAAPTOF and the IR vaporization SP-AMS, to monodisperse biomass-burning particles as we sequentially coated the particles with secondary organic aerosol (SOA from α-pinene ozonolysis. We studied three mobility-selected soot core sizes, each with a number of successively thicker coatings of SOA applied. Using IR laser vaporization, the SP-AMS had different changes in sensitivity to rBC compared to potassium as a function of applied SOA coatings. We show that this is due to different effective beam widths for the IR laser vaporization region of potassium versus black carbon. The SP-AMS's sensitivity to black carbon (BC mass was not observed to plateau following successive SOA coatings, despite achieving high OA : BC mass ratios greater than 9. We also measured the ion fragmentation pattern of biomass-burning rBC and found it changed only slightly with increasing SOA mass. The average organic matter ion signal measured by the LAAPTOF demonstrated a positive correlation with the condensed SOA mass on individual particles, despite the inhomogeneity of the particle core compositions. This demonstrates that the LAAPTOF can obtain quantitative mass measurements of aged soot-particle composition from realistic biomass-burning particles with complex morphologies and composition.

Determination of atmospheric aerosol properties over land using satellite measurements

NARCIS (Netherlands)

Kokhanovsky, A.A.; Leeuw, G. de

2009-01-01

Mostly, aerosol properties are poorly understood because the aerosol properties are very sparse. The first workshop on the determination of atmospheric aerosol properties over land using satellite measurements is convened in Bremen, Germany. In this workshop, the topics of discussions included a

The Ice Nucleation Activity of Surface Modified Soot

Science.gov (United States)

Häusler, Thomas; Witek, Lorenz; Felgitsch, Laura; Hitzenberger, Regina; Grothe, Hinrich

2017-04-01

The ice nucleation efficiency of many important atmospheric particles remains poorly understood. Since soot is ubiquitous in the Earth's troposphere, they might have the potential to significantly impact the Earth's climate (Finlayson-Pitts and Pitts, 2000; Seinfeld and Pandis, 1998). Here we present the ice nucleation activity (INA) in immersion freezing mode of different types of soot. Therefor a CAST (combustion aerosol standard) generator was used to produce different kinds of soot samples. The CAST generator combusts a propane-air-mixture and deposits thereby produced soot on a polyvinyl fluoride filter. By varying the propane to air ratio, the amount of organic portion of the soot can be varied from black carbon (BC) with no organic content to brown carbon (BrC) with high organic content. To investigate the impact of functional sites of ice nuclei (IN), the soot samples were exposed to NO2 gas for a certain amount of time (30 to 360 minutes) to chemically modify the surface. Immersion freezing experiments were carried out in a unique reaction gadget. In this device a water-in-oil suspension (with the soot suspended in the aqueous phase) was cooled till the freezing point and was observed through a microscope (Pummer et al., 2012; Zolles et al., 2015) It was found that neither modified nor unmodified BC shows INA. On the contrary, unmodified BrC shows an INA at -32˚ C, which can be increased up to -20˚ C. The INA of BrC depends on the duration of NO2- exposure. To clarify the characteristics of the surface modifications, surface sensitive analysis like infrared spectroscopy and X-ray photoelectron spectroscopy were carried out. Finlayson-Pitts, B. J. and Pitts, J. N. J.: Chemistry of the Upper and Lower Atmosphere, Elsevier, New York, 2000. Pummer, B. G., Bauer, H., Bernardi, J., Bleicher, S., and Grothe, H.: Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Atmos Chem Phys, 12, 2541-2550, 2012. Seinfeld, J

Chemical, microphysical and optical properties of the aerosols during foggy and nonfoggy day over a typical location in Indo-Gangetic Plain

Science.gov (United States)

Kaul, D. S.; Tripathi, S. N.; Gupta, T.

2012-04-01

An extensive experimental measurement was carried out from January 16, 2010 to February 20, 2010 at Kanpur to study the chemical, microphysical and optical properties of the aerosols. A Micro-Pulse Lidar Network (MPLNET), a part of National Aeronautic Space Administration (NASA), was used for identification of fog duration. PM1 samples and fogwater were collected to examine the organic and inorganic species of aerosol and fogwater. Organic Carbon (OC), Elemental Carbon (EC) and water soluble organic carbon analysis were carried out by an EC-OC analyzer and a TOC analyzer, respectively. Trace gases and solar flux measurement were carried out by gas analyzers and a pyranometer (a part of NASA Aeronet), respectively, to identify the photo-chemical activity. Meteorological data were measured by atmospheric weather station. The microphysical properties such as aerosol size distribution were measured using a scanning mobility particle sizer (SMPS). Optical properties were measured by a photo-acoustic soot spectrometer (PASS). Organic and inorganic species are processed by fog droplets such as production of secondary organic aerosol through aqueous mechanism (Kaul et al., 2011) and scavenging of various water soluble species. The concentrations of almost all the ionic species and organic carbon were higher in aerosols during foggy day. Presence of numerous ionic species and organic carbon in the fogwater indicates their wet scavenging and removal from the atmosphere by the fog droplets. Most of the aerosol is composed of inorganic component, ~80% during foggy day and ~85.5 % during clear day. Biomass burning contribution to PM1 mass concentration was considerably higher during clear days and lower during foggy days; lower concentration during foggy day could be due to wet scavenging of biomass generated aerosols. The study average higher number concentration of aerosol during foggy day during late evening and overnight was due to lower boundary layer height and subsequent

Aromatics Oxidation and Soot Formation in Flames

Energy Technology Data Exchange (ETDEWEB)

Howard, J. B.; Richter, H.

2005-03-29

This project is concerned with the kinetics and mechanisms of aromatics oxidation and the growth process to polycyclic aromatic hydrocarbons (PAH) of increasing size, soot and fullerenes formation in flames. The overall objective of the experimental aromatics oxidation work is to extend the set of available data by measuring concentration profiles for decomposition intermediates such as phenyl, cyclopentadienyl, phenoxy or indenyl radicals which could not be measured with molecular-beam mass spectrometry to permit further refinement and testing of benzene oxidation mechanisms. The focus includes PAH radicals which are thought to play a major role in the soot formation process while their concentrations are in many cases too low to permit measurement with conventional mass spectrometry. The radical species measurements are used in critical testing and improvement of a kinetic model describing benzene oxidation and PAH growth. Thermodynamic property data of selected species are determined computationally, for instance using density functional theory (DFT). Potential energy surfaces are explored in order to identify additional reaction pathways. The ultimate goal is to understand the conversion of high molecular weight compounds to nascent soot particles, to assess the roles of planar and curved PAH and relationships between soot and fullerenes formation. The specific aims are to characterize both the high molecular weight compounds involved in the nucleation of soot particles and the structure of soot including internal nanoscale features indicative of contributions of planar and/or curved PAH to particle inception.

Developing a predictive model for the chemical composition of soot nanoparticles

Energy Technology Data Exchange (ETDEWEB)

Violi, Angela [Univ. of Michigan, Ann Arbor, MI (United States); Michelsen, Hope [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Hansen, Nils [Sandia National Lab. (SNL-CA), Livermore, CA (United States); Wilson, Kevin [Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

2017-04-07

In order to provide the scientific foundation to enable technology breakthroughs in transportation fuel, it is important to develop a combustion modeling capability to optimize the operation and design of evolving fuels in advanced engines for transportation applications. The goal of this proposal is to develop a validated predictive model to describe the chemical composition of soot nanoparticles in premixed and diffusion flames. Atomistic studies in conjunction with state-of-the-art experiments are the distinguishing characteristics of this unique interdisciplinary effort. The modeling effort has been conducted at the University of Michigan by Prof. A. Violi. The experimental work has entailed a series of studies using different techniques to analyze gas-phase soot precursor chemistry and soot particle production in premixed and diffusion flames. Measurements have provided spatial distributions of polycyclic aromatic hydrocarbons and other gas-phase species and size and composition of incipient soot nanoparticles for comparison with model results. The experimental team includes Dr. N. Hansen and H. Michelsen at Sandia National Labs' Combustion Research Facility, and Dr. K. Wilson as collaborator at Lawrence Berkeley National Lab's Advanced Light Source. Our results show that the chemical and physical properties of nanoparticles affect the coagulation behavior in soot formation, and our results on an experimentally validated, predictive model for the chemical composition of soot nanoparticles will not only enhance our understanding of soot formation since but will also allow the prediction of particle size distributions under combustion conditions. These results provide a novel description of soot formation based on physical and chemical properties of the particles for use in the next generation of soot models and an enhanced capability for facilitating the design of alternative fuels and the engines they will power.

Sooting limit in counterflow diffusion flames of ethylene/propane fuels and implication to threshold soot index

KAUST Repository

Joo, Peter H.

2013-01-01

Sooting limits in counterflow diffusion flames of propane/ethylene fuels have been studied experimentally using a light scattering technique, including the effects of dilution, fuel mixing, and strain rate. The results are discussed in view of the threshold soot index (TSI). In soot-formation (SF) flames, where the flame is located on the oxidizer side of the stagnation plane, the sooting limit depends critically on fuel type and subsequently on flame temperature. The sooting limit has a non-linear dependence on the fuel-mixing ratio, which is similar to the non-linear mixing rule for TSI observed experimentally in rich premixed flames, where soot oxidation is absent for both SF and rich premixed flames. In soot-formation-oxidation (SFO) flames, where the flame is located on the fuel side, the sooting limit depends critically on flame temperature, while it is relatively independent on fuel type. This result suggests a linear mixing rule for sooting limits in SFO flames, which is similar to the TSI behavior for coflow diffusion flames. Soot oxidation takes place for both types of flames. The aerodynamic strain effect on the sooting limits has also been studied and an appreciable influence has been observed. Under sooting conditions, soot volume fraction was measured using a light extinction technique. The soot loadings in SF flames of the mixture fuels demonstrated a synergistic effect, i.e., soot production increased for certain mixture fuels as compared to the respective singlecomponent fuels. © 2012 The Combustion Institute.

On transient climate change at the Cretaceous−Paleogene boundary due to atmospheric soot injections

Science.gov (United States)

Garcia, Rolando R.; Toon, Owen B.; Conley, Andrew J.

2017-01-01

Climate simulations that consider injection into the atmosphere of 15,000 Tg of soot, the amount estimated to be present at the Cretaceous−Paleogene boundary, produce what might have been one of the largest episodes of transient climate change in Earth history. The observed soot is believed to originate from global wildfires ignited after the impact of a 10-km-diameter asteroid on the Yucatán Peninsula 66 million y ago. Following injection into the atmosphere, the soot is heated by sunlight and lofted to great heights, resulting in a worldwide soot aerosol layer that lasts several years. As a result, little or no sunlight reaches the surface for over a year, such that photosynthesis is impossible and continents and oceans cool by as much as 28 °C and 11 °C, respectively. The absorption of light by the soot heats the upper atmosphere by hundreds of degrees. These high temperatures, together with a massive injection of water, which is a source of odd-hydrogen radicals, destroy the stratospheric ozone layer, such that Earth’s surface receives high doses of UV radiation for about a year once the soot clears, five years after the impact. Temperatures remain above freezing in the oceans, coastal areas, and parts of the Tropics, but photosynthesis is severely inhibited for the first 1 y to 2 y, and freezing temperatures persist at middle latitudes for 3 y to 4 y. Refugia from these effects would have been very limited. The transient climate perturbation ends abruptly as the stratosphere cools and becomes supersaturated, causing rapid dehydration that removes all remaining soot via wet deposition. PMID:28827324

Hygroscopic properties of different aerosol types over the Atlantic and Indian Oceans

Directory of Open Access Journals (Sweden)

A. Maßling

2003-01-01

Full Text Available Hygroscopic properties of atmospheric particles were studied in the marine tropospheric boundary layer over the Atlantic and Indian Oceans during two consecutive field studies: the Aerosols99 cruise (Atlantic Ocean from 15 January to 20 February 1999, and the INDOEX cruise (Indian Ocean Experiment from 23 February to 30 March 1999. The hygroscopic properties were compared to optical and chemical properties, such as absorption, chemical inorganic composition, and mass concentration of organic and elemental carbon, to identify the influence of these parameters on hygroscopicity. During the two field studies, four types of aerosol-sampling instruments were used on board the NOAA (National Oceanic and Atmospheric Administration Research Vessel Ronald H. Brown: Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA, seven-stage cascade impactor, two-stage cascade impactor, and Particle Soot Absorption Photometer (PSAP. The HTDMA was used to determine the hygroscopic properties of atmospheric particles at initial dry sizes (Dp of 50, 150, and 250 nm and at relative humidities (RH of 30, 55, 75, and 90%. Simultaneously, a seven-stage cascade impactor of which 3 stages were in the sub-mm size range was used to determine the molar composition of the major inorganic ions such as ammonium and sulfate ions. A two-stage cascade impactor (1 in the sub-mm size range, 1 in the sup-mm size range was used to determine the mass concentration of organic and elemental carbon. The PSAP was used (at a wavelength of 565 nm to measure the light absorption coefficient of the aerosol. During the two field studies, air masses of several different origins passed the ship's cruise path. The occurrence of different air masses was classified into special time periods signifying the origin of the observed aerosol. All time periods showed a group of particles with high hygroscopic growth. The measured average hygroscopic growth factors defined by the ratio of dry and wet

Maritime Aerosol optical properties measured by ship-borne sky radiometer

Science.gov (United States)

Aoki, K.

2017-12-01

Maritime aerosols play an important role in the earth climate change. We started the measurements of aerosol optical properties since 1994 by using ship-borne sky radiometer (POM-01 MK-II and III; Prede Co. Ltd., Japan) over the ocean. We report the results of an aerosol optical properties over the ocean by using Research Vessel of the ship-borne sky radiometers. Aerosol optical properties observation were made in MR10-02 to MR16-09 onboard the R/V Mirai, JAMSTEC. The sky radiometer measure the direct and diffuse solar radiance with seven interference filters (0.315, 0.4, 0.5, 0.675, 0.87, 0.94, and 1.02 µm). Observation interval was made every five minutes by once, only in daytime under the clear sky conditions. GPS provides the position with longitude and latitude and heading direction of the vessel, and azimuth and elevation angle of the sun. The aerosol optical properties were computed using the SKYRAD.pack version 4.2. The obtained Aerosol optical properties (Aerosol optical thickness, Ångström exponent, Single scattering albedo, and etc.) and size distribution volume clearly showed spatial and temporal variability over the ocean. Aerosol optical thickness found over the near the coast (Asia and Tropical area) was high and variable. The size distribution volume have peaks at small particles at Asian coast and large particles at Tropical coast area. We provide the information, in this presentation, on the aerosol optical properties measurements with temporal and spatial variability in the Maritime Aerosol. This project is validation satellite of GCOM-C/SGLI, JAXA and other. The GCOM-C satellite scheduled to be launched in 2017 JFY.

Reservoir patterns of soot, organic particles, total carbon, soluble substances and aerosols (numbers and mass) in the droplet and interstitial phase of clouds; Reservoiraufteilung von Russ, organischen Bestandteilen, Gesamtkohlenstoff, loeslichen Substanzen und Aerosolpartikeln (Anzahl und Masse) in der Tropfen- und Zwischenraumphase von Wolken. Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Wieprecht, W.; Acker, K.; Moeller, D.; Auel, R.; Hofmeister, J.; Kalass, D.

2002-07-01

The reservoir patterns of the constitutents of representative clouds over Germany were investigated for a better characterisation of their optical, microphysical and chemical properties. One of the key points of interest was the distribution of carbonaceous aerosol particles in the droplet and interstitial phase, which was to provide information on the role of absorbing (soot or BC) and organic carbon (OC) in cloud formation. Data about the effects of potential CCN on cloud characteristics and about the changes in aerosol particles induced by cloud processes are required as input for models of the chemical and climate effects of atmospheric aerosol. [German] Ziel des Projektes war eine moeglichst umfassende experimentelle Ermittlung der Reservoiraufteilung der Inhaltsstoffe repraesentativer Wolken ueber der Bundesrepublik Deutschland, um ihre optischen, mikrophysikalischen und chemischen Eigenschaften besser zu charakterisieren. Ein besonderer Schwerpunkt des Gesamtprojekts lag auf der Bestimmung der Verteilung kohlenstoffhaltiger Aerosolpartikel auf die Tropfen- und interstitielle Phase, um Aufschluesse ueber die Rolle von absorbierendem (Russ oder BC) und organischem Kohlenstoff (OC) bei der Wolkenbildung zu erhalten. Erkenntnisse sowohl ueber die Beeinflussung potentieller CCN auf Wolkeneigenschaften als auch ueber die Veraenderung der Aerosolpartikel durch Wolkenprozesse sind erforderlich als Eingangsdaten in entsprechende Modelle, um die chemischen und klimatischen Effekte des atmosphaerischen Aerosols zu bestimmen. (orig.)

Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

Energy Technology Data Exchange (ETDEWEB)

Ogren, John A.; Sheridan, Patrick S.; Andrews, Elisabeth

2009-03-05

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models.

Diurnal Evolution of Aerosol Optical Properties and Morphology at Pico Tres Padres: A Phenomenological Analysis

Science.gov (United States)

Mazzoleni, C.; Chakrabarty, R.; Dubey, M. K.; Moosmuller, H.; Chylek, P.; Onasch, T. B.; Herndon, S.; Zavala, M.; Kolb, C.

2007-05-01

tens-of-minutes-to-hour time frame immediately following the growth of the boundary layer above the sampling site. Later in the day the single scattering albedo grew steadily to reach a maximum in the late afternoon. The SEM images show a wide variety of aerosol shapes including fractal-like chain aggregates (possibly soot), spherical particles (possibly tar balls), cylinders, and irregular non-fractal shapes. The increased afternoon single scattering albedo in the hottest part of the day qualitatively correlated with a relative increase in spherical particles that typically are not strongly light absorbing relative to fractal-like chain aggregates that are typically strongly light absorbing. These changes in optical properties and/or morphology can be explained by multiple mechanisms such as the collapse of fractal-like chain aggregates due to thermal effects and/or condensation of volatile compounds, coating by organic compounds, and photochemical secondary organic particle formation. Elemental analysis of a few individual particles yielded a relative large carbon abundance combined with smaller fractions of oxygen, silicon, metals, and other elements.

Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

Energy Technology Data Exchange (ETDEWEB)

Richard A. Ferrare; David D. Turner

2011-09-01

Project goals: (1) Use the routine surface and airborne measurements at the ARM SGP site, and the routine surface measurements at the NSA site, to continue our evaluations of model aerosol simulations; (2) Determine the degree to which the Raman lidar measurements of water vapor and aerosol scattering and extinction can be used to remotely characterize the aerosol humidification factor; (3) Use the high temporal resolution CARL data to examine how aerosol properties vary near clouds; and (4) Use the high temporal resolution CARL and Atmospheric Emitted Radiance Interferometer (AERI) data to quantify entrainment in optically thin continental cumulus clouds.

Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul [Boston College, Chestnut Hill, MA (United States)

2015-10-20

) two well-characterized source of soot particles and (b) a flow reactor for controlled OH and/or O3 oxidation of relevant gas phase species to produce well-characterized SOA particles. After formation, the aerosol particles are subjected to physical and chemical processes that simulate aerosol growth and aging. A suite of instruments in our laboratory is used to characterize the physical and chemical properties of aerosol particles before and after processing. The Time of Flight Aerosol Mass Spectrometer (ToF-AMS) together with a Scanning Mobility Particle Sizer (SMPS) measures particle mass, volume, density, composition (including black carbon content), dynamic shape factor, and fractal dimension. The–ToF-AMS was developed at ARI with Boston College participation. About 120 AMS instruments are now in service (including 5 built for DOE laboratories) performing field and laboratory studies world-wide. Other major instruments include a thermal denuder, two Differential Mobility Analyzers (DMA), a Cloud Condensation Nuclei Counter (CCN), a Thermal desorption Aerosol GC/MS (TAG) and the new Soot Particle Aerosol Mass Spectrometer (SP-AMS). Optical instrumentation required for the studies have been brought to our laboratory as part of ongoing and planned collaborative projects with colleagues from DOE, NOAA and university laboratories. Optical instruments that will be utilized include a Photoacoustic Spectrometer (PAS), a Cavity Ring Down Aerosol Extinction Spectrometer (CRD-AES), a Photo Thermal Interferometer (PTI), a new 7-wavelength Aethalometer and a Cavity Attenuated Phase Shift Extinction Monitor (CAPS). These instruments are providing aerosol absorption, extinction and scattering coefficients at a range of atmospherically relevant wavelengths. During the past two years our work has continued along the lines of our original proposal. We report on 12 completed and/or continuing projects conducted during the period 08/14 to 0814/2015. These projects are described in

Nitrogen dioxide and kerosene-flame soot calibration of photoacoustic instruments for measurement of light absorption by aerosols

International Nuclear Information System (INIS)

Arnott, W. Patrick; Moosmu''ller, Hans; Walker, John W.

2000-01-01

A nitrogen dioxide calibration method is developed to evaluate the theoretical calibration for a photoacoustic instrument used to measure light absorption by atmospheric aerosols at a laser wavelength of 532.0 nm. This method uses high concentrations of nitrogen dioxide so that both a simple extinction and the photoacoustically obtained absorption measurement may be performed simultaneously. Since Rayleigh scattering is much less than absorption for the gas, the agreement between the extinction and absorption coefficients can be used to evaluate the theoretical calibration, so that the laser gas spectra are not needed. Photoacoustic theory is developed to account for strong absorption of the laser beam power in passage through the resonator. Findings are that the photoacoustic absorption based on heat-balance theory for the instrument compares well with absorption inferred from the extinction measurement, and that both are well within values represented by published spectra of nitrogen dioxide. Photodissociation of nitrogen dioxide limits the calibration method to wavelengths longer than 398 nm. Extinction and absorption at 532 and 1047 nm were measured for kerosene-flame soot to evaluate the calibration method, and the single scattering albedo was found to be 0.31 and 0.20 at these wavelengths, respectively

Aerosol optical properties in the mega-cities Beijing and Guangzhou: Measurements and implications for regional air pollution, aerosol sources and remote sensing

Science.gov (United States)

Garland, R. M.; Yang, H.; Schmid, O.; Rose, D.; Gunthe, S. S.

2009-04-01

Aerosol optical properties were measured in two mega-city regions in China. The first site (Backgarden) was in a rural area approximately 60 km northwest of the mega-city Guangzhou in south China and was part of the "Program of Regional Integrated Experiments of Air Quality over the Pearl River Delta" intensive campaign in July 2006 (PRIDE-PRD2006). The second site (Yufa) was in a suburban area approximately 40 km south of Beijing and was part of "Campaigns of Air Quality Research in Beijing" (CAREBeijing-2006) in August 2006. Both sites were designed to measure the regional pollution of the mega-cities. The optical parameters determined with a nephelometer and photoacoustic spectrometer include absorption and scattering coefficients, single scattering albedos and Angstrom exponents at multiple wavelengths (450-700 nm). In both measurement campaigns, we observed pronounced diurnal cycles in absorption and scattering coefficients and single scattering albedo, which can be explained by boundary layer mixing effects and enhanced light absorbing carbon emissions from traffic activity during the nighttime and early morning, respectively (diesel soot from regulated truck traffic). In Beijing both the extensive and the intensive properties were highly dependent upon the origin of the air mass, which indicates that not only does the aerosol concentration change with air mass origin, but so do the chemical composition and sources. When the measured air masses originated in the north and passed over Beijing, the single scattering albedo was generally low (transported into the city from the south. The scattering and absorption coefficients measured in the outflow of the Guangzhou area during PRIDE-PRD2006 were ~2 times smaller than the southerly inflow into Beijing during CARBeijing-2006, which indicates that the sources of particulate pollution south of Beijing are even stronger than those in the Pearl River Delta. In both mega-city regions the Angstrom exponent exhibited a

The effect of aerosol on closure of the regionale short-wave radiation balance

NARCIS (Netherlands)

Henzing JS; Knap WH; Stammes P; ten Brink HM; Kos GPA; Even A; Swart DPJ; Bergwerff JP; Apituley A; NOP

2001-01-01

IPPC reports the aerosol radiative forcing per major aerosol category, like sulphate and fossil fuel derived carbon. Part of this carbon is reflective and part of the material (black carbon "soot") absorbs radiation. We find that in the Netherlands sulphate contributes some 30% to the

Development of a photoacoustic sensor system for the measurement of atmospheric soot aerosols. Final report; Weiterentwicklung und Charakterisierung des photoakustischen Russsensors. Schlussbericht

Energy Technology Data Exchange (ETDEWEB)

Kraemer, L.; Bozoki, Z.; Niessner, R.

2001-03-01

The photoacoustic soot sensor (PASS) has been optimised and characterised in this work to enable online atmospheric black carbon (BC) monitoring. The mobility of the sensor suited for outdoor measurements was already achieved by a former setup. The major technical modifications include the use of a new diode laser with an emission wavelength of 680 nm and an output power of 250 mW and the redesign of the photoacoustic resonance cell and all optical components. Additionally, most of the electronic compounds have been exchanged, e.g. function generator, microphone preamplifier, lock-in amplifier. Due to these modifications, the increase in the sensitivity of the system led to a detection limit in the order of 100 ng per m{sup 3}. The selectivity has been enhanced by the use of a magnetic valve, which enables the independent determination of particular and gaseous compounds of the sample. Cross-sensitivities to water vapor or nitrogen dioxide can be excluded by differential measurement. Any influence by other airborne atmospheric particles like scattering salt aerosols, desert dust or humic acid is negligable under atmospheric conditions as has been shown in laboratory experiments. For the determination of low atmospheric BC concentrations, the time resolution of the entire setup by employing a software controlled, automated measurement cycle equals {proportional_to}5 minutes. The PASS was tested in various field campaigns at different measurement sites to determine atmospheric BC (Munich-Grosshadern, Kleiner Feldberg) and diesel soot (AIDA, FZ Karlsruhe; diesel engine, DaimlerChrysler). (orig.)

Numerical investigation on soot particles emission in compression ignition diesel engine by using particulate mimic soot model

Directory of Open Access Journals (Sweden)

Ibrahim Fadzli

2017-01-01

Full Text Available Research via computational method, specifically by detailed-kinetic soot model offers much more advantages than the simple model as more detailed formation/oxidation process is taken into consideration, thus providing better soot mass concentration, soot size, soot number density as well as information regarding other related species. In the present computational study, investigation of in-cylinder soot concentration as well as other emissions in a single cylinder diesel engine has been conducted, using a commercial multidimensional CFD software, CONVERGE CFD. The simulation was carried out for a close-cycle combustion environment from inlet valve closing (IVC to exhaust valve opening (EVO. In this case, detailed-kinetic Particulate Mimic (PM soot model was implemented as to take benefit of the method of moment, instead of commonly implemented simple soot model. Analyses of the results are successfully plotted to demonstrate that the soot size and soot mass concentration are strongly dependent on the detailed soot formation and oxidation process rates. The calculated of soot mass concentration and average soot size at EVO provide the end value of 29.2 mg/m3 and 2.04 × 10−8 m, respectively. Besides, post-processing using EnSight shows the qualitative results of soot concentration along simulation period in the combustion chamber.

Satellite remote sensing of aerosol and cloud properties over Eurasia

Science.gov (United States)

Sogacheva, Larisa; Kolmonen, Pekka; Saponaro, Giulia; Virtanen, Timo; Rodriguez, Edith; Sundström, Anu-Maija; Atlaskina, Ksenia; de Leeuw, Gerrit

2015-04-01

Satellite remote sensing provides the spatial distribution of aerosol and cloud properties over a wide area. In our studies large data sets are used for statistical studies on aerosol and cloud interaction in an area over Fennoscandia, the Baltic Sea and adjacent regions over the European mainland. This area spans several regimes with different influences on aerosol cloud interaction such as a the transition from relative clean air over Fennoscandia to more anthropogenically polluted air further south, and the influence maritime air over the Baltic and oceanic air advected from the North Atlantic. Anthropogenic pollution occurs in several parts of the study area, and in particular near densely populated areas and megacities, but also in industrialized areas and areas with dense traffic. The aerosol in such areas is quite different from that produced over the boreal forest and has different effects on air quality and climate. Studies have been made on the effects of aerosols on air quality and on the radiation balance in China. The aim of the study is to study the effect of these different regimes on aerosol-cloud interaction using a large aerosol and cloud data set retrieved with the (Advanced) Along Track Scanning Radiometer (A)ATSR Dual View algorithm (ADV) further developed at Finnish Meteorological Institute and aerosol and cloud data provided by MODIS. Retrieval algorithms for aerosol and clouds have been developed for the (A)ATSR, consisting of a series of instruments of which we use the second and third one: ATSR-2 which flew on the ERS-2 satellite (1995-2003) and AATSR which flew on the ENVISAT satellite (2002-2012) (both from the European Space Agency, ESA). The ADV algorithm provides aerosol data on a global scale with a default resolution of 10x10km2 (L2) and an aggregate product on 1x1 degree (L3). Optional, a 1x1 km2 retrieval products is available over smaller areas for specific studies. Since for the retrieval of AOD no prior knowledge is needed on

CCN concentrations and BC warming influenced by maritime ship emitted aerosol plumes over southern Bay of Bengal.

Science.gov (United States)

Ramana, M V; Devi, Archana

2016-08-02

Significant quantities of carbon soot aerosols are emitted into pristine parts of the atmosphere by marine shipping. Soot impacts the radiative balance of the Earth-atmosphere system by absorbing solar-terrestrial radiation and modifies the microphysical properties of clouds. Here we examined the impact of black carbon (BC) on net warming during monsoon season over southern Bay-of-Bengal, using surface and satellite measurements of aerosol plumes from shipping. Shipping plumes had enhanced the BC concentrations by a factor of four around the shipping lane and exerted a strong positive influence on net warming. Compiling all the data, we show that BC atmospheric heating rates for relatively-clean and polluted-shipping corridor locations to be 0.06 and 0.16 K/day respectively within the surface layer. Emissions from maritime ships had directly heated the lower troposphere by two-and-half times and created a gradient of around 0.1 K/day on either side of the shipping corridor. Furthermore, we show that ship emitted aerosol plumes were responsible for increase in the concentration of cloud condensation nuclei (CCN) by an order of magnitude that of clean air. The effects seen here may have significant impact on the monsoonal activity over Bay-of-Bengal and implications for climate change mitigation strategies.

Soot and Spectral Radiation Modeling in ECN Spray A and in Engines

Energy Technology Data Exchange (ETDEWEB)

Haworth, Daniel C [Pennsylvania State Univ., University Park, PA (United States); Ferreyro-Fernandez, Sebastian [Pennsylvania State Univ., University Park, PA (United States); Paul, Chandan [Pennsylvania State Univ., University Park, PA (United States); Sircar, Arpan [Pennsylvania State Univ., University Park, PA (United States); Imren, Abdurrahman [Pennsylvania State Univ., University Park, PA (United States); Roy, Somesh P [Marquette University (United States); Modest, Michael F [University of California Merced (United States); Ge, Wenjun [University of California Merced (United States)

2017-04-03

The amount of soot formed in a turbulent combustion system is determined by a complex system of coupled nonlinear chemical and physical processes. Different physical subprocesses can dominate, depending on the hydrodynamic and thermochemical environments. Similarly, the relative importance of reabsorption, spectral radiation properties, and molecular gas radiation versus soot radiation varies with thermochemical conditions, and in ways that are difficult to predict for the highly nonhomogeneous in-cylinder mixtures in engines. Here it is shown that transport and mixing play relatively more important roles as rate-determining processes in soot formation at engine-relevant conditions. It is also shown that molecular gas radiation and spectral radiation properties are important for engine-relevant conditions.

Climatology of Aerosol Optical Properties in Southern Africa

Science.gov (United States)

Queface, Antonio J.; Piketh, Stuart J.; Eck, Thomas F.; Tsay, Si-Chee

2011-01-01

A thorough regionally dependent understanding of optical properties of aerosols and their spatial and temporal distribution is required before we can accurately evaluate aerosol effects in the climate system. Long term measurements of aerosol optical depth, Angstrom exponent and retrieved single scattering albedo and size distribution, were analyzed and compiled into an aerosol optical properties climatology for southern Africa. Monitoring of aerosol parameters have been made by the AERONET program since the middle of the last decade in southern Africa. This valuable information provided an opportunity for understanding how aerosols of different types influence the regional radiation budget. Two long term sites, Mongu in Zambia and Skukuza in South Africa formed the core sources of data in this study. Results show that seasonal variation of aerosol optical thicknesses at 500 nm in southern Africa are characterized by low seasonal multi-month mean values (0.11 to 0.17) from December to May, medium values (0.20 to 0.27) between June and August, and high to very high values (0.30 to 0.46) during September to November. The spatial distribution of aerosol loadings shows that the north has high magnitudes than the south in the biomass burning season and the opposite in none biomass burning season. From the present aerosol data, no long term discernable trends are observable in aerosol concentrations in this region. This study also reveals that biomass burning aerosols contribute the bulk of the aerosol loading in August-October. Therefore if biomass burning could be controlled, southern Africa will experience a significant reduction in total atmospheric aerosol loading. In addition to that, aerosol volume size distribution is characterized by low concentrations in the non biomass burning period and well balanced particle size contributions of both coarse and fine modes. In contrast high concentrations are characteristic of biomass burning period, combined with

Evaluation of a Lagrangian Soot Tracking Method for the prediction of primary soot particle size under engine-like conditions

DEFF Research Database (Denmark)

Cai Ong, Jiun; Pang, Kar Mun; Walther, Jens Honore

2018-01-01

This paper reports the implementation and evaluation of a Lagrangian soot tracking (LST) method for the modeling of soot in diesel engines. The LST model employed here has the tracking capability of a Lagrangian method and the ability to predict primary soot particle sizing. The Moss-Brookes soot...... in predicting temporal soot cloud development, mean soot diameter and primary soot size distribution is evaluated using measurements of n-heptane and n-dodecane spray combustion obtained under diesel engine-like conditions. In addition, sensitivity studies are carried out to investigate the influence of soot....... A higher rate of soot oxidation due to OH causes the soot particles to be fully oxidized downstream of the flame. In general, the LST model performs better than the Eulerian method in terms of predicting soot sizing and accessing information of individual soot particles, both of which are shortcomings...

Characterizing and Understanding Aerosol Optical Properties: CARES - Final Report

Energy Technology Data Exchange (ETDEWEB)

Cappa, Christopher D [Univ. of California, Davis, CA (United States); Atkinson, Dean B [Portland State Univ., Portland, OR (United States)

2017-12-17

The scientific focus of this study was to use ambient measurements to develop new insights into the understanding of the direct radiative forcing by atmospheric aerosol particles. The study used data collected by the PI’s and others as part of both the 2010 U.S. Department of Energy (DOE) sponsored Carbonaceous Aerosols and Radiative Effects Study (CARES), which took place in and around Sacramento, CA, and the 2012 Clean Air for London (ClearfLo) study. We focus on measurements that were made of aerosol particle optical properties, namely the wavelength-dependent light absorption, scattering and extinction. Interpretation of these optical property measurements is facilitated through consideration of complementary measurements of the aerosol particle chemical composition and size distributions. With these measurements, we addressed the following general scientific questions: 1. How does light scattering and extinction by atmospheric aerosol particles depend on particle composition, water uptake, and size? 2. To what extent is light absorption by aerosol particles enhanced through the mixing of black carbon with other particulate components? 3. What relationships exist between intensive aerosol particle optical properties, and how do these depend on particle source and photochemical aging? 4. How well do spectral deconvolution methods, which are commonly used in remote sensing, retrieve information about particle size distributions?

Black carbon's contribution to aerosol absorption optical depth over S. Korea

Science.gov (United States)

Lamb, K.; Perring, A. E.; Beyersdorf, A. J.; Anderson, B. E.; Segal-Rosenhaimer, M.; Redemann, J.; Holben, B. N.; Schwarz, J. P.

2017-12-01

Aerosol absorption optical depth (AAOD) monitored by ground-based sites (AERONET, SKYNET, etc.) is used to constrain climate radiative forcing from black carbon (BC) and other absorbing aerosols in global models, but few validation studies between in situ aerosol measurements and ground-based AAOD exist. AAOD is affected by aerosol size distributions, composition, mixing state, and morphology. Megacities provide appealing test cases for this type of study due to their association with very high concentrations of anthropogenic aerosols. During the KORUS-AQ campaign in S. Korea, which took place in late spring and early summer of 2016, in situ aircraft measurements over the Seoul Metropolitan Area and Taehwa Research Forest (downwind of Seoul) were repeated three times per flight over a 6 week period, providing significant temporal coverage of vertically resolved aerosol properties influenced by different meteorological conditions and sources. Measurements aboard the NASA DC-8 by the NOAA Humidified Dual Single Particle Soot Photometers (HD-SP2) quantified BC mass, size distributions, mixing state, and the hygroscopicity of BC containing aerosols. The in situ BC mass vertical profiles are combined with estimated absorption enhancement calculated from observed optical size and hygroscopicity using Mie theory, and then integrated over the depth of the profile to calculate BC's contribution to AAOD. Along with bulk aerosol size distributions and hygroscopicity, bulk absorbing aerosol optical properties, and on-board sky radiance measurements, these measurements are compared with ground-based AERONET site measurements of AAOD to evaluate closure between in situ vertical profiles of BC and AAOD measurements. This study will provide constraints on the relative importance of BC (including lensing and hygroscopicity effects) and non-BC components to AAOD over S. Korea.

Aerosol Optical Properties in Southeast Asia From AERONET Observations

Science.gov (United States)

Eck, T. F.; Holben, B. N.; Boonjawat, J.; Le, H. V.; Schafer, J. S.; Reid, J. S.; Dubovik, O.; Smirnov, A.

2003-12-01

There is little published data available on measured optical properties of aerosols in the Southeast Asian region. The AERONET project and collaborators commenced monitoring of aerosol optical properties in February 2003 at four sites in Thailand and two sites in Viet Nam to measure the primarily anthropogenic aerosols generated by biomass burning and fossil fuel combustion/ industrial emissions. Automatic sun/sky radiometers at each site measured spectral aerosol optical depth in 7 wavelengths from 340 to 1020 nm and combined with directional radiances in the almucantar, retrievals were made of spectral single scattering albedo and aerosol size distributions. Angstrom exponents, size distributions and spectral single scattering albedo of primarily biomass burning aerosols at rural sites are compared to measurements made at AERONET sites in other major biomass burning regions in tropical southern Africa, South America, and in boreal forest regions. Additionally, the aerosol single scattering albedo and size distributions measured in Bangkok, Thailand are compared with those measured at other urban sites globally. The influences of aerosols originating from other regions outside of Southeast Asia are analyzed using trajectory analyses. Specifically, cases of aerosol transport and mixing from Southern China and from India are presented.

Investigating Soot Morphology in Counterflow Flames at Elevated Pressures

KAUST Repository

Amin, Hafiz Muhammad Fahid

2018-01-01

Practical combustion devices such as gas turbines and diesel engines operate at high pressures to increase their efficiency. Pressure significantly increases the overall soot yield. Morphology of these ultra-fine particles determines their airborne lifetime and their interaction with the human respiratory system. Therefore, investigating soot morphology at high pressure is of practical relevance. In this work, a novel experimental setup has been designed and built to study the soot morphology at elevated pressures. The experimental setup consists of a pressure vessel, which can provide optical access from 10° to 165° for multi-angle light scattering, and a counterflow burner which produces laminar flames at elevated pressures. In the first part of the study, N2-diluted ethylene/air and ethane air counterflow flames are stabilized from 2 to 5 atm. Two-angle light scattering and extinction technique have been used to study the effects of pressure on soot parameters. Path averaged soot volume fraction is found to be very sensitive to pressure and increased significantly from 2 to 5 atm. Primary particle size and aggregate size also increased with pressure. Multi-angle light scattering is also performed and flames are investigated from 3 to 5 atm. Scattering to absorption ratio is calculated from multi-angle light scattering and extinction data. Scattering to absorption ratio increased with pressure whereas the number of primary particles in an aggregate decreased with increasing pressure. In the next part of the study, Thermophoretic Sampling of soot is performed, in counterflow flames from 3 to 10 atm, followed by transmission electron microscopy. Mean primary particle size increased with pressure and these trends are consistent withour light scattering measurements. Fractal properties of soot aggregates are found to be insensitive to pressure. 2D diffused light line of sight attenuation (LOSA) and Laser Induced Incandescence (LII) are used to measure local soot

Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

Energy Technology Data Exchange (ETDEWEB)

Turner, David, D.; Ferrare, Richard, A.

2011-07-06

The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

Physicochemical properties of aerosol released in the case of a fire involving materials used in the nuclear industry

Energy Technology Data Exchange (ETDEWEB)

Ouf, F.-X., E-mail: francois-xavier.ouf@irsn.fr [Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES/SCA/LPMA, PSN-RES/SCA/LECEV, Gif-Sur-Yvette 91192 (France); Mocho, V.-M.; Pontreau, S.; Wang, Z. [Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES/SCA/LPMA, PSN-RES/SCA/LECEV, Gif-Sur-Yvette 91192 (France); Ferry, D. [Aix-Marseille Université, CNRS UMR 7325, CINaM, 13009 Marseille (France); Yon, J. [CORIA-UMR 6614-Normandie Université, CNRS-Université et Insa de Rouen, Campus Universitaire du Madrillet, 76800 Saint-Etienne-du-Rouvray (France)

2015-02-11

Graphical abstract: - Highlights: • We characterize the aerosol emitted during thermal degradation of common materials. • Oxygen concentration on aerosol properties has been investigated. • Influence of oxygen concentration is limited to the organic carbon fraction. • The organic carbon fraction is correlated to the C:H ratio. • For pure materials, monomer diameter is correlated to the emission factor. - Abstract: For industrial concerns, and more especially for nuclear applications, the characterization of soot is essential for predicting the behaviour of containment barriers in fire conditions. This study deals with the characterization (emission factor, composition, size, morphology, microstructure) of particles produced during thermal degradation of materials found in nuclear facilities (electrical cables, polymers, oil and solvents). Small-scale experiments have been conducted for oxygen concentrations [O{sub 2}] ranging from 15% to 21% in order to imitate the oxygen depletion encountered during a confined fire. Particles denote distinct shapes, from aggregates composed of monomers with diameters ranging from 31.2 nm to 52.8 nm, to compact nanoparticles with diameters ranging from 15 nm to 400 nm, and their composition strongly depends on fuel type. Despite the organic to total carbon ratio (OC/TC), their properties are poorly influenced by the decrease in [O{sub 2}]. Finally, two empirical correlations are proposed for predicting the OC/TC ratio and the monomer diameter, respectively, as a function of the fuel's carbon to hydrogen ratio and the emission factor.

Ice Nucleation of Soot Particles in the Cirrus Regime: Is Pore Condensation and Freezing Relevant for Soot?

Science.gov (United States)

Kanji, Z. A.; Mahrt, F.; David, R.; Marcolli, C.; Lohmann, U.; Fahrni, J.; Brühwiler, D.

2017-12-01

Heterogeneous ice nucleation (HIN) onto soot particles from previous studies have produced inconsistent results of temperature and relative humidity conditions required for freezing depending on the source of soot particle investigated. The ability of soot to act as HIN depended on the type of soot and size of particle. Often homogenous freezing conditions or water saturation conditions were required to freeze soot particles, rendering HIN irrelevant. Using synthesised mesoporous silica particles, we show pore condensation and freezing works with experiments performed in the Zurich Ice Nucleation Chamber (ZINC). By testing a variety of soot particles in parallel in the Horizontal Ice Nucleation Chamber (HINC), we suggest that previously observed HIN on soot particles is not the responsible mechanism for ice formation. Laboratory generated CAST brown and black soot, commercially available soot and acid treated soot were investigated for their ice nucleation abilities in the mixed-phase and cirrus cloud temperature regimes. No heterogeneous ice nucleation activity is inferred at T > -38 °C (mixed-phase cloud regime), however depending on particle size and soot type, HIN was observed for T nucleation of ice in the pores or cavities that are ubiquitous in soot particles between the primary spherules. The ability of some particles to freeze at lower relative humidity compared to others demonstrates why hydrophobicity plays a role in ice nucleation, i.e. controlling the conditions at which these cavities fill with water. Thus for more hydrophobic particles pore filling occurs at higher relative humidity, and therefore freezing of pore water and ice crystal growth. Future work focusses on testing the cloud processing ability of soot particles and water adsorption isotherms of the different soot samples to support the hydrophobicity inferences from the ice nucleation results.

Simulation of temporal and spatial soot evolution in an automotive diesel engine using the Moss–Brookes soot model

International Nuclear Information System (INIS)

Pang, Kar Mun; Ng, Hoon Kiat; Gan, Suyin

2012-01-01

Highlights: ► Numerical models were validated against experimental data of two diesel engines. ► Soot model constant values were calibrated to predict in-cylinder soot processes. ► Effects of split-main injection parameters on soot distributions were determined. ► Soot cloud was distributed towards cylinder wall when using large dwell period. ► Greater soot deposition expected with large dwell period and retarded injection. - Abstract: In this reported work, computational study on the formation processes of soot particles from diesel combustion is conducted using an approach where Computational Fluid Dynamics (CFD) is coupled with a chemical kinetic model. A multi-step soot model which accounts for inception, surface growth, coagulation and oxidation was applied. Model constant values in the Moss–Brookes soot formation and Fenimore–Jones soot oxidation models were calibrated, and were validated against in-cylinder soot evolution and exhaust soot density of both heavy- and light-duty diesel engines, respectively. Effects of various injection parameters such as start of injection (SOI) timing, split-main ratio and dwell period of the split-main injection strategy on in-cylinder temporal/spatial soot evolution in a light-duty diesel engine were subsequently investigated. The spatial soot distributions at each crank angle degree after start of injection were found to be insensitive to the change of values in SOI and split-main ratio when close-coupled injection was implemented. Soot cloud was also observed to be distributed towards the cylinder wall when a large separation of 20° was used, even with an advanced SOI timing of −6° after top dead centre (ATDC). The use of large separation is hence not desired for this combustion system as it potentially leads to soot deposition on surface oil film and greater tailpipe soot emissions.

Aerosol-Cloud Interactions During Puijo Cloud Experiments - The effects of weather and local sources

Science.gov (United States)

Komppula, Mika; Portin, Harri; Leskinen, Ari; Romakkaniemi, Sami; Brus, David; Neitola, Kimmo; Hyvärinen, Antti-Pekka; Kortelainen, Aki; Hao, Liqing; Miettinen, Pasi; Jaatinen, Antti; Ahmad, Irshad; Lihavainen, Heikki; Laaksonen, Ari; Lehtinen, Kari E. J.

2013-04-01

The Puijo measurement station has provided continuous data on aerosol-cloud interactions since 2006. The station is located on top of the Puijo observation tower (306 m a.s.l, 224 m above the surrounding lake level) in Kuopio, Finland. The top of the tower is covered by cloud about 15 % of the time, offering perfect conditions for studying aerosol-cloud interactions. With a twin-inlet setup (total and interstitial inlets) we are able to separate the activated particles from the interstitial (non-activated) particles. The continuous twin-inlet measurements include aerosol size distribution, scattering and absorption. In addition cloud droplet number and size distribution are measured continuously with weather parameters. During the campaigns the twin-inlet system was additionally equipped with aerosol mass spectrometer (AMS) and Single Particle Soot Photometer (SP-2). This way we were able to define the differences in chemical composition of the activated and non-activated particles. Potential cloud condensation nuclei (CCN) in different supersaturations were measured with two CCN counters (CCNC). The other CCNC was operated with a Differential Mobility Analyzer (DMA) to obtain size selected CCN spectra. Other additional measurements included Hygroscopic Tandem Differential Mobility Analyzer (HTDMA) for particle hygroscopicity. Additionally the valuable vertical wind profiles (updraft velocities) are available from Halo Doppler lidar during the 2011 campaign. Cloud properties (droplet number and effective radius) from MODIS instrument onboard Terra and Aqua satellites were retrieved and compared with the measured values. This work summarizes the two latest intensive campaigns, Puijo Cloud Experiments (PuCE) 2010 & 2011. We study especially the effect of the local sources on the cloud activation behaviour of the aerosol particles. The main local sources include a paper mill, a heating plant, traffic and residential areas. The sources can be categorized and identified

Chinese Soot on a Vietnamese Soup

Science.gov (United States)

Mari, X.

2015-12-01

Black Carbon (BC) is an aerosol emitted as soot during biomass burning and fossil fuels combustion together with other carbonaceous aerosols such as organic carbon (OC) and polyaromatic hydrocarbons (PAHs). While the impacts of BC on health and climate have been studied for many years, studies about its deposition and impact on marine ecosystems are scares. This is rather surprising considering that a large fraction of atmospheric BC deposits on the surface of the ocean via dry or wet deposition. On a global scale, deposition on the ocean is about 45 Tg C per year, with higher fluxes in the northern hemisphere and in inter-tropical regions, following the occurrence of the hot-spots of concentration. In the present study conducted on shore, in Haiphong and Halong cities, North Vietnam, we measured the seasonal variations of atmospheric BC, OC and PAHs during a complete annual cycle. The presentation will discuss the atmospheric results in terms of seasonal variability and sources. Inputs to the marine system are higher during the dry season, concomitantly with the arrival of air masses enriched in BC coming from the North. However, the carbon fingerprint can significantly differ at shorter time periods depending on the air mass pathway and speed. Our work leads to the characterization and the determination of the relative contribution of more specific sources like local traffic, which includes tourism and fishing boats, coal dust emitted from the nearby mine, and long-range transported aerosols. This variable input of carbonaceous aerosols might have consequences for the cycling and the repartition of carbon and nutrients in the marine ecosystem of Halong Bay.

Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

Energy Technology Data Exchange (ETDEWEB)

Mills, Michael J. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Schmidt, Anja [School of Earth and Environment, University of Leeds, Leeds UK; Easter, Richard [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Solomon, Susan [Department of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge Massachusetts USA; Kinnison, Douglas E. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Ghan, Steven J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Neely, Ryan R. [School of Earth and Environment, University of Leeds, Leeds UK; National Centre for Atmospheric Science, University of Leeds, Leeds UK; Marsh, Daniel R. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Conley, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Bardeen, Charles G. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Gettelman, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA

2016-03-06

Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptions between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.

The impact of carbon dioxide and exhaust gas recirculation on the oxidative reactivity of soot from ethylene flames and diesel engines

Science.gov (United States)

Al-Qurashi, Khalid O.

Restrictive emissions standards to reduce nitrogen oxides (NOx) and particulate matter (PM) emissions from diesel engines necessitate the development of advanced emission control technology. The engine manufacturers in the United States have implemented the exhaust gas recirculation (EGR) and diesel particulate filters (DPF) to meet the stringent emissions limits on NOx and PM, respectively. Although the EGR-DPF system is an effective means to control diesel engine emissions, there are some concerns associated with its implementation. The chief concern with this system is the DPF regenerability, which depends upon several factors, among which are the physicochemical properties of the soot. Despite the plethora of research that has been conducted on DPF regenerability, the impact of EGR on soot reactivity and DPF regenerability is yet to be examined. This work concerns the impact of EGR on the oxidative reactivity of diesel soot. It is part of ongoing research to bridge the gap in establishing a relationship between soot formation conditions, properties, and reactivity. This work is divided into three phases. In the first phase, carbon dioxide (CO2) was added to the intake charge of a single cylinder engine via cylinders of compressed CO2. This approach simulates the cold-particle-free EGR. The results showed that inclusion of CO2 changes the soot properties and yields synergistic effects on the oxidative reactivity of the resulting soot. The second phase of this research was motivated by the findings from the first phase. In this phase, post-flame ethylene soot was produced from a laboratory co-flow laminar diffusion flame to better understand the mechanism by which the CO2 affects soot reactivity. This phase was accomplished by successfully isolating the dilution, thermal, and chemical effects of the CO2. The results showed that all of these effects account for a measurable increase in soot reactivity. Nevertheless, the thermal effect was found to be the most

Observational evidence for the aerosol impact on ice cloud properties regulated by cloud/aerosol types

Science.gov (United States)

Zhao, B.; Gu, Y.; Liou, K. N.; Jiang, J. H.; Li, Q.; Liu, X.; Huang, L.; Wang, Y.; Su, H.

2017-12-01

The interactions between aerosols and ice clouds (consisting only of ice) represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. The observational evidence for the aerosol impact on ice cloud properties has been quite limited and showed conflicting results, partly because previous observational studies did not consider the distinct features of different ice cloud and aerosol types. Using 9-year satellite observations, we find that, for ice clouds generated from deep convection, cloud thickness, cloud optical thickness (COT), and ice cloud fraction increase and decrease with small-to-moderate and high aerosol loadings, respectively. For in-situ formed ice clouds, however, the preceding cloud properties increase monotonically and more sharply with aerosol loadings. The case is more complicated for ice crystal effective radius (Rei). For both convection-generated and in-situ ice clouds, the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters, but the sensitivities of Rei to aerosols under the same water vapor amount differ remarkably between the two ice cloud types. As a result, overall Rei slightly increases with aerosol loading for convection-generated ice clouds, but decreases for in-situ ice clouds. When aerosols are decomposed into different types, an increase in the loading of smoke aerosols generally leads to a decrease in COT of convection-generated ice clouds, while the reverse is true for dust and anthropogenic pollution. In contrast, an increase in the loading of any aerosol type can significantly enhance COT of in-situ ice clouds. The modulation of the aerosol impacts by cloud/aerosol types is demonstrated and reproduced by simulations using the Weather Research and Forecasting (WRF) model. Adequate and accurate representations of the impact of different cloud/aerosol types in climate models are crucial for reducing the

Effects of methyl group on aromatic hydrocarbons on the nanostructures and oxidative reactivity of combustion-generated soot

KAUST Repository

Guerrero Peñ a, Gerardo D.J.; Alrefaai, Mhd Maher; Yang, Seung Yeon; Raj, Abhijeet; Brito, Joaquin L.; Stephen, Samuel; Anjana, Tharalekshmy; Pillai, Vinu; Al Shoaibi, Ahmed; Chung, Suk-Ho

2016-01-01

The substituted and unsubstituted aromatic hydrocarbons, present in transportation fuels such as gasoline and diesel, are thought to be responsible for most of the soot particles produced during their combustion. However, the effects of the substituted alkyl groups on the aromatic hydrocarbons on their sooting tendencies, and on the physical and chemical properties of soot produced from them are not well understood. In this work, the effect of the presence of methyl groups on aromatic hydrocarbons on their sooting propensity, and on the oxidative reactivity, morphology, and chemical composition of soot generated from them in diffusion flames is studied using benzene, toluene, and m-xylene as fuels. Several experimental techniques including high resolution transmission electron microscopy and X-ray diffraction are used to identify the morphological changes in soot, whereas the elemental and thermo-gravimetric analyses, electron energy loss spectroscopy, and Fourier transform infrared spectroscopy are used to study the changes in its chemical properties and reactivity. The activation energies for soot oxidation are calculated at different conversion levels, and a trend in the reactivity of soots from benzene, toluene and m-xylene is reported. It is observed that the sizes of primary particles and graphene-like sheets, and the concentrations of aliphatics and oxygenated groups in soot particles decreased with the addition of methyl group(s) on the aromatic ring. The physicochemical changes in soot are found to support the oxidative reactivity trends. © 2016 The Combustion Institute

Effects of methyl group on aromatic hydrocarbons on the nanostructures and oxidative reactivity of combustion-generated soot

KAUST Repository

Guerrero Peña, Gerardo D.J.

2016-07-23

The substituted and unsubstituted aromatic hydrocarbons, present in transportation fuels such as gasoline and diesel, are thought to be responsible for most of the soot particles produced during their combustion. However, the effects of the substituted alkyl groups on the aromatic hydrocarbons on their sooting tendencies, and on the physical and chemical properties of soot produced from them are not well understood. In this work, the effect of the presence of methyl groups on aromatic hydrocarbons on their sooting propensity, and on the oxidative reactivity, morphology, and chemical composition of soot generated from them in diffusion flames is studied using benzene, toluene, and m-xylene as fuels. Several experimental techniques including high resolution transmission electron microscopy and X-ray diffraction are used to identify the morphological changes in soot, whereas the elemental and thermo-gravimetric analyses, electron energy loss spectroscopy, and Fourier transform infrared spectroscopy are used to study the changes in its chemical properties and reactivity. The activation energies for soot oxidation are calculated at different conversion levels, and a trend in the reactivity of soots from benzene, toluene and m-xylene is reported. It is observed that the sizes of primary particles and graphene-like sheets, and the concentrations of aliphatics and oxygenated groups in soot particles decreased with the addition of methyl group(s) on the aromatic ring. The physicochemical changes in soot are found to support the oxidative reactivity trends. © 2016 The Combustion Institute

Origins of atmospheric aerosols. Basic concepts on aerosol main physical properties; L`aerosol atmospherique: ses origines quelques notions sur les principales proprietes physiques des aerosols

Energy Technology Data Exchange (ETDEWEB)

Renoux, A. [Paris-12 Univ., 94 - Creteil (France). Laboratoire de Physique des aerosols et de transferts des contaminations

1996-12-31

Natural and anthropogenic sources of atmospheric aerosols are reviewed and indications of their concentrations and granulometry are given. Calculation of the lifetime of an atmospheric aerosol of a certain size is presented and the various modes of aerosol granulometry and their relations with photochemical and physico-chemical processes in the atmosphere are discussed. The main physical, electrical and optical properties of aerosols are also presented: diffusion coefficient, dynamic mobility and relaxation time, Stokes number, limit rate of fall, electrical mobility, optical diffraction

Atmospheric Aerosol Properties and Climate Impacts

Science.gov (United States)

Chin, Mian; Kahn, Ralph A.; Remer, Lorraine A.; Yu, Hongbin; Rind, David; Feingold, Graham; Quinn, Patricia K.; Schwartz, Stephen E.; Streets, David G.; DeCola, Phillip;

Light-Absorbing Aerosol during NASA GRIP: Overview of Observations in the Free Troposphere and Associated with Tropical Storm Systems

Science.gov (United States)

Ziemba, L. D.; Beyersdorf, A. J.; Chen, G.; Corr, C. A.; Craig, L.; Dhaniyala, S.; Dibb, J. E.; Hudgins, C. H.; Ismail, S.; Latham, T.; Nenes, A.; Thornhill, K. L.; Winstead, E.; Anderson, B. E.

2010-12-01

Aerosols play a significant role in regulating Earth’s climate. Absorbing aerosols typically constitute a small fraction of ambient particle mass but can contribute significantly to direct and indirect climate forcing depending on size, mixing state, concentration, chemical composition, and vertical and spatial distribution. Aerosols may also significantly affect tropical storm/hurricane dynamics through direct light absorption and activation as cloud nuclei. An extensive suite of instrumentation measuring aerosol chemical, physical, and optical properties was deployed aboard the NASA DC-8 to characterize aerosol during the NASA GRIP (Genesis and Rapid Intensification Processes; August-September 2010) mission. The majority of flight time was spent at high altitude (greater than 9 km) and thus much of the sampling was done in the free troposphere, including extensive sampling in the vicinity of tropical storm systems and more diffuse cirrus clouds. With operations based in Fort Lauderdale, FL and St. Croix, U.S. Virgin Islands, a large geographic region was sampled including much of the Gulf of Mexico and tropical Atlantic Ocean. Observations are reported for light-absorbing carbon aerosol (mainly black carbon, BC) primarily using a single particle soot photometer (SP2). The SP2 employs single-particle laser-induced incandescence to provide a mass-specific measurement not subject to scattering interference that is optimal for the low concentration environments like those encountered during GRIP. BC mass concentrations, 100-500 nm size distributions, and mixing state (i.e. coating thickness of scattering material) are presented. Total and sub-micron aerosol absorption coefficients (principally from BC and dust aerosol) are reported using a particle soot absorption photometer (PSAP) along with comparisons with calculated absorption coefficients derived from SP2 observations in various conditions. In addition, dust aerosol is specifically identified using optical and

Mass spectrometric analysis and aerodynamic properties of various types of combustion-related aerosol particles

Science.gov (United States)

Schneider, J.; Weimer, S.; Drewnick, F.; Borrmann, S.; Helas, G.; Gwaze, P.; Schmid, O.; Andreae, M. O.; Kirchner, U.

2006-12-01

Various types of combustion-related particles in the size range between 100 and 850 nm were analyzed with an aerosol mass spectrometer and a differential mobility analyzer. The measurements were performed with particles originating from biomass burning, diesel engine exhaust, laboratory combustion of diesel fuel and gasoline, as well as from spark soot generation. Physical and morphological parameters like fractal dimension, effective density, bulk density and dynamic shape factor were derived or at least approximated from the measurements of electrical mobility diameter and vacuum aerodynamic diameter. The relative intensities of the mass peaks in the mass spectra obtained from particles generated by a commercial diesel passenger car, by diesel combustion in a laboratory burner, and by evaporating and re-condensing lubrication oil were found to be very similar. The mass spectra from biomass burning particles show signatures identified as organic compounds like levoglucosan but also others which are yet unidentified. The aerodynamic behavior yielded a fractal dimension (Df) of 2.09 +/- 0.06 for biomass burning particles from the combustion of dry beech sticks, but showed values around three, and hence more compact particle morphologies, for particles from combustion of more natural oak. Scanning electron microscope images confirmed the finding that the beech combustion particles were fractal-like aggregates, while the oak combustion particles displayed a much more compact shape. For particles from laboratory combusted diesel fuel, a Df value of 2.35 was found, for spark soot particles, Df [approximate] 2.10. The aerodynamic properties of fractal-like particles from dry beech wood combustion indicate an aerodynamic shape factor [chi] that increases with electrical mobility diameter, and a bulk density of 1.92 g cm-3. An upper limit of [chi] [approximate] 1.2 was inferred for the shape factor of the more compact particles from oak combustion.

Retrieval of aerosol complex refractive index from a synergy between lidar, sun photometer and in situ measurements during LISAIR experiment

International Nuclear Information System (INIS)

Raut, J.C.; Chazette, P.

2007-01-01

Particulate pollutant exchanges between the streets and the Planetary Boundary Layer (PBL), and their daily evolution linked to human activity were studied in the framework of the Lidar pour la Surveillance de l'AIR (LISAIR) experiment. This program lasted from 10 to 30 May 2005. A synergetic approach combining dedicated active (lidar) and passive (sun photometer) remote sensors as well as ground based in situ instrumentation (nephelometer, aethalometer and particle sizers) was used to investigate urban aerosol optical properties within Paris. Aerosol complex refractive indices were assessed to be 1.56-0.034 i at 355 nm and 1.59-0.040 i at 532 nm, thus leading to single-scattering albedo values between 0.80 and 0.88. These retrievals are consistent with soot components in the aerosol arising from traffic exhausts indicating that these pollutants have a radiative impact on climate. We also discussed the influence of relative humidity on aerosol properties. A good agreement was found between vertical extinction profile derived from lidar backscattering signal and retrieved from the coupling between radio sounding and ground in situ measurements. (authors)

Comprehensive Measurement of Atmospheric Aerosols with a Wide Range Aerosol Spectrometer

International Nuclear Information System (INIS)

Keck, L; Pesch, M; Grimm, H

2011-01-01

A wide range aerosol spectrometer (WRAS) was used for comprehensive long term measurements of aerosol size distributions. The system combines the results of an optical aerosol spectrometer with the results of a Scanning Mobility Particle Sizer (SMPS) to record essentially the full size range (5 nm - 32 μm) of atmospheric particles in 72 channels. Measurements were carried out over one year (2009) at the Global Atmospheric Watch (GAW)-Station Hohenpeissenberg, Bavaria. Total particle number concentrations obtained from the aerosol size distributions were compared to the total number concentrations measured by a Condensation Particle Counter (CPC). The comparison showed an excellent agreement of the data. The high time resolution of 5 minutes allows the combination of the measured size distributions with meteorological data and correlations to gaseous pollutants (CO, NOx and SO2). A good correlation of particle number and CO concentrations was found for long distance transported small particles, which were probably mainly soot particles. Correlations to NOx were observed for aerosols from local sources such as traffic emissions. The formation of secondary aerosols from gaseous precursors was also observed. Episodes of relatively high concentration of particles in the range of 2-3 μm were probably caused by pollen.

Development of high fidelity soot aerosol dynamics models using method of moments with interpolative closure

KAUST Repository

Roy, Subrata P.; Arias, Paul G.; Lecoustre, Vivien R.; Haworth, Daniel C.; Im, Hong G.; Trouvé , Arnaud C.

2014-01-01

of ad hoc treatments such as clipping. The solutions proposed and demonstrated here are being applied to generate new physical insight into complex turbulence-chemistry-soot-radiation interactions in turbulent reacting flows using DNS. © 2014 Copyright

Effect of Dopant Loading on the Structural and Catalytic Properties of Mn-Doped SrTiO3 Catalysts for Catalytic Soot Combustion

Directory of Open Access Journals (Sweden)

Santiago Iván Suárez-Vázquez

2018-02-01

Full Text Available Soot particles have been associated with respiratory diseases and cancer. To decrease these emissions, perovskite-mixed oxides have been proposed due to their thermal stability and redox surface properties. In this work, SrTiO3 doped with different amounts of Mn were synthesized by the hydrothermal method and tested for soot combustion. Results show that at low Mn content, structural distortion, and higher Oads/Olat ratio were observed which was attributed to the high content of Mn3+ in Ti sites. On the other hand, increasing the Mn content led to surface segregation of manganese oxide. All synthesized catalysts showed mesopores in the range of 32–47 nm. In the catalytic combustion of soot, the samples synthesized in this work lowered the combustion temperature by more than 100 °C compared with the uncatalyzed reaction. The sample doped with 1 wt % of Mn showed the best catalytic activity. The activation energy of these samples was also calculated, and the order of decreasing activation energy is as follows: uncatalyzed > Mn0 > Mn8 > Mn4 > Mn1. The best catalytic activity for Mn1 was attributed to its physicochemical properties and the mobility of the oxygen from the bulk to the surface at temperatures higher than 500 °C.

Influence of thermal radiation on soot production in Laminar axisymmetric diffusion flames

International Nuclear Information System (INIS)

Demarco, R.; Nmira, F.; Consalvi, J.L.

2013-01-01

The aim of this paper is to study the effect of radiative heat transfer on soot production in laminar axisymmetric diffusion flames. Twenty-four C 1 –C 3 hydrocarbon–air flames, consisting of normal (NDF) and inverse (IDF) diffusion flames at both normal gravity (1 g) and microgravity (0 g), and covering a wide range of conditions affecting radiative heat transfer, were simulated. The numerical model is based on the Steady Laminar Flamelet (SLF) model, a semi-empirical two-equation acetylene/benzene based soot model and the Statistical Narrow Band Correlated K (SNBCK) model coupled to the Finite Volume Method (FVM) to compute thermal radiation. Predictions relative to velocity, temperature, soot volume fraction and radiative losses are on the whole in good agreement with the available experimental data. Model results show that, for all the flames considered, thermal radiation is a crucial process with a view to providing accurate predictions for temperatures and soot concentrations. It becomes increasingly significant from IDFs to NDFs and its influence is much greater as gravity is reduced. The radiative contribution of gas prevails in the weakly-sooting IDFs and in the methane and ethane NDFs, whereas soot radiation dominates in the other flames. However, both contributions are significant in all cases, with the exception of the 1 g IDFs investigated where soot radiation can be ignored. The optically-thin approximation (OTA) was also tested and found to be applicable as long as the optical thickness, based on flame radius and Planck mean absorption coefficient, is less than 0.05. The OTA is reasonable for the IDFs and for most of the 1 g NDFs, but it fails to predict the radiative heat transfer for the 0 g NDFs. The accuracy of radiative-property models was then assessed in the latter cases. Simulations show that the gray approximation can be applied to soot but not to combustion gases. Both the non-gray and gray soot versions of the Full Spectrum Correlated

A model study of aggregates composed of spherical soot monomers with an acentric carbon shell

Science.gov (United States)

Luo, Jie; Zhang, Yongming; Zhang, Qixing

2018-01-01

Influences of morphology on the optical properties of soot particles have gained increasing attentions. However, studies on the effect of the way primary particles are coated on the optical properties is few. Aimed to understand how the primary particles are coated affect the optical properties of soot particles, the coated soot particle was simulated using the acentric core-shell monomers model (ACM), which was generated by randomly moving the cores of concentric core-shell monomers (CCM) model. Single scattering properties of the CCM model with identical fractal parameters were calculated 50 times at first to evaluate the optical diversities of different realizations of fractal aggregates with identical parameters. The results show that optical diversities of different realizations for fractal aggregates with identical parameters cannot be eliminated by averaging over ten random realizations. To preserve the fractal characteristics, 10 realizations of each model were generated based on the identical 10 parent fractal aggregates, and then the results were averaged over each 10 realizations, respectively. The single scattering properties of all models were calculated using the numerically exact multiple-sphere T-matrix (MSTM) method. It is found that the single scattering properties of randomly coated soot particles calculated using the ACM model are extremely close to those using CCM model and homogeneous aggregate (HA) model using Maxwell-Garnett effective medium theory. Our results are different from previous studies. The reason may be that the differences in previous studies were caused by fractal characteristics but not models. Our findings indicate that how the individual primary particles are coated has little effect on the single scattering properties of soot particles with acentric core-shell monomers. This work provides a suggestion for scattering model simplification and model selection.

Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing

Directory of Open Access Journals (Sweden)

J. E. Penner

2009-02-01

Full Text Available Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm⁻² while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm⁻² and −0.16 to −0.12 Wm⁻², respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.

A small porous-plug burner for studies of combustion chemistry and soot formation

Science.gov (United States)

Campbell, M. F.; Schrader, P. E.; Catalano, A. L.; Johansson, K. O.; Bohlin, G. A.; Richards-Henderson, N. K.; Kliewer, C. J.; Michelsen, H. A.

2017-12-01

We have developed and built a small porous-plug burner based on the original McKenna burner design. The new burner generates a laminar premixed flat flame for use in studies of combustion chemistry and soot formation. The size is particularly relevant for space-constrained, synchrotron-based X-ray diagnostics. In this paper, we present details of the design, construction, operation, and supporting infrastructure for this burner, including engineering attributes that enable its small size. We also present data for charactering the flames produced by this burner. These data include temperature profiles for three premixed sooting ethylene/air flames (equivalence ratios of 1.5, 1.8, and 2.1); temperatures were recorded using direct one-dimensional coherent Raman imaging. We include calculated temperature profiles, and, for one of these ethylene/air flames, we show the carbon and hydrogen content of heavy hydrocarbon species measured using an aerosol mass spectrometer coupled with vacuum ultraviolet photoionization (VUV-AMS) and soot-volume-fraction measurements obtained using laser-induced incandescence. In addition, we provide calculated mole-fraction profiles of selected gas-phase species and characteristic profiles for seven mass peaks from AMS measurements. Using these experimental and calculated results, we discuss the differences between standard McKenna burners and the new miniature porous-plug burner introduced here.

Aerosol Activation Properties within and above Mixing Layer in the North China Plain

Science.gov (United States)

Deng, Z.; Ran, L.

2013-12-01

Aerosol particles, serving as cloud condensation nuclei (CCN), may modify the properties of clouds and have an impact on climate. The vertical distribution of aerosols and their activation properties is critical to quantify the effect of aerosols on clouds. An intensive field campaign, Vertical Observations of trace Gases and Aerosols in the North China Plain (VOGA-NCP 2013), was conducted in the North China Plain during the late July and early August 2013 to measure the vertical profiles of atmospheric components in this polluted region and estimate their effects on atmospheric environment and climate. Aerosols were measured with in-situ instruments and Lidar. Particularly, the aerosols were collected at 1000 m height with a 1 m3 bag sampler attached to a tethered balloon, and subsequently measured with combined scanning mobility particle sizer (SMPS) and CCN counter. Comparisons of size-resolved activation ratios at ground level and 1000 m height showed that aerosols in upper atmosphere were not only less concentrated, but also less CCN-active than those at the surface. The difference in aerosol properties between upper atmosphere and the ground indicates that the analysis of impacts of aerosols on cloud might be misleading in heavily polluted region based on the relationship of cloud properties and surface aerosols or column without considering the vertical distribution of aerosol activation abilities.

Ground-Based Remote Sensing of Aerosol Properties over a Coastal Megacity of Pakistan

OpenAIRE

Tariq, Salman; Ul-Haq, Zia

2018-01-01

Atmospheric aerosols are considered to be an important constituent of Earth’s atmosphere because of their climatic, environmental, and health effects. Therefore, while studying the global climate change, investigation of aerosol concentrations and properties is essential both at local and regional levels. In this paper, we have used relatively long-term Aerosol Robotic Network (AERONET) data during September 2006–August 2014 to analyze aerosol properties such as aerosol optical depth at 500 n...

In situ aerosol characterization at Cape Verde. Part 2: Parametrization of relative humidity- and wavelength-dependent aerosol optical properties

Energy Technology Data Exchange (ETDEWEB)

Schladitz, Alexander; Muller, Thomas; Nordmann, Stephan; Tesche, Matthias; Wiedensohler, Alfred (Leibniz Institute for Tropospheric Research (IfT), Leipzig (Germany)), e-mail: alexander.schladitz@tropos.de; Gross, Silke; Freudenthaler, Volker; Gasteiger, Josef (Meteorological Institute, Ludwig-Maximilians-Universitaet, Munich (Germany))

2011-09-15

An observation-based numerical study of humidity-dependent aerosol optical properties of mixed marine and Saharan mineral dust aerosol is presented. An aerosol model was developed based on measured optical and microphysical properties to describe the marine and Saharan dust aerosol at Cape Verde. A wavelength-dependent optical equivalent imaginary part of the refractive index and a scattering non-sphericity factor for Saharan dust were derived. Simulations of humidity effects on optical properties by the aerosol model were validated with relative measurements of the extinction coefficient at ambient conditions. Parametrizations were derived to describe the humidity dependence of the extinction, scattering, and absorption coefficients as well as the asymmetry parameter and single scattering albedo. For wavelengths (300-950 nm) and dry dust volume fractions (0-1), aerosol optical properties as a function of relative humidity (RH = 0-90%) can be calculated from tabulated parameters. For instance, at a wavelength of 550 nm, a volume fraction of 0.5 of dust on the total particle volume (dry conditions) and a RH of 90%, the enhancements for the scattering, extinction and absorption coefficients are 2.55, 2.46 and 1.04, respectively, while the enhancements for the asymmetry parameter and single scattering albedo are 1.11 and 1.04

Quantifying the risks of solid aerosol geoengineering: the role of fundamental material properties

Science.gov (United States)

Dykema, J. A.; Keutsch, F. N.; Keith, D.

2017-12-01

Solid aerosols have been considered as an alternative to sulfate aerosols for solar geoengineering due to their optical and chemical properties, which lead to different and possibly more attractive risk profiles. Solid aerosols can achieve higher solar scattering efficiency due to their higher refractive index, and in some cases may also be less effective absorbers of thermal infrared radiation. The optical properties of solid aerosols are however sensitive functions of the detailed physical properties of solid materials in question. The relevant details include the exact crystalline structure of the aerosols, the physical size of the particles, and interactions with background stratospheric molecular and particulate constituents. In this work, we examine the impact of these detailed physical properties on the radiative properties of calcite (CaCO3) solid aerosols. We examine how crystal morphology, size, chemical reactions, and interaction with background stratospheric aerosol may alter the scattering and absorption properties of calcite aerosols for solar and thermal infrared radiation. For example, in small particles, crystal lattice vibrations associated with the particle surface may lead to substantially different infrared absorption properties than bulk materials. We examine the wavelength dependence of absorption by the particles, which may lead to altered patterns of stratospheric radiative heating and equilibrium temperatures. Such temperature changes can lead to dynamical changes, with consequences for both stratospheric composition and tropospheric climate. We identify important uncertainties in the current state of understanding, investigate risks associated with these uncertainties, and survey potential approaches to quantitatively improving our knowledge of the relevant material properties.

Sooting Characteristics and Modeling in Counterflow Diffusion Flames

KAUST Repository

Wang, Yu

2013-11-01

Soot formation is one of the most complex phenomena in combustion science and an understanding of the underlying physico-chemical mechanisms is important. This work adopted both experimental and numerical approaches to study soot formation in laminar counterfl ow diffusion flames. As polycyclic aromatic hydrocarbons (PAHs) are the precursors of soot particles, a detailed gas-phase chemical mechanism describing PAH growth upto coronene for fuels with 1 to 4 carbon atoms was validated against laminar premixed and counter- flow diffusion fl ames. Built upon this gas-phase mechanism, a soot model was then developed to describe soot inception and surface growth. This soot model was sub- sequently used to study fuel mixing effect on soot formation in counterfl ow diffusion flames. Simulation results showed that compared to the baseline case of the ethylene flame, the doping of 5% (by volume) propane or ethane in ethylene tends to increase the soot volume fraction and number density while keeping the average soot size almost unchanged. These results are in agreement with experimental observations. Laser light extinction/scattering as well as laser induced fluorescence techniques were used to study the effect of strain rate on soot and PAH formation in counterfl ow diffusion ames. The results showed that as strain rate increased both soot volume fraction and PAH concentrations decreased. The concentrations of larger PAH were more sensitive to strain rate compared to smaller ones. The effect of CO2 addition on soot formation was also studied using similar experimental techniques. Soot loading was reduced with CO2 dilution. Subsequent numerical modeling studies were able to reproduce the experimental trend. In addition, the chemical effect of CO2 addition was analyzed using numerical data. Critical conditions for the onset of soot were systematically studied in counterfl ow diffusion ames for various gaseous hydrocarbon fuels and at different strain rates. A sooting

A characterization of Arctic aerosols on the basis of aerosol optical depth and black carbon measurements

Directory of Open Access Journals (Sweden)

R. S. Stone

2014-06-01

Full Text Available Abstract Aerosols, transported from distant source regions, influence the Arctic surface radiation budget. When deposited on snow and ice, carbonaceous particles can reduce the surface albedo, which accelerates melting, leading to a temperature-albedo feedback that amplifies Arctic warming. Black carbon (BC, in particular, has been implicated as a major warming agent at high latitudes. BC and co-emitted aerosols in the atmosphere, however, attenuate sunlight and radiatively cool the surface. Warming by soot deposition and cooling by atmospheric aerosols are referred to as “darkening” and “dimming” effects, respectively. In this study, climatologies of spectral aerosol optical depth AOD (2001–2011 and Equivalent BC (EBC (1989–2011 from three Arctic observatories and from a number of aircraft campaigns are used to characterize Arctic aerosols. Since the 1980s, concentrations of BC in the Arctic have decreased by more than 50% at ground stations where in situ observations are made. AOD has increased slightly during the past decade, with variations attributed to changing emission inventories and source strengths of natural aerosols, including biomass smoke and volcanic aerosol, further influenced by deposition rates and airflow patterns.

Physics of aerosols - Second part: nucleation-condensation-ions-electrification-optical properties

International Nuclear Information System (INIS)

Bricard, Jean

1977-01-01

This report is made of two volumes. Volume 1 includes the general properties of aerosols, the fundamentals of the theory of gases and mechanics are related to particle suspensions, ant the theories of diffusion and coagulation with their applications to atmospheric aerosols. Volume 2 begins with a chapter on nucleation (gas-particle conversion) in the case of one vapor, then two vapors, followed by the theory of aerosol evaporation. The following two chapters are devoted to the study of ions and their attachment to aerosol particles. Finally their optical properties are stated in the last chapter

Effect of Dimethyl Ether Mixing on Soot Size Distribution in Premixed Ethylene Flame

KAUST Repository

Li, Zepeng

2016-04-21

As a byproduct of incomplete combustion, soot attracts increasing attentions as extensive researches exploring serious health and environmental effects from soot particles. Soot emission reduction requires a comprehensive understanding of the mechanism for polycyclic aromatic hydrocarbons and of soot formation and aging processes. Therefore, advanced experimental techniques and numerical simulations have been conducted to investigate this procedure. In order to investigate the effects of dimethyl ether (DME) mixing on soot particle size distribution functions (PSDFs), DME was mixed in premixed ethylene/oxygen/argon at flames at the equivalence ratio of 2.0 with a range of mixing ratio from 0% to 30% of the total carbon fed. Two series of atmospheric pressure flames were tested in which cold gas velocity was varied to obtain different flame temperatures. The evolution of PSDFs along the centerline of the flame was determined by burner stabilized stagnation probe and scanning mobility particle sizer (SMPS) techniques, yielding the PSDFs for various separation distances above the burner surface. Meanwhile, the flame temperature profiles were carefully measured by a thermocouple and the comparison to that of simulated laminar premixed burner-stabilized stagnation flame was satisfactory. Additionally, to understand the chemical role of DME mixing in soot properties, characterization measurements were conducted on soot samples using thermo-gravimetric analysis (TGA) and elemental analysis (EA). Results of the evolution of PSDFs and soot volume fraction showed that adding DME into ethylene flame could reduce soot yield significantly. The addition of DME led to the decrease of both the soot nucleation rate and the particle mass growth rate. To explain the possible mechanism for the observation, numerical simulations were performed. Although DME addition resulted in the slight increase of methyl radicals from pyrolysis, the decrease in acetylene and propargyl radicals

Improved soot blowing, based on needs, through measurement of the natural frequency of the heat transferring tubes; Foerbaettrad behovsstyrd sotning genom maetning av oeverfoerande tubernas egenfrekvens

Energy Technology Data Exchange (ETDEWEB)

Blom, Elisabet; Ivarsson, Christofer

2007-11-15

The aim of the project is to develop a method for detecting soot on the transferring tubes by measuring the Eigen frequency of the tubes as a function of the soot deposit growth. The project is a pilot study independent of boiler type and it is applicable to all boilers where soot deposit on transferring tubes is a repeating issue. The report is supposed to answer two major questions. Is it possible to make use of Eigen frequencies in order to trace soot deposit on transferring tubes? What governing parameters are related to the Eigen frequency of transferring tubes? By today, soot blowing is executed after recommendations from the manufacturer in terms of number of soot blowing per time unit. The fuel type as well as boiler type has great influence on the soot deposit growth. The objective of the project is to investigate whether the mechanical properties of the transferring tube can be used to detect soot deposit. The project is divided into a theoretical and a practical part. The theoretical part covers the design of the probe and the change of its mechanical properties when soot deposit is present. Practical experiments were then carried out in a laboratory were the probes mechanical properties with and without soot deposit were investigated. It was shown that the Eigen frequency of the probe decreased with an increased mass due to soot deposit. A test was also made in a boiler at SAKAB but difficulties in attaching the probe to the inspection hatch. The results varied and the interpretation of the results become difficult. However, it was obvious that the mechanical properties of the probe changed with the amount of soot deposit. It was concluded that detection of soot deposit by studying the mechanical properties of the transferring tubes is possible. Yet, using a probe is no optimal solution, instead measurements should be done directly on the heat transferring tubes. In addition, a strategy for controlling the soot deposit has to be developed

Climate impact of anthropogenic aerosols on cirrus clouds

Science.gov (United States)

Penner, J.; Zhou, C.

2017-12-01

Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. However, the efficacy with which particles act to form cirrus particles in a model depends on the representation of updrafts. Here, we use a representation of updrafts based on observations of gravity waves, and follow ice formation/evaporation during both updrafts and downdrafts. We examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning and from aircraft particles that have previously formed ice in contrails. Results show that fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of -0.15±0.02 Wm-2 while aircraft aerosols that have been pre-activated within contrails exert a forcing of -0.20±0.06 Wm-2, but it is possible to decrease these estimates of forcing if a larger fraction of dust particles act as heterogeneous ice nuclei. In addition aircraft aerosols may warm the climate if a large fraction of these particles act as ice nuclei. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds. This assessment could therefore support climate models with high sensitivity to greenhouse gas forcing, while still allowing the models to fit the overall historical temperature change.

Photoacoustic Optical Properties at UV, VIS, and near IR Wavelengths for Laboratory Generated and Winter Time Ambient Urban Aerosols

Science.gov (United States)

Gyawali, M.; Arnott, W. P.; Zaveri, R. A.; Song, C.; Moosmuller, H.; Liu, L.; Mishchenko, M. I.; Chen, L.-W.A.; Green, M. C.; Watson, J. G.;

Variation of diesel soot characteristics by different types and blends of biodiesel in a laboratory combustion chamber

Energy Technology Data Exchange (ETDEWEB)

Omidvarborna, Hamid; Kumar, Ashok [Department of Civil Engineering, The University of Toledo, Toledo, OH (United States); Kim, Dong-Shik, E-mail: dong.kim@utoledo.edu [Department of Chemical and Environmental Engineering, The University of Toledo, Toledo, OH (United States)

2016-02-15

Very little information is available on the physical and chemical properties of soot particles produced in the combustion of different types and blends of biodiesel fuels. A variety of feedstock can be used to produce biodiesel, and it is necessary to better understand the effects of feedstock-specific characteristics on soot particle emissions. Characteristics of soot particles, collected from a laboratory combustion chamber, are investigated from the blends of ultra-low sulfur diesel (ULSD) and biodiesel with various proportions. Biodiesel samples were derived from three different feedstocks, soybean methyl ester (SME), tallow oil (TO), and waste cooking oil (WCO). Experimental results showed a significant reduction in soot particle emissions when using biodiesel compared with ULSD. For the pure biodiesel, no soot particles were observed from the combustion regardless of their feedstock origins. The overall morphology of soot particles showed that the average diameter of ULSD soot particles is greater than the average soot particles from the biodiesel blends. Transmission electron microscopy (TEM) images of oxidized soot particles are presented to investigate how the addition of biodiesel fuels may affect structures of soot particles. In addition, inductively coupled plasma mass spectrometry (ICP-MS), Fourier transform infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA) were conducted for characterization of soot particles. Unsaturated methyl esters and high oxygen content of biodiesel are thought to be the major factors that help reduce the formation of soot particles in a laboratory combustion chamber. - Highlights: • The unsaturation of biodiesel fuel was correlated with soot characteristics. • Average diameters of biodiesel soot were smaller than that of ULSD. • Eight elements were detected as the marker metals in biodiesel soot particles. • As the degree of unsaturation increased, the oxygen content in FAMEs increased. • Biodiesel

Orientation-averaged optical properties of natural aerosol aggregates

International Nuclear Information System (INIS)

Zhang Xiaolin; Huang Yinbo; Rao Ruizhong

2012-01-01

Orientation-averaged optical properties of natural aerosol aggregates were analyzed by using discrete dipole approximation (DDA) for the effective radius in the range of 0.01 to 2 μm with the corresponding size parameter from 0.1 to 23 for the wavelength of 0.55 μm. Effects of the composition and morphology on the optical properties were also investigated. The composition show small influence on the extinction-efficiency factor in Mie scattering region, scattering- and backscattering-efficiency factors. The extinction-efficiency factor with the size parameter from 9 to 23 and asymmetry factor with the size parameter below 2.3 are almost independent of the natural aerosol composition. The extinction-, absorption, scattering-, and backscattering-efficiency factors with the size parameter below 0.7 are irrespective of the aggregate morphology. The intrinsic symmetry and discontinuity of the normal direction of the particle surface have obvious effects on the scattering properties for the size parameter above 4.6. Furthermore, the scattering phase functions of natural aerosol aggregates are enhanced at the backscattering direction (opposition effect) for large size parameters in the range of Mie scattering. (authors)

Influence of fuel properties on fundamental spray characteristics and soot emissions using different tailor-made fuels from biomass

International Nuclear Information System (INIS)

García, Antonio; Monsalve-Serrano, Javier; Heuser, Benedikt; Jakob, Markus; Kremer, Florian; Pischinger, Stefan

2016-01-01

Highlights: • TMFB show clear potential to reduce soot emissions under mixing-controlled combustion. • The larger lift-off-length of 2-MTHF and 1-octanol promotes soot emissions reduction. • Oxidation process governs the improved soot emissions of DNBE. - Abstract: This work evaluates the potential of some new biomass-derived fuels as candidates for compression ignition operation. Thus, fundamental spray characteristics related to fuel vaporization and fuel/air mixing process for 2-Methyltetrahydrofuran, Di-n-butyl ether and 1-octanol has been studied and compared with conventional EN590 Diesel fuel. For this purpose, OH"∗ chemiluminescence and shadowgraphy measurements in a high pressure chamber as well as 1D simulations with a spray model have been carried out at different operating conditions representative of the NEDC driving cycle. Finally, measured soot emissions in the single-cylinder engine were presented and discussed. Results from the high pressure chamber presented very good agreement in terms of liquid length and vapor penetration with simulation results. Thus, some analytical expressions related to macroscopic spray characteristics have been proposed and validated experimentally for all four fuels. Finally, the single-cylinder engine results confirmed the relevant role of soot formation on final emissions for 1-octanol and 2-MTHF. In addition, DNBE showed greater soot oxidation potential than diesel and other TMFB candidates.

Dust Aerosols at the Source Region During ACE-ASIA: A Surface/Satellite Perspective

Science.gov (United States)

Tsay, Si-Chee; Lau, William K. M. (Technical Monitor)

2001-01-01

ACE (Aerosol Characterization Experiment)-Asia is designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentrations over eastern Asia and along the rim of the western Pacific. The phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian dust is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of dust aerosol radiative flux in addition to measurements of loading and optical thickness. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

Thermal fragmentation and deactivation of combustion-generated soot particles

KAUST Repository

Raj, Abhijeet

2014-09-01

The effect of thermal treatment on diesel soot and on a commercial soot in an inert environment under isothermal conditions at intermediate temperatures (400-900°C) is studied. Two important phenomena are observed in both the soot samples: soot fragmentation leading to its mass loss, and loss of soot reactivity towards O2. Several experimental techniques such as high resolution transmission electron microscopy, electron energy loss spectroscopy, thermo-gravimetric analysis with mass spectrometry, elemental analysis, Fourier transform infrared spectroscopy and X-ray diffraction have been used to identify the changes in structures, functional groups such as oxygenates and aliphatics, σ and π bonding, O/C and H/C ratios, and crystallite parameters of soot particles, introduced by heat. A decrease in the size of primary particles and an increase in the average polycyclic aromatic hydrocarbon (PAH) size was observed in soots after thermal treatment. The activation energies of soot oxidation for thermally treated soot samples were found to be higher than those for the untreated ones at most conversion levels. The cyclic or acyclic aliphatics with sp3 hybridization were present in significant amounts in all the soot samples, but their concentration decreased with thermal treatment. Interestingly, the H/C and the O/C ratios of soot particles increased after thermal treatment, and thus, they do not support the decrease in soot reactivity. The increase in the concentration of oxygenates on soot surface indicate that their desorption from soot surface in the form of CO, CO2 and other oxygenated compounds may not be significant at the temperatures (400-900°C) studied in this work. © 2014 The Combustion Institute.

Microphysical and optical properties of aerosol particles in urban zone during ESCOMPTE

Science.gov (United States)

Mallet, M.; Roger, J. C.; Despiau, S.; Dubovik, O.; Putaud, J. P.

2003-10-01

Microphysical and optical properties of the main aerosol species on a peri-urban site have been investigated during the ESCOMPTE experiment. Ammonium sulfate (AS), nitrate (N), black carbon (BC), particulate organic matter (POM), sea salt (SS) and mineral aerosol (D) size distributions have been used, associated with their refractive index, to compute, from the Mie theory, the key radiative aerosol properties as the extinction coefficient Kext, the mass extinction efficiencies σext, the single scattering albedo ω0 and the asymmetry parameter g at the wavelength of 550 nm. Optical computations show that 90% of the light extinction is due to anthropogenic aerosol and only 10% is due to natural aerosol (SS and D). 44±6% of the extinction is due to (AS) and 40±6% to carbonaceous particles (20±4% to BC and 21±4% to POM). Nitrate aerosol has a weak contribution of 5±2%. Computations of the mass extinction efficiencies σext, single scattering albedo ω0 and asymmetry parameter g indicate that the optical properties of the anthropogenic aerosol are often quite different from those yet published and generally used in global models. For example, the (AS) mean specific mass extinction presents a large difference with the value classically adopted at low relative humidity ( h<60%) (2.6±0.5 instead of 6 m 2 g -1 at 550 nm). The optical properties of the total aerosol layer, including all the aerosol species, indicate a mean observed single-scattering albedo ω0=0.85±0.05, leading to an important absorption of the solar radiation and an asymmetry parameter g=0.59±0.05 which are in a reasonably good agreements with the AERONET retrieval of ω0 (=0.86±0.05) and g (=0.64±0.05) at this wavelength.

Changes in aerosol properties during spring-summer period in the Arctic troposphere

Directory of Open Access Journals (Sweden)

A.-C. Engvall

2008-02-01

Full Text Available The change in aerosol properties during the transition from the more polluted spring to the clean summer in the Arctic troposphere was studied. A six-year data set of observations from Ny-Ålesund on Svalbard, covering the months April through June, serve as the basis for the characterisation of this time period. In addition four-day-back trajectories were used to describe air mass histories. The observed transition in aerosol properties from an accumulation-mode dominated distribution to an Aitken-mode dominated distribution is discussed with respect to long-range transport and influences from natural and anthropogenic sources of aerosols and pertinent trace gases. Our study shows that the air-mass transport is an important factor modulating the physical and chemical properties observed. However, the air-mass transport cannot alone explain the annually repeated systematic and rather rapid change in aerosol properties, occurring within a limited time window of approximately 10 days. With a simplified phenomenological model, which delivers the nucleation potential for new-particle formation, we suggest that the rapid shift in aerosol microphysical properties between the Arctic spring and summer is mainly driven by the incoming solar radiation in concert with transport of precursor gases and changes in condensational sink.

Stochastic Simulation of Soot Formation Evolution in Counterflow Diffusion Flames

Directory of Open Access Journals (Sweden)

Xiao Jiang

2018-01-01

Full Text Available Soot generally refers to carbonaceous particles formed during incomplete combustion of hydrocarbon fuels. A typical simulation of soot formation and evolution contains two parts: gas chemical kinetics, which models the chemical reaction from hydrocarbon fuels to soot precursors, that is, polycyclic aromatic hydrocarbons or PAHs, and soot dynamics, which models the soot formation from PAHs and evolution due to gas-soot and soot-soot interactions. In this study, two detailed gas kinetic mechanisms (ABF and KM2 have been compared during the simulation (using the solver Chemkin II of ethylene combustion in counterflow diffusion flames. Subsequently, the operator splitting Monte Carlo method is used to simulate the soot dynamics. Both the simulated data from the two mechanisms for gas and soot particles are compared with experimental data available in the literature. It is found that both mechanisms predict similar profiles for the gas temperature and velocity, agreeing well with measurements. However, KM2 mechanism provides much closer prediction compared to measurements for soot gas precursors. Furthermore, KM2 also shows much better predictions for soot number density and volume fraction than ABF. The effect of nozzle exit velocity on soot dynamics has also been investigated. Higher nozzle exit velocity renders shorter residence time for soot particles, which reduces the soot number density and volume fraction accordingly.

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores: OPTICAL AND CHEMICAL PROPERTIES OF BROWN CARBON AEROSOLS

Energy Technology Data Exchange (ETDEWEB)

Bluvshtein, Nir [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Lin, Peng [Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Flores, J. Michel [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Segev, Lior [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Mazar, Yinon [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel; Tas, Eran [The Robert H. Smith Faculty of Agriculture, Food and Environment, The Hebrew University of Jerusalem, Rehovot Israel; Snider, Graydon [Department of Physics and Atmospheric Science, Dalhousie University, Halifax Nova Scotia Canada; Weagle, Crystal [Department of Chemistry, Dalhousie University, Halifax Nova Scotia Canada; Brown, Steven S. [Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder Colorado USA; Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder Colorado USA; Laskin, Alexander [Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland Washington USA; Rudich, Yinon [Department of Earth and Planetary Sciences, Weizmann Institute of Science, Rehovot Israel

2017-05-23

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. During the biomass burning event, the overall absorption at 400 nm increased by about two orders of magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.

Climatological aspects of aerosol optical properties in Northern Greece

Directory of Open Access Journals (Sweden)

E. Gerasopoulos

2003-01-01

Full Text Available Measurements of aerosol optical properties (aerosol optical depth, scattering and backscattering coefficients have been conducted at two ground-based sites in Northern Greece, Ouranoupolis (40° 23' N, 23° 57' E, 170 m a.s.l. and Thessaloniki (40° 38' N, 22° 57' E, 80 m a.s.l., between 1999 and 2002. The frequency distributions of the observed parameters have revealed the presence of individual modes of high and low values, indicating the influence from different sources. At both sites, the mean aerosol optical depth at 500 nm was 0.23. Values increase considerably during summer when they remain persistently between 0.3 and 0.5, going up to 0.7-0.8 during specific cases. The mean value of 65±40 Mm-1 of the particle scattering coefficient at 550 nm reflects the impact of continental pollution in the regional boundary layer. Trajectory analysis has shown that higher values of aerosol optical depth and the scattering coefficient are found in the east sector (former Soviet Union countries, eastern Balkan countries, whereas cleaner conditions are found for the NW direction. The influence of Sahara dust events is clearly reflected in the Ångström exponents. About 45-60% of the observed diurnal variation of the optical properties was attributed to the growth of aerosols with humidity, while the rest of the variability is in phase with the evolution of the sea-breeze cell. The contribution of local pollution is estimated to contribute 35±10% to the average aerosol optical depth at the Thessaloniki site during summer. Finally, the aerosol scale height (aerosol optical depth divided by scattering coefficient was found to be related to the height of the boundary layer with values between 0.5-1 km during winter and up to 2.5-3 km during summer.

Evaluation of simulated aerosol properties with the aerosol-climate model ECHAM5-HAM using observations from the IMPACT field campaign

NARCIS (Netherlands)

Roelofs, G.-J.; Brink, H. ten; Kiendler-Scharr, A.; Leeuw, G. de; Mensah, A.; Minikin, A.; Otjes, R.

2010-01-01

In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the

Global direct radiative forcing by process-parameterized aerosol optical properties

Science.gov (United States)

KirkevâG, Alf; Iversen, Trond

2002-10-01

A parameterization of aerosol optical parameters is developed and implemented in an extended version of the community climate model version 3.2 (CCM3) of the U.S. National Center for Atmospheric Research. Direct radiative forcing (DRF) by monthly averaged calculated concentrations of non-sea-salt sulfate and black carbon (BC) is estimated. Inputs are production-specific BC and sulfate from [2002] and background aerosol size distribution and composition. The scheme interpolates between tabulated values to obtain the aerosol single scattering albedo, asymmetry factor, extinction coefficient, and specific extinction coefficient. The tables are constructed by full calculations of optical properties for an array of aerosol input values, for which size-distributed aerosol properties are estimated from theory for condensation and Brownian coagulation, assumed distribution of cloud-droplet residuals from aqueous phase oxidation, and prescribed properties of the background aerosols. Humidity swelling is estimated from the Köhler equation, and Mie calculations finally yield spectrally resolved aerosol optical parameters for 13 solar bands. The scheme is shown to give excellent agreement with nonparameterized DRF calculations for a wide range of situations. Using IPCC emission scenarios for the years 2000 and 2100, calculations with an atmospheric global cliamte model (AFCM) yield a global net anthropogenic DRF of -0.11 and 0.11 W m-2, respectively, when 90% of BC from biomass burning is assumed anthropogenic. In the 2000 scenario, the individual DRF due to sulfate and BC has separately been estimated to -0.29 and 0.19 W m-2, respectively. Our estimates of DRF by BC per BC mass burden are lower than earlier published estimates. Some sensitivity tests are included to investigate to what extent uncertain assumptions may influence these results.

Simulation of soot size distribution in an ethylene counterflow flame

KAUST Repository

Zhou, Kun

2014-01-06

Soot, an aggregate of carbonaceous particles produced during the rich combustion of fossil fuels, is an undesirable pollutant and health hazard. Soot evolution involves various dynamic processes: nucleation soot formation from polycyclic aromatic hydrocarbons (PAHs) condensation PAHs condensing on soot particle surface surface processes hydrogen-abstraction-C2H2-addition, oxidation coagulation two soot particles coagulating to form a bigger particle This simulation work investigates soot size distribution and morphology in an ethylene counterflow flame, using i). Chemkin with a method of moments to deal with the coupling between vapor consumption and soot formation; ii). Monte Carlo simulation of soot dynamics.

Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles.

Science.gov (United States)

Koehler, Kirsten A; DeMott, Paul J; Kreidenweis, Sonia M; Popovicheva, Olga B; Petters, Markus D; Carrico, Christian M; Kireeva, Elena D; Khokhlova, Tatiana D; Shonija, Natalia K

2009-09-28

Cloud condensation nuclei (CCN) activity and ice nucleation behavior (for temperaturesnucleation experiments below -40 degrees C, AEC particles nucleated ice near the expected condition for homogeneous freezing of water from aqueous solutions. In contrast, GTS, TS, and TC1 required relative humidity well in excess of water saturation at -40 degrees C for ice formation. GTS particles required water supersaturation conditions for ice activation even at -51 degrees C. At -51 to -57 degrees C, ice formation in particles with electrical mobility diameter of 200 nm occurred in up to 1 in 1000 TS and TC1 particles, and 1 in 100 TOS particles, at relative humidities below those required for homogeneous freezing in aqueous solutions. Our results suggest that heterogeneous ice nucleation is favored in cirrus conditions on oxidized hydrophilic soot of intermediate polarity. Simple considerations suggest that the impact of hydrophilic soot particles on cirrus cloud formation would be most likely in regions of elevated atmospheric soot number concentrations. The ice formation properties of AEC soot are reasonably consistent with present understanding of the conditions required for aircraft contrail formation and the proportion of soot expected to nucleate under such conditions.

Long-term measurements of aerosol optical parameters in Athens, Greece

Science.gov (United States)

Paraskevopoulou, Despoina; Liakakou, Eleni; Gerasopoulos, Evangelos; Mihalopoulos, Nikolaos

2015-04-01

Aerosol chemical composition was studied in conjunction with its optical properties in the area of Athens Greece. For this purpose, sampling of fine aerosol fraction (PM2,5) took place on a daily basis from August 2010 to April 2013 at an urban background location. The samples are subsequently analyzed for their content in organic (OC) and elemental carbon (EC), major ions and trace metals, resulting in the exercise of chemical mass closure. In parallel, the optical properties of aerosols are recorded using a nephelometer and a particle soot absorption photometer (PSAP), leading to the calculation of scattering (σscat) and absorption (σabs) coefficients, respectively; while single scattering albedo (SSA) and mass scattering and absorption efficiencies are thereinafter calculated. Daily σscat values provide an average of 30.1±3.9 Μm-1 while, the average of σabs is 5.2±1.4 Μm-1. The seasonal cycle of σscat presents maximum during summer and in November, due to long-range transport of aerosol from continental Europe and dust transfer from Africa, respectively. The estimated mass absorption efficiency of EC is estimated to be 8.3±0.2 m2 g-1 for the whole studied period, while the corresponding estimated mass scattering efficiency of PM2.5 is 1.7±0.1 m2 g-1 and does not affected by the presence of dust. The average SSA equals to 0.87±0.11 for the three-year period. On a seasonal basis, SSA presents maximum values during summer that is consistent with the reduction of EC - the main absorbing specie. Finally, the reconstruction of scattering coefficients was performed taking into consideration the measured chemistry of fine aerosol.

Combustion characteristics of water-insoluble elemental and organic carbon in size selected ambient aerosol particles

Directory of Open Access Journals (Sweden)

K. Wittmaack

2005-01-01

Full Text Available Combustion of elemental carbon (EC and organic carbon (OC contained in ambient aerosol matter was explored using scanning electron microscopy (SEM in combination with energy dispersive X-ray analysis (EDX. To ease identification of the particles of interest and to avoid or at least reduce interaction with simultaneously sampled inorganic oxides and salts, the approach used in this work differed in two ways from commonly applied procedures. First, rather than using a mixture of particles of vastly different sizes, as in PM10 or PM2.5, aerosol matter was collected in a 5-stage impactor. Second, the water soluble fraction of the collected matter was removed prior to analysis. Diesel soot particles, which appeared in the well-known form of chain-type aggregates, constituted the major fraction of EC. In contrast, OC containing particles were observed in a variety of shapes, including a sizable amount of bioaerosol matter appearing mostly in the size range above about 1 µm. During heating in ambient air for 1h, diesel soot particles were found to be stable up to 470°C, but complete combustion occurred in a narrow temperature interval between about 480 and 510°C. After diesel soot combustion, minute quantities of 'ash' were observed in the form of aggregated tiny particles with sizes less than 10 nm. These particles could be due to elemental or oxidic contaminants of diesel soot. Combustion of OC was observed over a wide range of temperatures, from well below 200°C to at least 500°C. Incompletely burnt bioaerosol matter was still found after heating to 600°C. The results imply that the EC fraction in aerosol matter can be overestimated significantly if the contribution of OC to a thermogram is not well separated.

Longterm and spatial variability of Aerosol optical properties measured by sky radiometer in Japan sites

Science.gov (United States)

Aoki, K.

2016-12-01

Aerosols and cloud play an important role in the climate change. We started the long-term monitoring of aerosol and cloud optical properties since 1990's by using sky radiometer (POM-01, 02; Prede Co. Ltd., Japan). We provide the information, in this presentation, on the aerosol optical properties with respect to their temporal and spatial variability in Japan site (ex. Sapporo, Toyama, Kasuga and etc). The global distributions of aerosols have been derived from earth observation satellite and have been simulated in numerical models, which assume optical parameters. However, these distributions are difficult to derive because of variability in time and space. Therefore, Aerosol optical properties were investigated using the measurements from ground-based and ship-borne sky radiometer. The sky radiometer is an automatic instrument that takes observations only in daytime under the clear sky conditions. Observation of diffuse solar intensity interval was made every ten or five minutes by once. The aerosol optical properties were computed using the SKYRAD.pack version 4.2. The obtained Aerosol optical properties (Aerosol optical thickness, Ångström exponent, Single scattering albedo, and etc.) and size distribution volume clearly showed spatial and temporal variability in Japan area. In this study, we present the temporal and spatial variability of Aerosol optical properties at several Japan sites, applied to validation of satellite and numerical models. This project is validation satellite of GCOM-C, JAXA. The GCOM-C satellite scheduled to be launched in early 2017.

Airborne Lidar Measurements of Aerosol Optical Properties During SAFARI-2000

Science.gov (United States)

McGill, M. J.; Hlavka, D. L.; Hart, W. D.; Welton, E. J.; Campbell, J. R.; Starr, David OC. (Technical Monitor)

2002-01-01

The Cloud Physics Lidar (CPL) operated onboard the NASA ER-2 high altitude aircraft during the SAFARI-2000 field campaign. The CPL provided high spatial resolution measurements of aerosol optical properties at both 1064 nm and 532 nm. We present here results of planetary boundary layer (PBL) aerosol optical depth analysis and profiles of aerosol extinction. Variation of optical depth and extinction are examined as a function of regional location. The wide-scale aerosol mapping obtained by the CPL is a unique data set that will aid in future studies of aerosol transport. Comparisons between the airborne CPL and ground-based MicroPulse Lidar Network (MPL-Net) sites are shown to have good agreement.

Size-resolved measurement of the mixing state of soot in the megacity Beijing, China: diurnal cycle, aging and parameterization

Directory of Open Access Journals (Sweden)

Y. F. Cheng

2012-05-01

Full Text Available Soot particles are the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences.

The size-resolved (30–320 nm diameter mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa during the CAREBeijing 2006 campaign in Beijing, using a volatility tandem differential mobility analyzer (VTDMA. Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (F_in, decreased from 0.80 to 0.57 when initial D_p increased from 30 to 320 nm. Further analysis reveals that: (1 F_in was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2 F_in had pronounced diurnal cycles. For particles in the accumulation mode (D_p at 100–320 nm, largest F_in were observed at noon time, with "apparent" turnover rates (k_{ex → in} up to 7.8% h⁻¹. (3 F_in was subject to competing effects of both aging and emissions. While aging increases F_in by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce F_in by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4 Under the estimated emission

Aerosol-Cloud Interactions and Cloud Microphysical Properties in the Asir Region of Saudi Arabia

Science.gov (United States)

Kucera, P. A.; Axisa, D.; Burger, R. P.; Li, R.; Collins, D. R.; Freney, E. J.; Buseck, P. R.

2009-12-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region, located adjacent to the Red Sea in the southwest region of Saudi Arabia. Ground measurements of aerosol size distributions, hygroscopic growth factors, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were observed in the Asir region in August 2009. The presentation will include a summary of the analysis and results with a focus on aerosol-cloud interactions and cloud microphysical properties observed during the convective season in the Asir region.

A perspective on SOA generated in aerosol water from glyoxal and methylglyoxal and its impacts on climate-relevant aerosol properties

Science.gov (United States)

Sareen, N.; McNeill, V. F.

2011-12-01

In recent years, glyoxal and methylglyoxal have emerged to be potentially important SOA precursors with significant implications for climate-related aerosol properties. Here we will discuss how the chemistry of these and similar organic compounds in aerosol water can affect the aerosol optical and cloud formation properties. Aqueous-phase SOA production from glyoxal and methylglyoxal is a potential source of strongly light-absorbing organics, or "brown carbon". We characterized the kinetics of brown carbon formation from these precursors in mixtures of ammonium sulfate and water using UV-Vis spectrophotometry. This mechanism has been incorporated into a photochemical box model with coupled gas phase-aqueous aerosol chemistry. Methylglyoxal and related compounds also may impact an aerosol's ability to act as a cloud condensation nucleus. We recently showed via pendant drop tensiometry and aerosol chamber studies that uptake of methylglyoxal from the gas phase driven by aqueous-phase oligomerization chemistry is a potentially significant, previously unidentified source of surface-active organic material in aerosols. Results from pendant drop tensiometry showed significantly depressed surface tension in methylglyoxal-ammonium sulfate solutions. We further found that ammonium sulfate particles exposed to gas-phase methylglyoxal in a 3.5 m3 aerosol reaction chamber activate into cloud droplets at sizes up to 15% lower at a given supersaturation than do pure ammonium sulfate particles. The observed enhancement exceeds that predicted based on Henry's Law and our measurements of surface tension depression in bulk solutions, suggesting that surface adsorption of methylglyoxal plays a role in determining CCN activity. Methylglyoxal and similar gas-phase surfactants may be an important and overlooked source of enhanced CCN activity in the atmosphere. To characterize the SOA products formed in these solutions, an Aerosol Chemical Ionization Mass Spectrometer (CIMS) was used

An investigation of late-combustion soot burnout in a DI diesel engine using simultaneous planar imaging of soot and OH radical

Energy Technology Data Exchange (ETDEWEB)

John E. Dec; Peter L. Kelly-Zion

1999-10-01

Diesel engine design continues to be driven by the need to improve performance while at the same time achieving further reductions in emissions. The development of new designs to accomplish these goals requires an understanding of how the emissions are produced in the engine. Laser-imaging diagnostics are uniquely capable of providing this information, and the understanding of diesel combustion and emissions formation has been advanced considerably in recent years by their application. However, previous studies have generally focused on the early and middle stages of diesel combustion. These previous laser-imaging studies do provide important insight into the soot formation and oxidation processes during the main combustion event. They indicate that prior to the end of injection, soot formation is initiated by fuel-rich premixed combustion (equivalence ratio > 4) near the upstream limit of the luminous portion of the reacting fuel jet. The soot is then oxidized at the diffusion flame around the periphery of the luminous plume. Under typical diesel engine conditions, the diffusion flame does not burn the remaining fuel and soot as rapidly as it is supplied, resulting in an expanding region of rich combustion products and soot. This is evident in natural emission images by the increasing size of the luminous soot cloud prior to the end of injection. Hence, the amount of soot in the combustion chamber typically increases until shortly after the end of fuel injection, at which time the main soot formation period ends and the burnout phase begins. Sampling valve and two-color pyrometry data indicate that the vast majority (more than 90%) of the soot formed is oxidized before combustion ends; however, it is generally thought that a small fraction of this soot from the main combustion zones is not consumed and is the source of tail pipe soot emissions.

Soot oxidation over NOx storage catalysts. Activity and deactivation

International Nuclear Information System (INIS)

Krishna, K.; Makkee, M.

2006-01-01

Soot oxidation activity and deactivation of NO x storage and reduction (NSR) catalysts containing Pt, K, and Ba supported on Al 2 O 3 , are studied under a variety of reaction conditions. K-containing catalysts decrease soot oxidation temperature with O 2 alone and the presence of Pt further enhance the activity due to synergetic effect. The active species responsible for synergism on Pt/K-Al 2 O 3 are unstable and cannot be regenerated. Soot oxidation temperature decreases by about 150 o C with NO+O 2 exhaust feed gas and under lean conditions NSR system acts as catalysed soot filter (CSF). The reactions that are mainly responsible for decreasing soot oxidation temperature are: (1) soot oxidation with NO 2 followed by NO recycles to NO 2 , and (2) soot oxidation with O 2 assisted by NO 2 . Only a part of the stored NO x that is decomposed at high temperatures under lean conditions is found to be useful for soot oxidation. NO x storage capacity of NSR catalysts decreases upon ageing under soot oxidising conditions. This will lead to a decreased soot oxidation activity on stored nitrate decomposition. Pt/K-Al 2 O 3 catalyst is more active, but least stable compared with Pt/Ba-Al 2 O 3 . (author)

Modelling thermal radiation and soot formation in buoyant diffusion flames

International Nuclear Information System (INIS)

Demarco Bull, R.A.

2012-01-01

The radiative heat transfer plays an important role in fire problems since it is the dominant mode of heat transfer between flames and surroundings. It controls the pyrolysis, and therefore the heat release rate, and the growth rate of the fire. In the present work a numerical study of buoyant diffusion flames is carried out, with the main objective of modelling the thermal radiative transfer and the soot formation/destruction processes. In a first step, different radiative property models were tested in benchmark configurations. It was found that the FSCK coupled with the Modest and Riazzi mixing scheme was the best compromise in terms of accuracy and computational requirements, and was a good candidate to be implemented in CFD codes dealing with fire problems. In a second step, a semi-empirical soot model, considering acetylene and benzene as precursor species for soot nucleation, was validated in laminar co flow diffusion flames over a wide range of hydrocarbons (C1-C3) and conditions. In addition, the optically-thin approximation was found to produce large discrepancies in the upper part of these small laminar flames. Reliable predictions of soot volume fractions require the use of an advanced radiation model. Then the FSCK and the semi-empirical soot model were applied to simulate laboratory-scale and intermediate-scale pool fires of methane and propane. Predicted flame structures as well as the radiant heat flux transferred to the surroundings were found to be in good agreement with the available experimental data. Finally, the interaction between radiation and turbulence was quantified. (author)

Aerosol and Cloud Microphysical Properties in the Asir region of Saudi Arabia

Science.gov (United States)

Axisa, Duncan; Kucera, Paul; Burger, Roelof; Li, Runjun; Collins, Don; Freney, Evelyn; Posada, Rafael; Buseck, Peter

2010-05-01

In recent advertent and inadvertent weather modification studies, a considerable effort has been made to understand the impact of varying aerosol properties and concentration on cloud properties. Significant uncertainties exist with aerosol-cloud interactions for which complex microphysical processes link the aerosol and cloud properties. Under almost all environmental conditions, increased aerosol concentrations within polluted air masses will enhance cloud droplet concentration relative to that in unperturbed regions. The interaction between dust particles and clouds are significant, yet the conditions in which dust particles become cloud condensation nuclei (CCN) are uncertain. In order to quantify this aerosol effect on clouds and precipitation, a field campaign was launched in the Asir region of Saudi Arabia as part of a Precipitation Enhancement Feasibility Study. Ground measurements of aerosol size distributions, hygroscopic growth factor, CCN concentrations as well as aircraft measurements of cloud hydrometeor size distributions were done in the Asir region of Saudi Arabia in August 2009. Research aircraft operations focused primarily on conducting measurements in clouds that are targeted for cloud top-seeding, on their microphysical characterization, especially the preconditions necessary for precipitation; understanding the evolution of droplet coalescence, supercooled liquid water, cloud ice and precipitation hydrometeors is necessary if advances are to be made in the study of cloud modification by cloud seeding. Non-precipitating mixed-phase clouds less than 3km in diameter that developed on top of the stable inversion were characterized by flying at the convective cloud top just above the inversion. Aerosol measurements were also done during the climb to cloud base height. The presentation will include a summary of the analysis and results with a focus on the unique features of the Asir region in producing convective clouds, characterization of the

Emissions of soot particles from heat generators

Science.gov (United States)

Lyubov, V. K.; Popov, A. N.; Popova, E. I.

2017-11-01

«Soot carbon» or «Soot» - incomplete combustion or thermal decomposition particulate carbon product of hydrocarbons consisting of particles of various shapes and sizes. Soot particles are harmful substances Class 2 and like a dust dispersed by wind for thousands of kilometers. Soot have more powerful negative factor than carbon dioxide. Therefore, more strict requirements on ecological and economical performance for energy facilities at Arctic areas have to be developed to protect fragile Arctic ecosystems and global climate change from degradation and destruction. Quantity of soot particles in the flue gases of energy facilities is a criterion of effectiveness for organization of the burning process. Some of heat generators do not provide the required energy and environmental efficiency which results in irrational use of energy resources and acute pollution of environment. The paper summarizes the results of experimental study of solid particles emission from wide range of capacity boilers burning different organic fuels (natural gas, fuel oil, coal and biofuels). Special attention is paid to environmental and energy performance of the biofuels combustion. Emissions of soot particles PM2.5 are listed. Structure, composition and dimensions of entrained particles with the use of electronic scanning microscope Zeiss SIGMA VP were also studied. The results reveal an impact of several factors on soot particles emission.

Monte carlo simulation for soot dynamics

KAUST Repository

Zhou, Kun

2012-01-01

A new Monte Carlo method termed Comb-like frame Monte Carlo is developed to simulate the soot dynamics. Detailed stochastic error analysis is provided. Comb-like frame Monte Carlo is coupled with the gas phase solver Chemkin II to simulate soot formation in a 1-D premixed burner stabilized flame. The simulated soot number density, volume fraction, and particle size distribution all agree well with the measurement available in literature. The origin of the bimodal distribution of particle size distribution is revealed with quantitative proof.

Influence of thermal radiation on soot production in Laminar axisymmetric diffusion flames

Science.gov (United States)

Demarco, R.; Nmira, F.; Consalvi, J. L.

2013-05-01

The aim of this paper is to study the effect of radiative heat transfer on soot production in laminar axisymmetric diffusion flames. Twenty-four C1-C3 hydrocarbon-air flames, consisting of normal (NDF) and inverse (IDF) diffusion flames at both normal gravity (1 g) and microgravity (0 g), and covering a wide range of conditions affecting radiative heat transfer, were simulated. The numerical model is based on the Steady Laminar Flamelet (SLF) model, a semi-empirical two-equation acetylene/benzene based soot model and the Statistical Narrow Band Correlated K (SNBCK) model coupled to the Finite Volume Method (FVM) to compute thermal radiation. Predictions relative to velocity, temperature, soot volume fraction and radiative losses are on the whole in good agreement with the available experimental data. Model results show that, for all the flames considered, thermal radiation is a crucial process with a view to providing accurate predictions for temperatures and soot concentrations. It becomes increasingly significant from IDFs to NDFs and its influence is much greater as gravity is reduced. The radiative contribution of gas prevails in the weakly-sooting IDFs and in the methane and ethane NDFs, whereas soot radiation dominates in the other flames. However, both contributions are significant in all cases, with the exception of the 1 g IDFs investigated where soot radiation can be ignored. The optically-thin approximation (OTA) was also tested and found to be applicable as long as the optical thickness, based on flame radius and Planck mean absorption coefficient, is less than 0.05. The OTA is reasonable for the IDFs and for most of the 1 g NDFs, but it fails to predict the radiative heat transfer for the 0 g NDFs. The accuracy of radiative-property models was then assessed in the latter cases. Simulations show that the gray approximation can be applied to soot but not to combustion gases. Both the non-gray and gray soot versions of the Full Spectrum Correlated k (FSCK

Classifying Aerosols Based on Fuzzy Clustering and Their Optical and Microphysical Properties Study in Beijing, China

Directory of Open Access Journals (Sweden)

Wenhao Zhang

2017-01-01

Full Text Available Classification of Beijing aerosol is carried out based on clustering optical properties obtained from three Aerosol Robotic Network (AERONET sites. The fuzzy c-mean (FCM clustering algorithm is used to classify fourteen-year (2001–2014 observations, totally of 6,732 records, into six aerosol types. They are identified as fine particle nonabsorbing, two kinds of fine particle moderately absorbing (fine-MA1 and fine-MA2, fine particle highly absorbing, polluted dust, and desert dust aerosol. These aerosol types exhibit obvious optical characteristics difference. While five of them show similarities with aerosol types identified elsewhere, the polluted dust aerosol has no comparable prototype. Then the membership degree, a significant parameter provided by fuzzy clustering, is used to analyze internal variation of optical properties of each aerosol type. Finally, temporal variations of aerosol types are investigated. The dominant aerosol types are polluted dust and desert dust in spring, fine particle nonabsorbing aerosol in summer, and fine particle highly absorbing aerosol in winter. The fine particle moderately absorbing aerosol occurs during the whole year. Optical properties of the six types can also be used for radiative forcing estimation and satellite aerosol retrieval. Additionally, methodology of this study can be applied to identify aerosol types on a global scale.

Thermo-optical properties of residential coals and combustion aerosols

Science.gov (United States)

Pintér, Máté; Ajtai, Tibor; Kiss-Albert, Gergely; Kiss, Diána; Utry, Noémi; Janovszky, Patrik; Palásti, Dávid; Smausz, Tomi; Kohut, Attila; Hopp, Béla; Galbács, Gábor; Kukovecz, Ákos; Kónya, Zoltán; Szabó, Gábor; Bozóki, Zoltán

2018-04-01

In this study, we present the inherent optical properties of carbonaceous aerosols generated from various coals (hard through bituminous to lignite) and their correlation with the thermochemical and energetic properties of the bulk coal samples. The nanoablation method provided a unique opportunity for the comprehensive investigation of the generated particles under well controlled laboratory circumstances. First, the wavelength dependent radiative features (optical absorption and scattering) and the size distribution (SD) of the generated particulate matter were measured in-situ in aerosol phase using in-house developed and customised state-of-the-art instrumentation. We also investigated the morphology and microstructure of the generated particles using Transmission Electron Microscopy (TEM) and Electron Diffraction (ED). The absorption spectra of the measured samples (quantified by Absorption Angström Exponent (AAE)) were observed to be distinctive. The correlation between the thermochemical features of bulk coal samples (fixed carbon (FC) to volatile matter (VM) ratio and calorific value (CV)) and the AAE of aerosol assembly were found to be (r2 = 0.97 and r2 = 0.97) respectively. Lignite was off the fitted curves in both cases most probably due to its high optically inactive volatile material content. Although more samples are necessary to be investigated to draw statistically relevant conclusion, the revealed correlation between CV and Single Scattering Albedo (SSA) implies that climatic impact of coal combusted aerosol could depend on the thermal and energetic properties of the bulk material.

Impact on vehicle fuel economy of the soot loading on diesel particulate filters made of different substrate materials

International Nuclear Information System (INIS)

Millo, Federico; Andreata, Maurizio; Rafigh, Mahsa; Mercuri, Davide; Pozzi, Chiara

2015-01-01

Wall flow DPFs (Diesel Particulate Filters) are nowadays universally adopted for all European passenger cars. Since the properties of the filter substrate material play a fundamental role in determining the optimal soot loading level to be reached before DPF regeneration, three different filter material substrates (Silicon Carbide, Aluminum Titanate and Cordierite) were investigated in this work, considering different driving conditions, after treatment layouts and regeneration strategies. In the first step of the research, an experimental investigation on the three different substrates over the NEDC (New European Driving Cycle) was performed. The data obtained from experiments were then used for the calibration and the validation of a one dimensional fluid-dynamic engine and after treatment simulation model. Afterward, the model was used to predict the vehicle fuel consumption increments as a function of the exhaust back pressure due to the soot loading for different driving cycles. The results showed that appreciable fuel consumption increments could be noticed only in particular driving conditions, and, as a consequence, in most of the cases the optimal filter regeneration strategy corresponds to reach the highest soot loading that still ensures the component safety even in case of uncontrolled regeneration events. - Highlights: • Three different substrate materials for a Diesel Particulate Filter were investigated. • Fuel consumption increases due to DPF soot loading were generally not appreciable. • Optimal soot loading before regeneration was the highest safeguarding DPF integrity. • SiC substrate showed highest soot load limit and lowest fuel consumption penalties. • AT and Cd substrate properties lead to lower soot load limits than SiC

Mutagenicity of diesel exhaust soot dispersed in phospholipid surfactants

Energy Technology Data Exchange (ETDEWEB)

Wallace, W.; Keane, M.; Xing, S.; Harrison, J.; Gautam, M.; Ong, T.

1994-06-01

Organics extractable from respirable diesel exhaust soot particles by organic solvents have been known for some time to be direct acting frameshift mutagens in the Ames Salmonella typhimurium histidine reversion assay. Upon deposition in a pulmonary alveolus or respiratory bronchiole, respirable diesel soot particles will contact first the hypophase which is coated by and laden with surfactants. To model interactions of soot and pulmonary surfactant, the authors dispersed soots in vitro in the primary phospholipid pulmonary surfactant dipalmitoyl glycerophosphorylcholine (lecithin) (DPL) in physiological saline. They have shown that diesel soots dispersed in lecithin surfactant can express mutagenic activity, in the Ames assay system using S. typhimurium TA98, comparable to that expressed by equal amounts of soot extracted by dichloromethane/dimethylsulfoxide (DCM/DMSO). Here the authors report additional data on the same system using additional exhaust soots and also using two other phospholipids, dipalmitoyl glycerophosphoryl ethanolamine (DPPE), and dipalmitoyl phosphatidic acid (DPPA), with different ionic character hydrophilic moieties. A preliminary study of the surfactant dispersed soot in an eucaryotic cell test system also is reported.

An in situ cell to study phase transitions in individual aerosol particles on a substrate using scanning transmission x-ray microspectroscopy

International Nuclear Information System (INIS)

Huthwelker, T.; Zelenay, V.; Birrer, M.; Krepelova, A.; Raabe, J.; Ammann, M.; Tzvetkov, G.; Vernooij, M. G. C.

2010-01-01

A new in situ cell to study phase transitions and chemical processes on individual aerosol particles in the x-ray transmission microscope at the PolLux beamline of the Swiss light source has been built. The cell is machined from stainless steel and aluminum components and is designed to be used in the standard mount of the microscope without need of complicated rearrangements of the microscope. The cell consists of two parts, a back part which contains connections for the gas supply, heating, cooling devices, and temperature measurement. The second part is a removable clip, which hosts the sample. This clip can be easily exchanged and brought into a sampling unit for aerosol particles. Currently, the cell can be operated at temperatures ranging from -40 to +50 deg. C. The function of the cell is demonstrated using two systems of submicron size: inorganic sodium bromide aerosols and soot originating from a diesel passenger car. For the sodium bromide we demonstrate how phase transitions can be studied in these systems and that O1s spectra from aqueous sodium bromide solution can be taken from submicron sized particles. For the case of soot, we demonstrate that the uptake of water onto individual soot particles can be studied.

Two-Column Aerosol Project: Aerosol Light Extinction Measurements Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Dubey, Manvendra [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Aiken, Allison [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Berg, Larry K. [Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Freedman, Andrew [Aerodyne Research, Inc., Billerica, MA (United States); Gorkowski, Kyle [Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

2016-09-01

We deployed Aerodyne Research Inc.’s first Cavity Attenuated Phase Shift extinction (CAPS PMex) monitor (built by Aerodyne) that measures light extinction by using a visible-light-emitting diode (LED) as a light source, a sample cell incorporating two high-reflectivity mirrors centered at the wavelength of the LED, and a vacuum photodiode detector in Cape Cod in 2012/13 for the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s Two-Column Aerosol Project (TCAP). The efficacy of this instrument is based on the fact that aerosols are broadband scatterers and absorbers of light. The input LED is square-wave modulated and passed through the sample cell that distorts it due to exponential decay by aerosol light absorption and scattering; this is measured at the detector. The amount of phase shift of the light at the detector is used to determine the light extinction. This extinction measurement provides an absolute value, requiring no calibration. The goal was to compare the CAPS performance with direct measurements of absorption with ARM’s baseline photoacoustic soot spectrometer (PASS-3) and nephelometer instruments to evaluate its performance.

Effective Density and Mixing State of Aerosol Particles in a Near-Traffic Urban Environment

DEFF Research Database (Denmark)

Rissler, Jenny; Nordin, Erik Z; Eriksson, Axel C

2014-01-01

-range transport from polluted continental areas. The effective density of each group was relatively stable over time, especially of the soot aggregates, which had effective densities similar to those observed in laboratory studies of fresh diesel exhaust emissions. When heated to 300 °C, the soot aggregate......In urban environments, airborne particles are continuously emitted, followed by atmospheric aging. Also, particles emitted elsewhere, transported by winds, contribute to the urban aerosol. We studied the effective density (mass-mobility relationship) and mixing state with respect to the density...... and more dense particles. Both groups were present at each size in varying proportions. Two types of temporal variability in the relative number fraction of the two groups were found: soot correlated with intense traffic in a diel pattern and dense particles increased during episodes with long...

Climatic impacts of anthropogenic aerosols

Energy Technology Data Exchange (ETDEWEB)

Iversen, T. [Oslo Univ. (Norway)

1996-03-01

This paper was read at the workshop ``The Norwegian Climate and Ozone Research Programme`` held on 11-12 March 1996. Anthropogenic production of aerosols is mainly connected with combustion of fossil fuel. Measured by particulate mass, the anthropogenic sulphate production is the dominating source of aerosols in the Northern Hemisphere. Particles emitted in mechanical processes, fly ash etc. are less important because of their shorter atmospheric residence time. Possible climatological effects of anthropogenic aerosols are usually classified in two groups: direct and indirect. Direct effects are alterations of the radiative heating budget due to the aerosol particles in clear air. Indirect effects involve the interaction between particles and cloud processes. A simplified one-layer radiation model gave cooling in the most polluted mid-latitude areas and heating due to soot absorption in the Arctic. This differential trend in heating rates may have significant effects on atmospheric meridional circulations, which is important for the atmosphere as a thermodynamic system. Recently the description of sulphur chemistry in the hemispheric scale dispersion model has been improved and will be used in a model for Mie scattering and absorption

Experimental and computational investigation of temperature effects on soot mechanisms

Directory of Open Access Journals (Sweden)

Bi Xiaojie

2014-01-01

Full Text Available Effects of initial ambient temperatures on combustion and soot emission characteristics of diesel fuel were investigated through experiment conducted in optical constant volume chamber and simulation using phenomenological soot model. There are four difference initial ambient temperatures adopted in our research: 1000 K, 900 K, 800 K and 700 K. In order to obtain a better prediction of soot behavior, phenomenological soot model was revised to take into account the soot oxidation feedback on soot number density and good agreement was observed in the comparison of soot measurement and prediction. Results indicated that ignition delay prolonged with the decrease of initial ambient temperature. The heat release rate demonstrated the transition from mixing controlled combustion at high ambient temperature to premixed combustion mode at low ambient temperature. At lower ambient temperature, soot formation and oxidation mechanism were both suppressed. But finally soot mass concentration reduced with decreasing initial ambient temperature. Although the drop in ambient temperature did not cool the mean in-cylinder temperature during the combustion, it did shrink the total area of local high equivalence ratio, in which soot usually generated fast. At 700 K initial ambient temperature, soot emissions were almost negligible, which indicates that sootless combustion might be achieved at super low initial temperature operation conditions.

Optics of Water Microdroplets with Soot Inclusions: Exact Versus Approximate Results

Science.gov (United States)

Liu, Li; Mishchenko, Michael I.

2016-01-01

We use the recently generalized version of the multi-sphere superposition T-matrix method (STMM) to compute the scattering and absorption properties of microscopic water droplets contaminated by black carbon. The soot material is assumed to be randomly distributed throughout the droplet interior in the form of numerous small spherical inclusions. Our numerically-exact STMM results are compared with approximate ones obtained using the Maxwell-Garnett effective-medium approximation (MGA) and the Monte Carlo ray-tracing approximation (MCRTA). We show that the popular MGA can be used to calculate the droplet optical cross sections, single-scattering albedo, and asymmetry parameter provided that the soot inclusions are quasi-uniformly distributed throughout the droplet interior, but can fail in computations of the elements of the scattering matrix depending on the volume fraction of soot inclusions. The integral radiative characteristics computed with the MCRTA can deviate more significantly from their exact STMM counterparts, while accurate MCRTA computations of the phase function require droplet size parameters substantially exceeding 60.

Comparing multiple model-derived aerosol optical properties to spatially collocated ground-based and satellite measurements

Science.gov (United States)

Ocko, Ilissa B.; Ginoux, Paul A.

2017-04-01

Anthropogenic aerosols are a key factor governing Earth's climate and play a central role in human-caused climate change. However, because of aerosols' complex physical, optical, and dynamical properties, aerosols are one of the most uncertain aspects of climate modeling. Fortunately, aerosol measurement networks over the past few decades have led to the establishment of long-term observations for numerous locations worldwide. Further, the availability of datasets from several different measurement techniques (such as ground-based and satellite instruments) can help scientists increasingly improve modeling efforts. This study explores the value of evaluating several model-simulated aerosol properties with data from spatially collocated instruments. We compare aerosol optical depth (AOD; total, scattering, and absorption), single-scattering albedo (SSA), Ångström exponent (α), and extinction vertical profiles in two prominent global climate models (Geophysical Fluid Dynamics Laboratory, GFDL, CM2.1 and CM3) to seasonal observations from collocated instruments (AErosol RObotic NETwork, AERONET, and Cloud-Aerosol Lidar with Orthogonal Polarization, CALIOP) at seven polluted and biomass burning regions worldwide. We find that a multi-parameter evaluation provides key insights on model biases, data from collocated instruments can reveal underlying aerosol-governing physics, column properties wash out important vertical distinctions, and improved models does not mean all aspects are improved. We conclude that it is important to make use of all available data (parameters and instruments) when evaluating aerosol properties derived by models.

Linking Aerosol Optical Properties Between Laboratory, Field, and Model Studies

Science.gov (United States)

Murphy, S. M.; Pokhrel, R. P.; Foster, K. A.; Brown, H.; Liu, X.

2017-12-01

The optical properties of aerosol emissions from biomass burning have a significant impact on the Earth's radiative balance. Based on measurements made during the Fourth Fire Lab in Missoula Experiment, our group published a series of parameterizations that related optical properties (single scattering albedo and absorption due to brown carbon at multiple wavelengths) to the elemental to total carbon ratio of aerosols emitted from biomass burning. In this presentation, the ability of these parameterizations to simulate the optical properties of ambient aerosol is assessed using observations collected in 2017 from our mobile laboratory chasing wildfires in the Western United States. The ambient data includes measurements of multi-wavelength absorption, scattering, and extinction, size distribution, chemical composition, and volatility. In addition to testing the laboratory parameterizations, this combination of measurements allows us to assess the ability of core-shell Mie Theory to replicate observations and to assess the impact of brown carbon and mixing state on optical properties. Finally, both laboratory and ambient data are compared to the optical properties generated by a prominent climate model (Community Earth System Model (CESM) coupled with the Community Atmosphere Model (CAM 5)). The discrepancies between lab observations, ambient observations and model output will be discussed.

Theophylline cocrystals prepared by spray drying: physicochemical properties and aerosolization performance.

Science.gov (United States)

Alhalaweh, Amjad; Kaialy, Waseem; Buckton, Graham; Gill, Hardyal; Nokhodchi, Ali; Velaga, Sitaram P

2013-03-01

The purpose of this work was to characterize theophylline (THF) cocrystals prepared by spray drying in terms of the physicochemical properties and inhalation performance when aerosolized from a dry powder inhaler. Cocrystals of theophylline with urea (THF-URE), saccharin (THF-SAC) and nicotinamide (THF-NIC) were prepared by spray drying. Milled THF and THF-SAC cocrystals were also used for comparison. The physical purity, particle size, particle morphology and surface energy of the materials were determined. The in vitro aerosol performance of the spray-dried cocrystals, drug-alone and a drug-carrier aerosol, was assessed. The spray-dried particles had different size distributions, morphologies and surface energies. The milled samples had higher surface energy than those prepared by spray drying. Good agreement was observed between multi-stage liquid impinger and next-generation impactor in terms of assessing spray-dried THF particles. The fine particle fractions of both formulations were similar for THF, but drug-alone formulations outperformed drug-carrier formulations for the THF cocrystals. The aerosolization performance of different THF cocrystals was within the following rank order as obtained from both drug-alone and drug-carrier formulations: THF-NIC>THF-URE>THF-SAC. It was proposed that micromeritic properties dominate over particle surface energy in terms of determining the aerosol performance of THF cocrystals. Spray drying could be a potential technique for preparing cocrystals with modified physical properties.

Heterogeneous reaction of SO2 with soot: The roles of relative humidity and surface composition of soot in surface sulfate formation

Science.gov (United States)

Zhao, Yan; Liu, Yongchun; Ma, Jinzhu; Ma, Qingxin; He, Hong

2017-03-01

The conversion of SO2 to sulfates on the surface of soot is still poorly understood. Soot samples with different fractions of unsaturated hydrocarbons and oxygen-containing groups were prepared by combusting n-hexane under well-controlled conditions. The heterogeneous reaction of SO2 with soot was investigated using in situ attenuated total internal reflection infrared (ATR-IR) spectroscopy, ion chromatography (IC) and a flow tube reactor at the ambient pressure and relative humidity (RH). Water promoted SO2 adsorption and sulfate formation at the RH range from 6% to 70%, while exceeded water condensed on soot was unfavorable for sulfate formation due to inhibition of SO2 adsorption when RH was higher than 80%. The surface composition of soot, which was governed by combustion conditions, also played an important role in the heterogeneous reaction of SO2 with soot. This effect was found to greatly depend on RH. At low RH of 6%, soot with the highest fuel/oxygen ratio of 0.162 exhibited a maximum uptake capacity for SO2 because it contained a large amount of aromatic Csbnd H groups, which acted as active sites for SO2 adsorption. At RH of 54%, soot produced with a fuel/oxygen ratio of 0.134 showed the highest reactivity toward SO2 because it contained appropriate amounts of aromatic Csbnd H groups and oxygen-containing groups, subsequently leading to the optimal surface concentrations of both SO2 and water. These results suggest that variation in the surface composition of soot from different sources and/or resulting from chemical aging in the atmosphere likely affects the conversion of SO2 to sulfates.

Large eddy simulation of soot evolution in an aircraft combustor

Science.gov (United States)

Mueller, Michael E.; Pitsch, Heinz

2013-11-01

An integrated kinetics-based Large Eddy Simulation (LES) approach for soot evolution in turbulent reacting flows is applied to the simulation of a Pratt & Whitney aircraft gas turbine combustor, and the results are analyzed to provide insights into the complex interactions of the hydrodynamics, mixing, chemistry, and soot. The integrated approach includes detailed models for soot, combustion, and the unresolved interactions between soot, chemistry, and turbulence. The soot model is based on the Hybrid Method of Moments and detailed descriptions of soot aggregates and the various physical and chemical processes governing their evolution. The detailed kinetics of jet fuel oxidation and soot precursor formation is described with the Radiation Flamelet/Progress Variable model, which has been modified to account for the removal of soot precursors from the gas-phase. The unclosed filtered quantities in the soot and combustion models, such as source terms, are closed with a novel presumed subfilter PDF approach that accounts for the high subfilter spatial intermittency of soot. For the combustor simulation, the integrated approach is combined with a Lagrangian parcel method for the liquid spray and state-of-the-art unstructured LES technology for complex geometries. Two overall fuel-to-air ratios are simulated to evaluate the ability of the model to make not only absolute predictions but also quantitative predictions of trends. The Pratt & Whitney combustor is a Rich-Quench-Lean combustor in which combustion first occurs in a fuel-rich primary zone characterized by a large recirculation zone. Dilution air is then added downstream of the recirculation zone, and combustion continues in a fuel-lean secondary zone. The simulations show that large quantities of soot are formed in the fuel-rich recirculation zone, and, furthermore, the overall fuel-to-air ratio dictates both the dominant soot growth process and the location of maximum soot volume fraction. At the higher fuel

Properties of arctic haze aerosol from lidar observations during iarea 2015 campaign on spitsbergen

Science.gov (United States)

Stachlewska, Iwona S.; Ritter, Christoph; Böckmann, Christine; Engelmann, Ronny

2018-04-01

Arctic Haze event was observed on 5-8 April 2015 using simultaneously Near-range Aerosol Raman Lidar of IGFUW and Koldewey Aerosol Raman Lidar of AWI, both based at AWIPEV German-French station in Ny-Ålesund, Spitsbergen. The alterations in particle abundance and altitude of the aerosol load observed on following days of the event is analyzed. The daytime profiles of particle optical properties were obtained for both lidars, and then served as input for microphysical parameters inversion. The results indicate aerosol composition typical for the Arctic Haze. However, in some layers, a likely abundance of aqueous aerosol or black carbon originating in biomass burning over Siberia, changes measurably the Arctic Haze properties.

Investigation of black soot staining in houses

Energy Technology Data Exchange (ETDEWEB)

Fugler, D. [Canada Mortgage and Housing Corp., Ottawa, ON (Canada)

2000-07-01

Air quality investigators are frequently called upon to determine the origin of streaking, staining or soot marks in both new and old homes. Those marks display common characteristics: black marks along baseboards at interior or exterior walls, behind furniture and at doorways; black smudges on window frames and plastic cabinets; and even shadowing of studs on exterior wall drywall in a few cases. In most instances, carbon soot from a combustion source is the culprit. The combustion sources include furnaces, water heaters, fireplaces, gas dryers, gas ranges, smoking, vehicle exhaust and candle burning. Scepticism about candle soot is prevalent among callers. As a result, a study was initiated in homes where occupants burn candles regularly to investigate soot problems. Samples were collected from five homes, and included stained carpets, filters, and swab samples of black dust or soot. All the houses selected for the study had been built within a three-year period. Some samples of candles commonly burned in those homes were burnt in a laboratory. Air quality audits had been performed in the homes and had revealed other potential pollutant sources. Best practices for cost-effective clean up and control of soot were researched in industry information. The tests conducted in the laboratory found materials consistent with candle soot or residue during microscopic investigations, but no link was established with the stained material obtained from the homes. A few tips for homeowners were included concerning candle burning, and tips for builders were also offered. 1 tab.

Candle Soot-Driven Performance Enhancement in Pyroelectric Energy Conversion

Science.gov (United States)

Azad, Puneet; Singh, V. P.; Vaish, Rahul

2018-05-01

We observed substantial enhancement in pyroelectric output with the help of candle soot coating on the surface of lead zirconate titanate (PZT). Candle soot of varying thicknesses was coated by directly exposing pyroelectric material to the candle flame. The open-circuit pyroelectric voltage and closed-circuit pyroelectric current were recorded while applying infrared heating across the uncoated and candle soot-coated samples for different heating and cooling cycles. In comparison to the uncoated sample, the maximum open-circuit voltage improves seven times for the candle soot-coated sample and electric current increases by eight times across a resistance of 10Å. Moreover, the harvested energy is enhanced by 50 times for candle soot-coated sample. Results indicate that candle soot coating is an effective and economic method to improve infrared sensing performance of pyroelectric materials.

Computational Investigation of Soot and Radiation in Turbulent Reacting Flows

Science.gov (United States)

Lalit, Harshad

This study delves into computational modeling of soot and infrared radiation for turbulent reacting flows, detailed understanding of both of which is paramount in the design of cleaner engines and pollution control. In the first part of the study, the concept of Stochastic Time and Space Series Analysis (STASS) as a numerical tool to compute time dependent statistics of radiation intensity is introduced for a turbulent premixed flame. In the absence of high fidelity codes for large eddy simulation or direct numerical simulation of turbulent flames, the utility of STASS for radiation imaging of reacting flows to understand the flame structure is assessed by generating images of infrared radiation in spectral bands dominated by radiation from gas phase carbon dioxide and water vapor using an assumed PDF method. The study elucidates the need for time dependent computation of radiation intensity for validation with experiments and the need for accounting for turbulence radiation interactions for correctly predicting radiation intensity and consequently the flame temperature and NOx in a reacting fluid flow. Comparison of single point statistics of infrared radiation intensity with measurements show that STASS can not only predict the flame structure but also estimate the dynamics of thermochemical scalars in the flame with reasonable accuracy. While a time series is used to generate realizations of thermochemical scalars in the first part of the study, in the second part, instantaneous realizations of resolved scale temperature, CO2 and H2O mole fractions and soot volume fractions are extracted from a large eddy simulation (LES) to carry out quantitative imaging of radiation intensity (QIRI) for a turbulent soot generating ethylene diffusion flame. A primary motivation of the study is to establish QIRI as a computational tool for validation of soot models, especially in the absence of conventional flow field and measured scalar data for sooting flames. Realizations of

Effects of compositional heterogeneity and nanoporosity of raw and treated biomass-generated soot on adsorption and absorption of organic contaminants

International Nuclear Information System (INIS)

Chen Baoliang; Huang Wenhai

2011-01-01

A biomass-generated soot was sequentially treated by HCl-HF solution, organic solvent, and oxidative acid to remove ash, extractable native organic matter (EOM), and amorphous carbon. The compositional heterogeneity and nano-structure of the untreated and treated soot samples were characterized by elemental analysis, thermal gravimetric analysis, BET-N 2 surface area, and electron microscopic analysis. Sorption properties of polar and nonpolar organic pollutants onto the soot samples were compared, and individual contributions of adsorption and absorption were quantified. The sorption isotherms for raw sample were practically linear, while were nonlinear for the pretreated-soot. The removal of EOM enhanced adsorption and reduced absorption, indicating that EOM served as a partitioning phase and simultaneously masked the adsorptive sites. By drastic-oxidation, the outer amorphous carbon and the inner disordered core of the soot particles were completely removed, and a fullerene-like nanoporous structure (aromatic shell) was created, which promoted additional π-π interaction between phenanthrene and the soot. - Graphical abstract: The dual sorptive nature of the biomass-generated soot, i.e., the adsorptive effect of the carbonized soot fraction and the partition effect of the amorphous soot component. Research highlights: → The biomass-generated soot owns the heterogeneous compositions and nano-structures. → The soot exhibits the dual sorptive nature, i.e., adsorption and absorption. → Removal of the amorphous component weakens absorption, but strengthens adsorption. → The exposed adsorptive sites with highly aromatic nature promotes π-π interaction. → The dual sorptive nature of the soot depends on the various soot components. - The compositional heterogeneity and nano-structure play a regulating role in the adsorption and absorption of organic contaminants with the untreated and treated soot samples.

On the Scattering Properties of Urban and Maritime Aerosols and its ...

African Journals Online (AJOL)

The scattering properties of aerosols play a dominant role in radiative energy transfer and consequently influencing the visibility and turbidity in the atmosphere. In the present attempt, calculations for scattered intensity have been made in case of urban and maritime aerosols in the varying conditions of relative humidity.

Adaptation of an aerosol retrieval algorithm using multi-wavelength and multi-pixel information of satellites (MWPM) to GOSAT/TANSO-CAI

Science.gov (United States)

Hashimoto, M.; Takenaka, H.; Higurashi, A.; Nakajima, T.

2017-12-01

Aerosol in the atmosphere is an important constituent for determining the earth's radiation budget, so the accurate aerosol retrievals from satellite is useful. We have developed a satellite remote sensing algorithm to retrieve the aerosol optical properties using multi-wavelength and multi-pixel information of satellite imagers (MWPM). The method simultaneously derives aerosol optical properties, such as aerosol optical thickness (AOT), single scattering albedo (SSA) and aerosol size information, by using spatial difference of wavelegths (multi-wavelength) and surface reflectances (multi-pixel). The method is useful for aerosol retrieval over spatially heterogeneous surface like an urban region. In this algorithm, the inversion method is a combination of an optimal method and smoothing constraint for the state vector. Furthermore, this method has been combined with the direct radiation transfer calculation (RTM) numerically solved by each iteration step of the non-linear inverse problem, without using look up table (LUT) with several constraints. However, it takes too much computation time. To accelerate the calculation time, we replaced the RTM with an accelerated RTM solver learned by neural network-based method, EXAM (Takenaka et al., 2011), using Rster code. And then, the calculation time was shorternd to about one thouthandth. We applyed MWPM combined with EXAM to GOSAT/TANSO-CAI (Cloud and Aerosol Imager). CAI is a supplement sensor of TANSO-FTS, dedicated to measure cloud and aerosol properties. CAI has four bands, 380, 674, 870 and 1600 nm, and observes in 500 meters resolution for band1, band2 and band3, and 1.5 km for band4. Retrieved parameters are aerosol optical properties, such as aerosol optical thickness (AOT) of fine and coarse mode particles at a wavelenth of 500nm, a volume soot fraction in fine mode particles, and ground surface albedo of each observed wavelength by combining a minimum reflectance method and Fukuda et al. (2013). We will show

Ignition delay and soot oxidative reactivity of MTBE blended diesel fuel

KAUST Repository

Yang, Seung Yeon; Naser, Nimal; Chung, Suk-Ho; Al-Qurashi, Khalid

2014-01-01

Methyl tert-butyl ether (MTBE) was added to diesel fuel to investigate the effect on ignition delay and soot oxidative reactivity. An ignition quality tester (IQT) was used to study the ignition propensity of MTBE blended diesel fuels in a reactive spray environment. The IQT data showed that ignition delay increases linearly as the MTBE fraction increases in the fuel. A four-stroke single cylinder diesel engine was used to generate soot samples for a soot oxidation study. Soot samples were pre-treated using a tube furnace in a nitrogen environment to remove any soluble organic fractions and moisture content. Non-isothermal oxidation of soot samples was conducted using a thermogravimetric analyzer (TGA). It was observed that oxidation of 'MTBE soot' started began at a lower temperature and had higher reaction rate than 'diesel soot' across a range of temperatures. Several kinetic analyses including an isoconversional method and a combined model fitting method were carried out to evaluate kinetic parameters. The results showed that Diesel and MTBE soot samples had similar activation energy but the pre-exponential factor of MTBE soot was much higher than that of the Diesel soot. This may explain why MTBE soot was more reactive than Diesel soot. It is suggested that adding MTBE to diesel fuel is better for DPF regeneration since an MTBE blend can significantly influence the ignition characteristics and, consequently, the oxidative reactivity of soot. Copyright © 2014 SAE International.

Ignition delay and soot oxidative reactivity of MTBE blended diesel fuel

KAUST Repository

Yang, Seung Yeon

2014-04-01

Methyl tert-butyl ether (MTBE) was added to diesel fuel to investigate the effect on ignition delay and soot oxidative reactivity. An ignition quality tester (IQT) was used to study the ignition propensity of MTBE blended diesel fuels in a reactive spray environment. The IQT data showed that ignition delay increases linearly as the MTBE fraction increases in the fuel. A four-stroke single cylinder diesel engine was used to generate soot samples for a soot oxidation study. Soot samples were pre-treated using a tube furnace in a nitrogen environment to remove any soluble organic fractions and moisture content. Non-isothermal oxidation of soot samples was conducted using a thermogravimetric analyzer (TGA). It was observed that oxidation of \\'MTBE soot\\' started began at a lower temperature and had higher reaction rate than \\'diesel soot\\' across a range of temperatures. Several kinetic analyses including an isoconversional method and a combined model fitting method were carried out to evaluate kinetic parameters. The results showed that Diesel and MTBE soot samples had similar activation energy but the pre-exponential factor of MTBE soot was much higher than that of the Diesel soot. This may explain why MTBE soot was more reactive than Diesel soot. It is suggested that adding MTBE to diesel fuel is better for DPF regeneration since an MTBE blend can significantly influence the ignition characteristics and, consequently, the oxidative reactivity of soot. Copyright © 2014 SAE International.

Optical, microphysical and radiative properties of aerosols over a tropical rural site in Kenya, East Africa: Source identification, modification and aerosol type discrimination

Science.gov (United States)

Boiyo, Richard; Kumar, K. Raghavendra; Zhao, Tianliang

2018-03-01

A better understanding of aerosol optical, microphysical and radiative properties is a crucial challenge for climate change studies. In the present study, column-integrated aerosol optical and radiative properties observed at a rural site, Mbita (0.42°S, 34.20 °E, and 1125 m above sea level) located in Kenya, East Africa (EA) are investigated using ground-based Aerosol Robotic Network (AERONET) data retrieved during January, 2007 to December, 2015. The annual mean aerosol optical depth (AOD500 nm), Ångström exponent (AE440-870 nm), fine mode fraction of AOD500 nm (FMF500 nm), and columnar water vapor (CWV, cm) were found to be 0.23 ± 0.08, 1.01 ± 0.16, 0.60 ± 0.07, and 2.72 ± 0.20, respectively. The aerosol optical properties exhibited a unimodal distribution with substantial seasonal heterogeneity in their peak values being low (high) during the local wet (dry) seasons. The observed data showed that Mbita and its environs are significantly influenced by various types of aerosols, with biomass burning and/or urban-industrial (BUI), mixed (MXD), and desert dust (DDT) aerosol types contributing to 37.72%, 32.81%, and 1.40%, respectively during the local dry season (JJA). The aerosol volume size distribution (VSD) exhibited bimodal lognormal structure with a geometric mean radius of 0.15 μm and 3.86-5.06 μm for fine- and coarse-mode aerosols, respectively. Further, analysis of single scattering albedo (SSA), asymmetry parameter (ASY) and refractive index (RI) revealed dominance of fine-mode absorbing aerosols during JJA. The averaged aerosol direct radiative forcing (ARF) retrieved from the AERONET showed a strong cooling effect at the bottom of the atmosphere (BOA) and significant warming within the atmosphere (ATM), representing the important role of aerosols played in this rural site of Kenya. Finally, the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model revealed that aerosols from distinct sources resulted in enhanced loading

Airborne lidar measurements of aerosol spatial distribution and optical properties over the Atlantic Ocean during a European pollution outbreak of ACE-2[Special issue with manuscripts related to the second Aerosol Characterization Experiment (ACE-2), 16 June-25 July 1997

Energy Technology Data Exchange (ETDEWEB)

Flamant, Cyrille; Pelon, Jaques; Trouillet, Vincent; Bruneau, Didier [CNRS-UPMC-UVSQ, Paris (France). Service d' Aeronomie; Chazette, Patrick; Leon, J.F. [CEA-CNRS, Gif-sur-Yvette (France). Lab. des Sciences du Climat et de l' Environment; Quinn, P.K.; Bates, T.S.; Johnson, James [National Oceanic and Atmospheric Administration, Seattle, WA (United States). Pacific Marine Environmental Lab.; Frouin, Robert [Scripps Inst. of Oceanography, La Jolla, CA (United States); Livingston, John [SRI International, Menlo Park, CA (United States)

2000-04-01

Airborne lidar measurements of the aerosol spatial distribution and optical properties associated with an European pollution outbreak which occurred during the Second Aerosol Characterization Experiment (ACE-2) are presented. Size distribution spectra measured over the ocean near Sagres (Portugal), on-board the Research Vessel Vodyanitsky and on-board the Avion de Recherche Atmospherique et Teledetection (ARAT) have been used to parameterize the aerosol vertical distribution. This parameterization, which is essential to the analysis of airborne lidar measurements, has been validated via closure experiments on extinction coefficient profiles and aerosol optical depth (AOD). During the studied event, AOD's retrieved from lidar measurements at 0.73 {mu}m range between 0.055 and 0.10. The parameterized aerosol vertical distribution has been used to shift AOD retrievals from 0.73 to 0.55 {mu}m to enable comparison with other remote sensing instruments. At the latter wavelength, AOD's retrieved from lidar measurements range between 0.08 and 0.14. An agreement better than 20% is obtained between AOD's derived from lidar and sunphotometer measurements made at the same time and place over the ocean near the coast. However, large differences are observed with the AOD estimated from Meteosat imagery in the same area. These differences are thought to be caused by large uncertainties associated with the Meteosat sensitivity for small AOD's or by the presence of thin scattered clouds. Lidar-derived particulate extinction profiles and scattering coefficient profiles measured by a nephelometer mounted on the ARAT, in a different part of the plume, were found in good agreement, which could be an indication that absorption by pollution aerosols is small and/or that soot is present in small amounts in the European pollution plume. Lidar measurements have also been used to differentiate the contribution of different aerosol layers to the total AOD. It is shown that

Catalytic Oxidation of Soot on a Novel Active Ca-Co Dually-Doped Lanthanum Tin Pyrochlore Oxide

Directory of Open Access Journals (Sweden)

Lijie Ai

2018-04-01

Full Text Available A novel active Ca-Co dually-doping pyrochlore oxide La2−xCaxSn2−yCoyO7 catalyst was synthesized by the sol-gel method for catalytic oxidation of soot particulates. The microstructure, atomic valence, reduction, and adsorption performance were investigated by X-ray powder diffraction (XRD, scanning electron microscope (SEM, Fourier-transform infrared spectroscopy (FT-IR, X-ray photoelectron spectroscopy (XPS, H2-TPR (temperature-programmed reduction, and in situ diffuse reflection infrared Fourier transformed (DRIFTS techniques. Temperature programmed oxidation (TPO tests were performed with the mixture of soot-catalyst under tight contact conditions to evaluate the catalytic activity for soot combustion. Synergetic effect between Ca and Co improved the structure and redox properties of the solids, increased the surface oxygen vacancies, and provided a suitable electropositivity for oxide, directly resulting in the decreased ignition temperature for catalyzed soot oxidation as low as 317 °C. The presence of NO in O2 further promoted soot oxidation over the catalysts with the ignition temperature decreased to about 300 °C. The DRIFTS results reveal that decomposition of less stable surface nitrites may account for NO2 formation in the ignition period of soot combustion, which thus participate in the auxiliary combustion process.

NASA: Black soot fuels global warming

CERN Multimedia

2003-01-01

New research from NASA's Goddard Space Center scientists suggests emissions of black soot have been altering the way sunlight reflects off Earth's snow. The research indicates the soot could be responsible for as much as 25 percent of global warming over the past century (assorted news items, 1 paragraph each).

Method for removing soot from exhaust gases

Science.gov (United States)

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).

Strain rate effect on sooting characteristics in laminar counterflow diffusion flames

KAUST Repository

Wang, Yu

2016-01-20

The effects of strain rate, oxygen enrichment and fuel type on the sooting characteristics of counterflow diffusion flames were studied. The sooting structures and relative PAH concentrations were measured with laser diagnostics. Detailed soot modeling using recently developed PAH chemistry and surface reaction mechanism was performed and the results were compared with experimental data for ethylene flames, focusing on the effects of strain rates. The results showed that increase in strain rate reduced soot volume fraction, average size and peak number density. Increase in oxygen mole fraction increased soot loading and decreased its sensitivity on strain rate. The soot volume fractions of ethane, propene and propane flames were also measured as a function of global strain rate. The sensitivity of soot volume fraction to strain rate was observed to be fuel dependent at a fixed oxygen mole fraction, with the sensitivity being higher for more sooting fuels. However, when the soot loadings were matched at a reference strain rate for different fuels by adjusting oxygen mole fraction, the dependence of soot loading on strain rate became comparable among the tested fuels. PAH concentrations were shown to decrease with increase in strain rate and the dependence on strain rate is more pronounced for larger PAHs. Soot modeling was performed using detailed PAH growth chemistry with molecular growth up to coronene. A qualitative agreement was obtained between experimental and simulation results, which was then used to explain the experimentally observed strain rate effect on soot growth. However, quantitatively, the simulation result exhibits higher sensitivity to strain rate, especially for large PAHs and soot volume fractions.

Effects of DME mixing on number density and size properties of soot particles in counterflow non-premixed ethylene flames

KAUST Repository

Choi, J. H.

2015-05-01

In order to investigate the effect of DME mixing on the number density and size of soot particles, DME was mixed in a counter flow non-premixed ethylene flame with mixture ratios of 5%, 14% and 30%. A laser extinction/scattering technique has been adopted to measure the volume fraction, number density, and mean size of soot particles. The experimental results showed that the highest soot concentrations were observed for flames with mixture ratios of 5% and 14%; however, for a mixture ratio of 30% the soot concentration decreased. Numerical results showed that the concentrations of propargyl radicals (C3H3) at the 5% and 14% ratios were higher than those measured in the ethylene-based flame, and the production of benzene (C6H6) in the 5% and 14% DME mixture flames was also increased. This indicates the crucial role of propargyl in benzene ring formation. These reactions generally become stronger with increased DME mixing, except for A1- + H2 → A1 + H (-R554) and n-C4H5 + C2H2 → A1 + H (R542). Therefore, it is indicated that adding DME to ethylene flames promotes benzene ring formation. Note that although the maximum C6H6 concentration is largest in the 30% DME mixing flame, the soot volume fraction is smaller than those for the 5% and 14% mixture ratios. This is because the local C6H6 concentration decreases in the relatively low temperature region in the fuel side where soot growth occurs. © 2015, The Korean Society of Mechanical Engineers and Springer-Verlag Berlin Heidelberg.

Effects of DME mixing on number density and size properties of soot particles in counterflow non-premixed ethylene flames

KAUST Repository

Choi, J. H.; Choi, B. C.; Lee, S. M.; Chung, Suk-Ho; Jung, K. S.; Jeong, W. L.; Choi, S. K.; Park, S. K.

2015-01-01

In order to investigate the effect of DME mixing on the number density and size of soot particles, DME was mixed in a counter flow non-premixed ethylene flame with mixture ratios of 5%, 14% and 30%. A laser extinction/scattering technique has been adopted to measure the volume fraction, number density, and mean size of soot particles. The experimental results showed that the highest soot concentrations were observed for flames with mixture ratios of 5% and 14%; however, for a mixture ratio of 30% the soot concentration decreased. Numerical results showed that the concentrations of propargyl radicals (C3H3) at the 5% and 14% ratios were higher than those measured in the ethylene-based flame, and the production of benzene (C6H6) in the 5% and 14% DME mixture flames was also increased. This indicates the crucial role of propargyl in benzene ring formation. These reactions generally become stronger with increased DME mixing, except for A1- + H2 → A1 + H (-R554) and n-C4H5 + C2H2 → A1 + H (R542). Therefore, it is indicated that adding DME to ethylene flames promotes benzene ring formation. Note that although the maximum C6H6 concentration is largest in the 30% DME mixing flame, the soot volume fraction is smaller than those for the 5% and 14% mixture ratios. This is because the local C6H6 concentration decreases in the relatively low temperature region in the fuel side where soot growth occurs. © 2015, The Korean Society of Mechanical Engineers and Springer-Verlag Berlin Heidelberg.

Durable superhydrophobic carbon soot coatings for sensor applications

Science.gov (United States)

Esmeryan, K. D.; Radeva, E. I.; Avramov, I. D.

2016-01-01

A novel approach for the fabrication of durable superhydrophobic (SH) carbon soot coatings used in quartz crystal microbalance (QCM) based gas or liquid sensors is reported. The method uses modification of the carbon soot through polymerization of hexamethyldisiloxane (HMDSO) by means of glow discharge RF plasma. The surface characterization shows a fractal-like network of carbon nanoparticles with diameter of ~50 nm. These particles form islands and cavities in the nanometer range, between which the plasma polymerized hexamethyldisiloxane (PPHMDSO) embeds and binds to the carbon chains and QCM surface. Such modified surface structure retains the hydrophobic nature of the soot and enhances its robustness upon water droplet interactions. Moreover, it significantly reduces the insertion loss and dynamic resistance of the QCM compared to the commonly used carbon soot/epoxy resin approach. Furthermore, the PPHMDSO/carbon soot coating demonstrates durability and no aging after more than 40 probing cycles in water based liquid environments. In addition, the surface layer keeps its superhydrophobicity even upon thermal annealing up to 540 °C. These experiments reveal an opportunity for the development of soot based SH QCMs with improved electrical characteristics, as required for high-resolution gas or liquid measurements.

Delayed condensation and frost formation on superhydrophobic carbon soot coatings by controlling the presence of hydrophilic active sites

Science.gov (United States)

Esmeryan, Karekin D.; Castano, Carlos E.; Mohammadi, Reza; Lazarov, Yuliyan; Radeva, Ekaterina I.

2018-02-01

Condensation frosting is an undesired natural phenomenon that could be impeded efficiently using appropriate wettability and morphologically patterned surfaces. The icephobic properties of carbon soot and the fabrication scalability of its synthesis method are a good foundation for anti-frosting applications; however, the fundamentals of frost growth and spreading on sooted surfaces have not been examined yet. In this study, we investigate the anti-frosting performance of three groups of superhydrophobic soot coatings by means of 16 MHz quartz crystal microbalances (QCMs). The analysis of the real-time sensor signal of each soot coated QCM pattern shows that frost formation and its propagation velocity depend on the quantity of oxygen functionalities and structural defects in the material. In turn, the reduction of both parameters shifts the onset of frost growth to temperatures below  -20 °C, whereas the interdroplet ice bridging is slowed by a factor of four. Moreover, high-resolution scanning electron micrographs of the samples imply delamination upon defrosting of the soot with spherical-like morphology via polar interactions driven mechanism. These results reveal an opportunity for control of frost incipiency on sooted surfaces by adjusting the synthesis conditions and depositing soot coatings with as low as possible content of hydrophilic active sites.

Soot measurements by two angle scattering and extinction in an N 2 -diluted ethylene/air counterflow diffusion flame from 2 to 5 atm

KAUST Repository

Amin, Hafiz M.F.

2016-06-27

The soot formed in an N-diluted ethylene/air counterflow diffusion flame at elevated pressure was investigated using two angle light scattering/extinction technique. To provide a well-controlled pressurized environment for the flame, a novel pressure vessel was built with the required optical access. The soot parameters were measured along the centerline of the counterflow flame. These properties included soot volume fraction (f ), primary particle diameter (d ), population averaged radius of gyration (R ) and number density of primary particles (n ). The Rayleigh-Debye-Gans theory for Fractal Aggregates (RDG-FA) was used to retrieve these properties from scattering and extinction measurements. Soot volume fraction was measured via light extinction from 2 to 5atm while maintaining the same global strain rate at all pressures. Scattered light from soot particles was measured at 45° and 135° and primary particle diameter was calculated using scattering/extinction ratio and the radius of gyration was determined from the dissymmetry ratio. Soot volume fraction, primary particle diameter and radius of gyration all increased with pressure while the number density of primary particles decreased with increasing pressure.

Soot measurements by two angle scattering and extinction in an N 2 -diluted ethylene/air counterflow diffusion flame from 2 to 5 atm

KAUST Repository

Amin, Hafiz M.F.; Roberts, William L.

2016-01-01

The soot formed in an N-diluted ethylene/air counterflow diffusion flame at elevated pressure was investigated using two angle light scattering/extinction technique. To provide a well-controlled pressurized environment for the flame, a novel pressure vessel was built with the required optical access. The soot parameters were measured along the centerline of the counterflow flame. These properties included soot volume fraction (f ), primary particle diameter (d ), population averaged radius of gyration (R ) and number density of primary particles (n ). The Rayleigh-Debye-Gans theory for Fractal Aggregates (RDG-FA) was used to retrieve these properties from scattering and extinction measurements. Soot volume fraction was measured via light extinction from 2 to 5atm while maintaining the same global strain rate at all pressures. Scattered light from soot particles was measured at 45° and 135° and primary particle diameter was calculated using scattering/extinction ratio and the radius of gyration was determined from the dissymmetry ratio. Soot volume fraction, primary particle diameter and radius of gyration all increased with pressure while the number density of primary particles decreased with increasing pressure.

Marine Stratocumulus Properties from the FPDR - PDI as a Function of Aerosol during ORACLES

Science.gov (United States)

Small Griswold, J. D.; Heikkila, A.

2016-12-01

Aerosol-cloud interactions in the southeastern Atlantic (SEA) region were investigated during year 1 of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) field project in Aug-Sept 2016. This region is of interest due to seasonally persistent marine stratocumulus cloud decks that are an important component of the climate system due to their radiative and hydrologic impacts. The SEA deck is unique due to the interactions between these clouds and transported biomass burning aerosol during the July-October fire season. These biomass burning aerosol play multiple roles in modifying the cloud deck through interactions with radiation as absorbing aerosol and through modifications to cloud microphysical properties as cloud condensation nuclei. This work uses in situcloud data obtained with a Flight Probe Dual Range - Phase Doppler Interferometer (FPDR - PDI), standard aerosol instrumentation on board the NASA P-3, and reanalysis data to investigate Aerosol-Cloud Interactions (ACI). The FPDR - PDI provides unique cloud microphysical observations of individual cloud drop arrivals allowing for the computation of a variety of microphysical cloud properties including individual drop size, cloud drop number concentration, cloud drop size distributions, liquid water content, and cloud thickness. The FPDR - PDI measurement technique also provides droplet spacing and drop velocity information which is used to investigate turbulence and entrainment mixing processes. We use aerosol information such as average background aerosol amount (low, mid, high) and location relative to cloud (above or mixing) to sort FPDR - PDI cloud properties. To control for meteorological co-variances we further sort the data within aerosol categories by lower tropospheric stability, vertical velocity, and surface wind direction. We then determine general marine stratocumulus cloud characteristics under each of the various aerosol categories to investigate ACI in the SEA.

SAGE II Measurements of Stratospheric Aerosol Properties at Non-Volcanic Levels

Science.gov (United States)

Thomason, Larry W.; Burton, Sharon P.; Luo, Bei-Ping; Peter, Thomas

2008-01-01

Since 2000, stratospheric aerosol levels have been relatively stable and at the lowest levels observed in the historical record. Given the challenges of making satellite measurements of aerosol properties at these levels, we have performed a study of the sensitivity of the product to the major components of the processing algorithm used in the production of SAGE II aerosol extinction measurements and the retrieval process that produces the operational surface area density (SAD) product. We find that the aerosol extinction measurements, particularly at 1020 nm, remain robust and reliable at the observed aerosol levels. On the other hand, during background periods, the SAD operational product has an uncertainty of at least a factor of 2 during due to the lack of sensitivity to particles with radii less than 100 nm.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

Science.gov (United States)

Enroth, Joonas; Mikkilä, Jyri; Németh, Zoltán; Kulmala, Markku; Salma, Imre

2018-04-01

Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20), 50, 75, 110 and 145 nm were determined in situ by using a volatility-hygroscopicity tandem differential mobility analyser (VH-TDMA) system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014-2015. The probability density function of the hygroscopic growth factor (HGF) showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033) independently of the particle size and was assigned to nearly hydrophobic (NH) particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196) with particle diameter, and it was attributed to less hygroscopic (LH) particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF) also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV) and volatile (V) particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non-hygroscopic hydrocarbon-like organics. The hygroscopic

Hygroscopic Properties and Chemical Composition of Aerosol Particles at the High Alpine Site Jungfraujoch

Energy Technology Data Exchange (ETDEWEB)

Weingarter, E.; Gysel, M.; Sjoegren, S.; Baltesperger, U.; Alfarra, R.; Bower, K.; Coe, H.

2004-03-01

The hygroscopic properties of aerosols play a significant role in atmospheric phenomena such as acid deposition, visibility degradation and climate change. Due to the hygroscopic growth of the particles, water is often the dominant component of the ambient aerosol at high relative humidity (RH) conditions. The ability to absorb water depends on the particle chemical composition, dry size, and shape. The aim of this study is to link the chemical composition of the atmospheric aerosol to its hygroscopic properties. (author)

Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

Energy Technology Data Exchange (ETDEWEB)

Srivastava, A.K. [Indian Institute of Tropical Meteorology (Branch), Prof Ramnath Vij Marg, New Delhi (India); Ram, K. [Institute of Environment and Sustainable Development, Banaras Hindu University, Varanasi (India); Singh, Sachchidanand, E-mail: ssingh@nplindia.org [Radio and Atmospheric Sciences Division, CSIR-National Physical Laboratory, New Delhi (India); Kumar, Sanjeev [Radio and Atmospheric Sciences Division, CSIR-National Physical Laboratory, New Delhi (India); Tiwari, S. [Indian Institute of Tropical Meteorology (Branch), Prof Ramnath Vij Marg, New Delhi (India)

2015-01-01

The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (∼ 2000 m amsl) in central Himalaya over a period of more than two years (February 2006–May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm{sup −2}) and high values of corresponding heating rate (0.80 ± 0.14 Kday{sup −1}) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from − 2 to + 14 Wm{sup −2} and from − 3 to − 50 Wm{sup −2} at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm{sup −2} resulting in a heating rate of 0.1–1.8 Kday{sup −1}. - Highlights: • Aerosol chemical and optical properties at Manora Peak, in central Himalaya, were significantly affected by dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. • Elevated AOD and lower SSA values were observed at Manora Peak during summer. • Enhancement in absorbing aerosols was observed during summer. • Large aerosol radiative forcing and heating rate was observed

Aerosol optical properties and radiative effects over Manora Peak in the Himalayan foothills: seasonal variability and role of transported aerosols

International Nuclear Information System (INIS)

Srivastava, A.K.; Ram, K.; Singh, Sachchidanand; Kumar, Sanjeev; Tiwari, S.

2015-01-01

The higher altitude regions of Himalayas and Tibetan Plateau are influenced by the dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. In this study, we present impacts of advection of polluted air masses of natural and anthropogenic emissions, on aerosol optical and radiative properties at Manora Peak (∼ 2000 m amsl) in central Himalaya over a period of more than two years (February 2006–May 2008). We used the most updated and comprehensive data of chemical and optical properties available in one of the most climatically sensitive region, the Himalaya, to estimate atmospheric radiative forcing and heating rate. Aerosol optical depth (AOD) was found to vary from 0.04 to 0.45 with significantly higher values in summer mainly due to an increase in mineral dust and biomass burning aerosols due to transport. In contrast, single scattering albedo (SSA) varied from 0.74 to 0.88 with relatively lower values during summer, suggesting an increase in absorbing BC and mineral dust aerosols. As a result, a large positive atmospheric radiative forcing (about 28 ± 5 Wm −2 ) and high values of corresponding heating rate (0.80 ± 0.14 Kday −1 ) has been found during summer. During the entire observation period, radiative forcing at the top of the atmosphere varied from − 2 to + 14 Wm −2 and from − 3 to − 50 Wm −2 at the surface whereas atmospheric forcing was in the range of 3 to 65 Wm −2 resulting in a heating rate of 0.1–1.8 Kday −1 . - Highlights: • Aerosol chemical and optical properties at Manora Peak, in central Himalaya, were significantly affected by dust and black carbon (BC) aerosols from the emissions and long-range transport from the adjoining areas. • Elevated AOD and lower SSA values were observed at Manora Peak during summer. • Enhancement in absorbing aerosols was observed during summer. • Large aerosol radiative forcing and heating rate was observed over the station in the

Physical and chemical comparison of soot in hydrocarbon and biodiesel fuel diffusion flames: A study of model and commercial fuels

Energy Technology Data Exchange (ETDEWEB)

Matti Maricq, M. [Research and Advanced Engineering, Ford Motor Company, Dearborn, MI (United States)

2011-01-15

Data are presented to compare soot formation in both surrogate and practical fatty acid methyl ester biodiesel and petroleum fuel diffusion flames. The approach here uses differential mobility analysis to follow the size distributions and electrical charge of soot particles as they evolve in the flame, and laser ablation particle mass spectrometry to elucidate their composition. Qualitatively, these soot properties exhibit a remarkably similar development along the flames. The size distributions begin as a single mode of precursor nanoparticles, evolve through a bimodal phase marking the onset of aggregate formation, and end in a self preserving mode of fractal-like particles. Both biodiesel and hydrocarbon fuels yield a common soot composition dominated by C{sub x}H{sub y}{sup +} ions, stabilomer PAHs, and fullerenes in the positive ion mass spectrum, and C{sub x}{sup -} and C{sub 2x}H{sup -} in the negative ion spectrum. These ion intensities initially grow with height in the diffusion flames, but then decline during later stages, consistent with soot carbonization. There are important quantitative differences between fuels. The surrogate biodiesel fuel methyl butanoate substantially reduces soot levels, but soot formation and evolution in this flame are delayed relative to both soy and petroleum fuels. In contrast, soots from soy and hexadecane flames exhibit nearly quantitative agreement in their size distribution and composition profiles with height, suggesting similar soot precursor chemistry. (author)

Preliminary results of aerosols' properties studied with EPF measurements from the SPICAM/UV instrument

Science.gov (United States)

Willame, Yannick; Carine Vandaele, Ann; Depiesse, Cedric; Gillotay, Didier; Kochenova, Svetlana; Montmessin, Franck

2013-04-01

Aerosols on Mars have an important impact on the radiative transfer properties of its atmosphere. Today their spectral properties and therefore their interaction with UV radiation are only poorly known. Improving the radiative transfer modeling requires a better knowledge of their characteristics, in particular of their opacity, phase function and single scattering albedo. Part of such information can be accessed by using EPF observations. The SPICAM instrument on board of the Mars-Express satellite is a 2 channel spectrometer. One channel operates in the ultraviolet (118-320 nm) and the second one in the infrared (1.0-1.7μm). SPICAM has been orbiting around the red planet since 2003 and has thus provided a large set of data. The instrument is capable of measuring under different geometries (nadir, limb, occultation) and one of them, called EPF (Emission Phase Function), can be a tool to study aerosols' properties. We have developed a new retrieval algorithm for nadir measurements based on the radiative transfer model LIDORT. This new code performs simulations of spectra taking into account gas absorption, surface reflection and scattering by aerosols and gases. The retrieval method, based on the optimal estimation, allows us up to now to deduce the ozone column density, the aerosols' optical depth and the surface albedo (with fixed wavelength dependencies). We are developing our model further in order to better study the aerosols' characteristics using EPF observations, which consist in looking at the same point on the planet while the satellite moves along the orbit. As the attempt to study all the aerosols' properties simultaneously was not convincing, we started studying their opacity and the influence of its altitude distribution with the other characteristics fixed. We will present preliminary results of our study on aerosols' properties using EPF data from SPICAM.

Aerosol physical and optical properties in the Eastern Mediterranean Basin, Crete, from Aerosol Robotic Network data

Directory of Open Access Journals (Sweden)

A. Fotiadi

2006-01-01

Full Text Available In this study, we investigate the aerosol optical properties, namely aerosol extinction optical thickness (AOT, Angström parameter and size distribution over the Eastern Mediterranean Basin, using spectral measurements from the recently established FORTH (Foundation for Research and Technology-Hellas AERONET station in Crete, for the two-year period 2003–2004. The location of the FORTH-AERONET station offers a unique opportunity to monitor aerosols from different sources. Maximum values of AOT are found primarily in spring, which together with small values of the Angström parameter indicate dust transported from African deserts, whereas the minimum values of AOT occur in winter. In autumn, large AOT values observed at near-infrared wavelengths arise also from dust transport. In summer, large AOT values at ultraviolet (340 nm and visible wavelengths (500 nm, together with large values of the Angström parameter, are associated with transport of fine aerosols of urban/industrial and biomass burning origin. The Angström parameter values vary on a daily basis within the range 0.05–2.20, and on a monthly basis within the range 0.68–1.9. This behaviour, together with broad frequency distributions and back-trajectory analyses, indicates a great variety of aerosol types over the study region including dust, urban-industrial and biomass-burning pollution, and maritime, as well as mixed aerosol types. Large temporal variability is observed in AOT, Angström parameter, aerosol content and size. The fine and coarse aerosol modes persist throughout the year, with the coarse mode dominant except in summer. The highest values of AOT are related primarily to southeasterly winds, associated with coarse aerosols, and to a less extent to northwesterly winds associated with fine aerosols. The results of this study show that the FORTH AERONET station in Crete is well suited for studying the transport and mixing of different types of aerosols from a variety

Simulation of soot size distribution in an ethylene counterflow flame

KAUST Repository

Zhou, Kun; Abdelgadir, Ahmed Gamaleldin; Bisetti, Fabrizio

2014-01-01

Soot, an aggregate of carbonaceous particles produced during the rich combustion of fossil fuels, is an undesirable pollutant and health hazard. Soot evolution involves various dynamic processes: nucleation soot formation from polycyclic aromatic

Formation of Soot in Counterflow Diffusion Flames with Carbon Dioxide Dilution

KAUST Repository

Wang, Yu

2016-05-04

Experimental and numerical modeling studies have been performed to investigate the effect of CO2 dilution on soot formation in ethylene counterflow diffusion flames. Thermal and chemical effects of CO2 addition on soot growth was numerically identified by using a fictitious CO2 species, which was treated as inert in terms of chemical reactions. The results showed that CO2 addition reduces soot formation both thermodynamically and chemically. In terms of chemical effect, the addition of CO2 decreases soot formation through various pathways, including: (1) reduced soot precursor (PAH) formation leading to lower inception rates and soot number density, which in turn results in lower surface area for soot mass addition; (2) reduced H, CH3, and C3H3 concentrations causing lower H abstraction rate and therefore less active site per surface area for soot growth; and (3) reduced C2H2 mole fraction and thus a slower C2H2 mass addition rate. In addition, the sooting limits were also measured for ethylene counterflow flames in both N2 and CO2 atmosphere and the results showed that sooting region was significantly reduced in the CO2 case compared to the N2 case. © 2016 Taylor & Francis.

Dust, Pollution, and Biomass Burning Aerosols in Asian Pacific: A Column Surface/Satellite Perspective

Science.gov (United States)

Tsay, Si-Chee; Lau, William K. M. (Technical Monitor)

2002-01-01

Many recent field experiments are designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentrations over eastern/southeastern Asia and along the rim of the western Pacific. For example, the phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Springtime is also the peak season for biomass burning in southeastern Asia. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian aerosols is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of aerosol radiative flux in addition to measurements of loading and optical depth. At the time of the Terra/MODIS (Moderate Resolution Imaging Spectroradiometer), SeaWiFS (Sea-viewing Wide Field-of-view Sensor), TOMS (Total Ozone Mapping Spectrometer) and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. A column satellite-surface perspective of Asian aerosols will be presented

On the Response of Nascent Soot Nanostructure and Oxidative Reactivity to Photoflash Exposure

Directory of Open Access Journals (Sweden)

Wei Wang

2017-07-01

Full Text Available Soot particles are a kind of major pollutant from fuel combustion. To enrich the understanding of soot, this work focuses on investigating detailed influences of instantaneous external irradiation (conventional photoflash exposure on nanostructure as well as oxidation reactivity of nascent soot particles. By detailed soot characterizations flash can reduce the mass of soot and soot nanostructure can be reconstructed substantially without burning. After flash, the degree of soot crystallization increases while the soot reactive rate decreases and the activation energy increases. In addition, nanostructure and oxidative reactivity of soot in air and Ar after flash are different due to their different thermal conductivities.

Aerosol numerical modelling at local scale

International Nuclear Information System (INIS)

Albriet, Bastien

2007-01-01

At local scale and in urban areas, an important part of particulate pollution is due to traffic. It contributes largely to the high number concentrations observed. Two aerosol sources are mainly linked to traffic. Primary emission of soot particles and secondary nanoparticle formation by nucleation. The emissions and mechanisms leading to the formation of such bimodal distribution are still badly understood nowadays. In this thesis, we try to provide an answer to this problematic by numerical modelling. The Modal Aerosol Model MAM is used, coupled with two 3D-codes: a CFD (Mercure Saturne) and a CTM (Polair3D). A sensitivity analysis is performed, at the border of a road but also in the first meters of an exhaust plume, to identify the role of each process involved and the sensitivity of different parameters used in the modelling. (author) [fr

Variability of aerosol optical properties in the Western Mediterranean Basin

Directory of Open Access Journals (Sweden)

M. Pandolfi

2011-08-01

Full Text Available Aerosol light scattering, absorption and particulate matter (PM concentrations were measured at Montseny, a regional background site in the Western Mediterranean Basin (WMB which is part of the European Supersite for Atmospheric Aerosol Research (EUSAAR. Off line analyses of 24 h PM filters collected with Hi-Vol instruments were performed for the determination of the main chemical components of PM. Mean scattering and hemispheric backscattering coefficients (@ 635 nm were 26.6±23.2 Mm⁻¹ and 4.3±2.7 Mm⁻¹, respectively and the mean aerosol absorption coefficient (@ 637 nm was 2.8±2.2 Mm⁻¹. Mean values of Single Scattering Albedo (SSA and Ångström exponent (å (calculated from 450 nm to 635 nm at MSY were 0.90±0.05 and 1.3±0.5 respectively. A clear relationship was observed between the PM₁/PM₁₀ and PM_2.5/PM₁₀ ratios as a function of the calculated Ångström exponents. Mass scattering cross sections (MSC for fine mass and sulfate at 635 nm were 2.8±0.5 m² g⁻¹ and 11.8±2.2 m² g⁻¹, respectively, while the mean aerosol absorption cross section (MAC was 10.4±2.0 m² g⁻¹. The variability in aerosol optical properties in the WMB were largely explained by the origin and ageing of air masses over the measurement site. The MAC values appear dependent of particles aging: similar to the expected absorption cross-section for fresh emissions under Atlantic Advection episodes and higher under aerosol pollution episodes. The analysis of the Ångström exponent as a function of the origin the air masses revealed that polluted winter anticyclonic conditions and summer recirculation scenarios typical of the WMB led to an increase of fine particles in the atmosphere (å = 1.5±0.1 while the aerosol optical properties under Atlantic Advection episodes and Saharan dust outbreaks were clearly

Physical metrology of aerosols; Metrologie physique des aerosols

Energy Technology Data Exchange (ETDEWEB)

Boulaud, D.; Vendel, J. [CEA Saclay, 91 - Gif-sur-Yvette (France). Inst. de Protection et de Surete Nucleaire

1996-12-31

The various detection and measuring methods for aerosols are presented, and their selection is related to aerosol characteristics (size range, concentration or mass range), thermo-hydraulic conditions (carrier fluid temperature, pressure and flow rate) and to the measuring system conditions (measuring frequency, data collection speed, cost...). Methods based on aerosol dynamic properties (inertial, diffusional and electrical methods) and aerosol optical properties (localized and integral methods) are described and their performances and applications are compared

On the formation and early evolution of soot in turbulent nonpremixed flames

KAUST Repository

Bisetti, Fabrizio

2012-01-01

A Direct Numerical Simulation (DNS) of soot formation in an n-heptane/air turbulent nonpremixed flame has been performed to investigate unsteady strain effects on soot growth and transport. For the first time in a DNS of turbulent combustion, Polycyclic Aromatic Hydrocarbons (PAH) are included via a validated, reduced chemical mechanism. A novel statistical representation of soot aggregates based on the Hybrid Method of Moments is used [M.E. Mueller, G. Blanquart, H. Pitsch, Combust. Flame 156 (2009) 1143-1155], which allows for an accurate state-of-the-art description of soot number density, volume fraction, and morphology of the aggregates. In agreement with previous experimental studies in laminar flames, Damköhler number effects are found to be significant for PAH. Soot nucleation and growth from PAH are locally inhibited by high scalar dissipation rate, thus providing a possible explanation for the experimentally observed reduction of soot yields at increasing levels of mixing in turbulent sooting flames. Furthermore, our data indicate that soot growth models that rely on smaller hydrocarbon species such as acetylene as a proxy for large PAH molecules ignore or misrepresent the effects of turbulent mixing and hydrodynamic strain on soot formation due to differences in the species Damköhler number. Upon formation on the rich side of the flame, soot is displaced relative to curved mixture fraction iso-surfaces due to differential diffusion effects between soot and the gas-phase. Soot traveling towards the flame is oxidized, and aggregates displaced away from the flame grow primarily by condensation of PAH on the particle surface. In contrast to previous DNS studies based on simplified soot and chemistry models, surface reactions are found to contribute barely to the growth of soot, for nucleation and condensation processes occurring in the fuel stream are responsible for the most of soot mass generation. Furthermore, the morphology of the soot aggregates is

Quantitative effects of rapid heating on soot-particle sizing through analysis of two-pulse LII

KAUST Repository

Cenker, Emre

2017-02-27

During the rapid laser pulse heating and consecutive cooling in laser-induced incandescence (LII), soot particles may undergo thermal annealing and sublimation processes which lead to a permanent change in its optical properties and its primary particle size, respectively. Overall, effects of these two processes on soot and LII model-based particle sizing are investigated by measuring the two-color time-resolved (2C-TiRe) LII signal decay from in-flame soot after two consecutive laser pulses at 1064-nm wavelength. Experiments are carried out on a non-premixed laminar ethylene/air flame from a Santoro burner with both low and moderate laser fluences suitable for particle sizing. The probe volume is set to a radial position close to the flame axis where the soot particles are known to be immature or less graphitic. With the first pulse, soot is pre-heated, and the LII signal after the consecutive second pulse is used for analysis. The two-color incandescence emission technique is used for the pyrometric determination of the LII-heated peak soot temperature at the second pulse. A new LII simulation tool is developed which accounts for particle heating via absorption and annealing, and cooling via sublimation, conduction, and radiation with various existing sub-models from the literature. The same approach of using two laser pulses is implemented in the simulations. Measurements indicate that thermal annealing and associated absorption enhancement becomes important at laser fluences above 0.17 J/cm2 for the immature in-flame soot. After a heating pulse at 0.33 J/cm2, the increase of the soot absorption function is calculated as 35% using the temperature measured at the second pulse and an absorption model based on the Rayleigh approximation. Present annealing model, on the other hand, predicts graphitization of soot even in the absence of laser heating at typical flame temperatures. Recorded experimental LII signal decays and LII-heated peak soot temperature

Relative importance of nitrate and sulfate aerosol production mechanisms in urban atmospheres

International Nuclear Information System (INIS)

Middleton, P.; Kiang, C.S.

1979-01-01

The relative importance of the various sulfate and nitrate aerosol production mechanisms is calculated for different atmospheric conditions. The calculation scheme used to determine the rates of nitrate and sulfate production, based on the concept that vapor transfer to the aerosols and nitrate and sulfate formation within the aerosols are coupled kinetic processes, considers sulfate formation by ozone and hydrogen peroxide oxidation and catalytic oxidation in the presence of soot, iron and manganese of sulfite solutions and sulfuric acid condensation and nitrate formation by the liquid-phase oxidation of dissolved nitrogen oxides for different initial gas concentrations and particle compositions and sizes. It is found that sulfate production is higher under daytime conditions, primarily proceeding by mechanisms involving sulfuric acid and hydrogen peroxide, while at night oxidation processes on the surface of the aerosol film are more important. Nitrate tends to decrease nighttime sulfate production due to an increase in aerosol acidity and nitrate production is found to be higher under nighttime conditions and in the winter

Effect of CALIPSO Cloud Aerosol Discrimination (CAD) Confidence Levels on Observations of Aerosol Properties near Clouds

Science.gov (United States)

Yang, Weidong; Marshak, Alexander; Varnai, Tamas; Liu, Zhaoyan

2012-01-01

CALIPSO aerosol backscatter enhancement in the transition zone between clouds and clear sky areas is revisited with particular attention to effects of data selection based on the confidence level of cloud-aerosol discrimination (CAD). The results show that backscatter behavior in the transition zone strongly depends on the CAD confidence level. Higher confidence level data has a flatter backscatter far away from clouds and a much sharper increase near clouds (within 4 km), thus a smaller transition zone. For high confidence level data it is shown that the overall backscatter enhancement is more pronounced for small clear-air segments and horizontally larger clouds. The results suggest that data selection based on CAD reduces the possible effects of cloud contamination when studying aerosol properties in the vicinity of clouds.

Soot modeling of counterflow diffusion flames of ethylene-based binary mixture fuels

KAUST Repository

Wang, Yu

2015-03-01

A soot model was developed based on the recently proposed PAH growth mechanism for C1-C4 gaseous fuels (KAUST PAH Mechanism 2, KM2) that included molecular growth up to coronene (A7) to simulate soot formation in counterflow diffusion flames of ethylene and its binary mixtures with methane, ethane and propane based on the method of moments. The soot model has 36 soot nucleation reactions from 8 PAH molecules including pyrene and larger PAHs. Soot surface growth reactions were based on a modified hydrogen-abstraction-acetylene-addition (HACA) mechanism in which CH3, C3H3 and C2H radicals were included in the hydrogen abstraction reactions in addition to H atoms. PAH condensation on soot particles was also considered. The experimentally measured profiles of soot volume fraction, number density, and particle size were well captured by the model for the baseline case of ethylene along with the cases involving mixtures of fuels. The simulation results, which were in qualitative agreement with the experimental data in the effects of binary fuel mixing on the sooting structures of the measured flames, showed in particular that 5% addition of propane (ethane) led to an increase in the soot volume fraction of the ethylene flame by 32% (6%), despite the fact that propane and ethane are less sooting fuels than is ethylene, which is in reasonable agreement with experiments of 37% (14%). The model revealed that with 5% addition of methane, there was an increase of 6% in the soot volume fraction. The average soot particle sizes were only minimally influenced while the soot number densities were increased by the fuel mixing. Further analysis of the numerical data indicated that the chemical cross-linking effect between ethylene and the dopant fuels resulted in an increase in PAH formation, which led to higher soot nucleation rates and therefore higher soot number densities. On the other hand, the rates of soot surface growth per unit surface area through the HACA mechanism were

Modeling organic aerosol concentrations and properties during winter 2014 in the northwestern Mediterranean region

OpenAIRE

Chrit, Mounir; Sartelet, Karine; Sciare, Jean; Majdi, Marwa; Nicolas, José; Petit, Jean-Eudes; Dulac, François

2018-01-01

Organic aerosols are measured at a remote site (Ersa) on Corsica Cape in the northwestern Mediterranean basin during the Chemistry-Aerosol Mediterranean Experiment (CharMEx) winter campaign of 2014, when high organic concentrations from anthropogenic origin are observed. This work aims at representing the observed organic aerosol concentrations and properties (oxidation state) using the air-quality model Polyphemus with a surrogate approach for secondary organic aerosol (SOA) formation. Becau...

Chemical and microphysical properties of the aerosol during foggy and nonfoggy episodes: a relationship between organic and inorganic content of the aerosol

Science.gov (United States)

Kaul, D. S.; Gupta, T.; Tripathi, S. N.

2012-06-01

An extensive field measurement during winter was carried out at a site located in the Indo-Gangetic Plain (IGP) which gets heavily influenced by the fog during winter almost every year. The chemical and microphysical properties of the aerosols during foggy and nonfoggy episodes and chemical composition of the fogwater are presented. Positive matrix factorization (PMF) as a tool for the source apportionment was employed to understand the sources of pollution. Four major sources viz. biomass burning, refractory, secondary and mineral dust were identified. Aerosols properties during foggy episodes were heavily influenced by almost all the sources and they caused considerable loading of almost all the organic and inorganic species during the period. The biomass generated aerosols were removed from the atmosphere by scavenging during foggy episodes. The wet removal of almost all the species by the fog droplets was observed. The K+, water soluble organic carbon (WSOC), water soluble inorganic carbon (WSIC) and NO3- were most heavily scavenged among the species and their concentrations consequently became lower than the nonfoggy episode concentrations. The production of secondary inorganic aerosol, mainly sulfate and ammonium, during foggy episodes was considerably higher than nitrate which was rather heavily scavenged and removed by the fog droplets. The fogwater analysis showed that dissolved inorganic species play a vital role in processing of organic carbon such as the formation of organo-sulfate and organo-nitrate inside the fog droplets. The formation of organo-sulfate and organo-nitrate in aerosol and the influence of acidity on the secondary organic aerosol (SOA) formation were rather found to be negligible. The study average inorganic component of the aerosol was considerably higher than the carbonaceous component during both foggy and nonfoggy episode. The secondary production of the aerosol changed the microphysical properties of aerosol which was reflected by

Characterization and reactivity of soot from fast pyrolysis of lignocellulosic compounds and monolignols

DEFF Research Database (Denmark)

Trubetskaya, Anna; Brown, Avery; Tompsett, Geoffrey

2018-01-01

spectroscopy. The CO2 reactivity of soot was investigated by thermogravimetric analysis. Soot from cellulose was more reactive than soot produced from extractives, lignin and monolignols. Soot reactivity was correlated with the separation distances between adjacent graphene layers, as measured using...... transmission electron microscopy. Particle size, free radical concentration, differences in a degree of curvature and multi-core structures influenced the soot reactivity less than the interlayer separation distances. Soot yield was correlated with the lignin content of the feedstock. The selection...... of the extraction solvent had a strong influence on the soot reactivity. The Soxhlet extraction of softwood and wheat straw lignin soot using methanol decreased the soot reactivity, whereas acetone extraction had only a modest effect....

Use of the NASA GEOS-5 SEAC4RS Meteorological and Aerosol Reanalysis for assessing simulated aerosol optical properties as a function of smoke age

Science.gov (United States)

Randles, C. A.; da Silva, A. M., Jr.; Colarco, P. R.; Darmenov, A.; Buchard, V.; Govindaraju, R.; Chen, G.; Hair, J. W.; Russell, P. B.; Shinozuka, Y.; Wagner, N.; Lack, D.

2014-12-01

The NASA Goddard Earth Observing System version 5 (GEOS-5) Earth system model, which includes an online aerosol module, provided chemical and weather forecasts during the SEAC4RS field campaign. For post-mission analysis, we have produced a high resolution (25 km) meteorological and aerosol reanalysis for the entire campaign period. In addition to the full meteorological observing system used for routine NWP, we assimilate 550 nm aerosol optical depth (AOD) derived from MODIS (both Aqua and Terra satellites), ground-based AERONET sun photometers, and the MISR instrument (over bright surfaces only). Daily biomass burning emissions of CO, CO2, SO2, and aerosols are derived from MODIS fire radiative power retrievals. We have also introduced novel smoke "age" tracers, which provide, for a given time, a snapshot histogram of the age of simulated smoke aerosol. Because GEOS-5 assimilates remotely sensed AOD data, it generally reproduces observed (column) AOD compared to, for example, the airborne 4-STAR instrument. Constraining AOD, however, does not imply a good representation of either the vertical profile or the aerosol microphysical properties (e.g., composition, absorption). We do find a reasonable vertical structure for aerosols is attained in the model, provided actual smoke injection heights are not much above the planetary boundary layer, as verified with observations from DIAL/HRSL aboard the DC8. The translation of the simulated aerosol microphysical properties to total column AOD, needed in the aerosol assimilation step, is based on prescribed mass extinction efficiencies that depend on wavelength, composition, and relative humidity. Here we also evaluate the performance of the simulated aerosol speciation by examining in situ retrievals of aerosol absorption/single scattering albedo and scattering growth factor (f(RH)) from the LARGE and AOP suite of instruments. Putting these comparisons in the context of smoke age as diagnosed by the model helps us to

Reductions of PAH and Soot by Center Air Injection

Directory of Open Access Journals (Sweden)

Kazuhiro Yamamoto

2014-07-01

Full Text Available In this study, to reduce the amount of pollutant PAH and soot in the flame, we examined the burner system equipped with a center air injection. For this purpose, by using PAH-LIF and soot LII, we evaluated relative PAH and soot amounts in both the triple port burner and the conventional co-axial burner (double port burner to discuss effects of center air injection on the formation of PAH and soot. The fuel was propane. In the triple port burner, two different blue flames are observed near the burner rim, followed by bright luminous flames with soot. The flame length is longer when the fuel flow velocity is increased. On the other hand, the flame length is shorter with an increase in internal air flow velocity. As for PAH and soot, these amounts of the triple port burner are much smaller than those of the double port burner. For the triple port burner, due to the center air injection, the fuel consumption occurs in both inner and outer flames. On the other hand, for the double port burner, the oxygen is supplied from one side air, and as a result, the fuel consumption rate is relatively lower. Hence, by the center air injection, the fuel consumption is largely accelerated, resulting in the reduction of PAH and soot.

Understanding and predicting soot generation in turbulent non-premixed jet flames.

Energy Technology Data Exchange (ETDEWEB)

Wang, Hai (University of Southern California, Los Angeles, CA); Kook, Sanghoon; Doom, Jeffrey; Oefelein, Joseph Charles; Zhang, Jiayao; Shaddix, Christopher R.; Schefer, Robert W.; Pickett, Lyle M.

2010-10-01

This report documents the results of a project funded by DoD's Strategic Environmental Research and Development Program (SERDP) on the science behind development of predictive models for soot emission from gas turbine engines. Measurements of soot formation were performed in laminar flat premixed flames and turbulent non-premixed jet flames at 1 atm pressure and in turbulent liquid spray flames under representative conditions for takeoff in a gas turbine engine. The laminar flames and open jet flames used both ethylene and a prevaporized JP-8 surrogate fuel composed of n-dodecane and m-xylene. The pressurized turbulent jet flame measurements used the JP-8 surrogate fuel and compared its combustion and sooting characteristics to a world-average JP-8 fuel sample. The pressurized jet flame measurements demonstrated that the surrogate was representative of JP-8, with a somewhat higher tendency to soot formation. The premixed flame measurements revealed that flame temperature has a strong impact on the rate of soot nucleation and particle coagulation, but little sensitivity in the overall trends was found with different fuels. An extensive array of non-intrusive optical and laser-based measurements was performed in turbulent non-premixed jet flames established on specially designed piloted burners. Soot concentration data was collected throughout the flames, together with instantaneous images showing the relationship between soot and the OH radical and soot and PAH. A detailed chemical kinetic mechanism for ethylene combustion, including fuel-rich chemistry and benzene formation steps, was compiled, validated, and reduced. The reduced ethylene mechanism was incorporated into a high-fidelity LES code, together with a moment-based soot model and models for thermal radiation, to evaluate the ability of the chemistry and soot models to predict soot formation in the jet diffusion flame. The LES results highlight the importance of including an optically-thick radiation

Numerical Investigation of Soot Formation in Non-premixed Flames

KAUST Repository

Abdelgadir, Ahmed Gamaleldin

2017-05-01

Soot is a carbon particulate formed as a result of the combustion of fossil fuels. Due to the health hazard posed by the carbon particulate, government agencies have applied strict regulations to control soot emissions from road vehicles, airplanes, and industrial plants. Thus, understanding soot formation and evolution is critical. Practical combustion devices operate at high pressure and in the turbulent regime. Elevated pressures and turbulence on soot formation significantly and fundamental understanding of these complex interactions is still poor. In this study, the effects of pressure and turbulence on soot formation and growth are investigated numerically. As the first step, the evolution of the particle size distribution function (PSDF) and soot particles morphology are investigated in turbulent non-premixed flames. A Direct Simulation Monte Carlo (DSMC) code is developed and used. The stochastic reactor describes the evolution of soot in fluid parcels following Lagrangian trajectories in a turbulent flow field. The trajectories are sampled from a Direct Numerical Simulation (DNS) of an n-heptane turbulent non-premixed flame. Although individual trajectories display strong bimodality as in laminar flames, the ensemble-average PSDF possesses only one mode and a broad tail, which implies significant polydispersity induced by turbulence. Secondly, the effect of the flow and mixing fields on soot formation at atmospheric and elevated pressures is investigated in coflow laminar diffusion flames. The experimental observation and the numerical prediction of the spatial distribution are in good agreement. Based on the common scaling methodology of the flames (keeping the Reynolds number constant), the scalar dissipation rate decreases as pressure increases, promoting the formation of PAH species and soot. The decrease of the scalar dissipation rate significantly contributes to soot formation occurring closer to the nozzle and outward on the flames wings as pressure

Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

Science.gov (United States)

Logan, Timothy S.

Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the

Soot emissions from turbulent diffusion flames burning simple alkane fuels

Energy Technology Data Exchange (ETDEWEB)

Canteenwalla, P.M.; Johnson, M.R. [Carleton Univ., Ottawa, ON (Canada). Dept. of Mechanical and Aerospace Engineering; Thomson, K.A.; Smallwood, G.J. [National Research Council of Canada, Ottawa, ON (Canada). Inst. for Chemical Process and Environmental Technology

2007-07-01

A classic problem in combustion involves measurement and prediction of soot emissions from turbulent diffusion flames. Very high-sensitivity measurements of particulate matter (PM) from very low-sooting diffusion flames burning methane and other simple alkane fuels have been enabled from recent advances in laser-induced incandescence (LII). In order to quantify soot emissions from a lab-scale turbulent diffusion flame burner, this paper presented a study that used LII to develop a sampling protocol. The purpose of the study was to develop an experimentally based model to predict PM emissions from flares used in industry using soot emissions from lab-scale flares. Quantitative results of mass of soot emitted per mass of fuel burned were presented across a range of flow conditions and fuels. The experiment used digital imaging to measure flame lengths and estimate flame residence times. Comparisons were also made between current measurements and results of previous researchers for soot in the overfire region. The study also considered the validity applicability of buoyancy based models for predicting and scaling soot emissions. The paper described the experimental setup including sampling system and flame length imaging. Background information on soot yield and a comparison of flame residence time definitions were provided. The results and discussion of results were also presented. It was concluded that the results highlighted the subjective nature of flame length measurements. 10 refs., 4 figs.

Potassium and soot interaction in fast biomass pyrolysis at high temperatures

DEFF Research Database (Denmark)

Trubetskaya, Anna; Hofmann Larsen, Flemming; Shchukarev, Andrey

2018-01-01

2 reactivity was studied by thermogravimetric analysis. The XPS results showed that potassium incorporation with oxygen-containing surface groups in the soot matrix did not occur during high temperature pyrolysis. The potassium was mostly found as water-soluble salts such as KCl, KOH, KHCO3 and K2CO...... potassium amount was incorporated in the soot matrix during pyrolysis. Raman spectroscopy results showed that the carbon chemistry of biomass soot also affected the CO2 reactivity. The less reactive pinewood soot was more graphitic than herbaceous biomass soot samples with the disordered carbon structure...

Compositional effects on PAH and soot formation in counterflow diffusion flames of gasoline surrogate fuels

KAUST Repository

Park, Sungwoo

2017-02-05

Gasoline surrogate fuels are widely used to understand the fundamental combustion properties of complex refinery gasoline fuels. In this study, the compositional effects on polycyclic aromatic hydrocarbons (PAHs) and soot formation were investigated experimentally for gasoline surrogate mixtures comprising n-heptane, iso-octane, and toluene in counterflow diffusion flames. A comprehensive kinetic model for the gasoline surrogate mixtures was developed to accurately predict the fuel oxidation along with the formation of PAHs and soot in flames. This combined model was first tested against ignition delay times and laminar burning velocities data. The proposed model for the formation and growth of PAHs up to coronene (C24H12) was based on previous studies and was tested against existing and present new experimental data. Additionally, in the accompanied soot model, PAHs with sizes larger than (including) pyrene were used for the inception of soot particles, followed by particle coagulations and PAH condensation/chemical reactions on soot surfaces. The major pathways for the formation of PAHs were also identified for the surrogate mixtures. The model accurately captures the synergistic PAH formation characteristics observed experimentally for n-heptane/toluene and iso-octane/toluene binary mixtures. Furthermore, the present experimental and modeling results also elucidated different trends in the formation of larger PAHs and soot between binary n-heptane/iso-octane and ternary n-heptane/iso-octane/toluene mixtures. Propargyl radicals (C3H3) were shown to be important in the formation and growth of PAHs for n-heptane/iso-octane mixtures when the iso-octane concentration increased; however, reactions involving benzyl radicals (C6H5CH2) played a significant role in the formation of PAHs for n-heptane/iso-octane/toluene mixtures. These results indicated that the formation of PAHs and subsequently soot was strongly affected by the composition of gasoline surrogate mixtures.

Compositional effects on PAH and soot formation in counterflow diffusion flames of gasoline surrogate fuels

KAUST Repository

Park, Sungwoo; Wang, Yu; Chung, Suk-Ho; Sarathy, Mani

2017-01-01

Gasoline surrogate fuels are widely used to understand the fundamental combustion properties of complex refinery gasoline fuels. In this study, the compositional effects on polycyclic aromatic hydrocarbons (PAHs) and soot formation were investigated experimentally for gasoline surrogate mixtures comprising n-heptane, iso-octane, and toluene in counterflow diffusion flames. A comprehensive kinetic model for the gasoline surrogate mixtures was developed to accurately predict the fuel oxidation along with the formation of PAHs and soot in flames. This combined model was first tested against ignition delay times and laminar burning velocities data. The proposed model for the formation and growth of PAHs up to coronene (C24H12) was based on previous studies and was tested against existing and present new experimental data. Additionally, in the accompanied soot model, PAHs with sizes larger than (including) pyrene were used for the inception of soot particles, followed by particle coagulations and PAH condensation/chemical reactions on soot surfaces. The major pathways for the formation of PAHs were also identified for the surrogate mixtures. The model accurately captures the synergistic PAH formation characteristics observed experimentally for n-heptane/toluene and iso-octane/toluene binary mixtures. Furthermore, the present experimental and modeling results also elucidated different trends in the formation of larger PAHs and soot between binary n-heptane/iso-octane and ternary n-heptane/iso-octane/toluene mixtures. Propargyl radicals (C3H3) were shown to be important in the formation and growth of PAHs for n-heptane/iso-octane mixtures when the iso-octane concentration increased; however, reactions involving benzyl radicals (C6H5CH2) played a significant role in the formation of PAHs for n-heptane/iso-octane/toluene mixtures. These results indicated that the formation of PAHs and subsequently soot was strongly affected by the composition of gasoline surrogate mixtures.

High-throughput approach to the catalytic combustion of diesel soot

Energy Technology Data Exchange (ETDEWEB)

Iojoiu, Eduard Emil; Bassou, Badr; Guilhaume, Nolven; Farrusseng, David; Desmartin-Chomel, Arnold; Bianchi, Daniel; Mirodatos, Claude [Institut de recherches sur la catalyse et l' environnement de Lyon IRCELYON, UMR5256 CNRS Universite Lyon 1, 2 avenue Albert Einstein, F-69626 Villeurbanne Cedex (France); Lombaert, Karine [Renault, Diesel Innovative Catalytic Materials, Direction de l' Ingenierie Materiaux, 1 Allee Cornuel, 91510 Lardy (France)

2008-08-30

A methodology for the evaluation of diesel soot oxidation catalysts by high-throughput (HT) screening was developed. The optimal experimental conditions (soot amount, catalyst/soot ratio, type of contact, composition and flow rate of gas reactants) ensuring a reliable and reproducible detection of light-off temperatures in a 16 parallel channels reactor were set up. The temperature profile measured in the catalyst/soot bed under TPO conditions when the exothermic combustion of soot takes place was shown to provide an accurate measurement of the ignition. Its reproducibility and relevance were checked. The results obtained with a reference noble metal free catalyst (La{sub 0.8}Cr{sub 0.8}Li{sub 0.2}O{sub 3} perovskite) agree very well with literature data. Qualitative mechanistic features could be derived from these experiments, stressing the likely limiting step of oxygen transfer from catalyst surface to soot particulates to ignite the soot combustion. Ceria material was shown to be more appropriate than perovskite one. From an HT screening of a large diverse library (over 100 mixed oxides catalysts) under optimized conditions, about 10 new formulations were found to perform better than selected noble metal free reference materials. (author)

Isothermal Kinetics of Catalyzed Air Oxidation of Diesel Soot

Directory of Open Access Journals (Sweden)

R. Prasad

2011-01-01

Full Text Available To comply with the stringent emission regulations on soot, diesel vehicles manufacturers more and more commonly use diesel particulate filters (DPF. These systems need to be regenerated periodically by burning soot that has been accumulated during the loading of the DPF. Design of the DPF requires rate of soot oxidation. This paper describes the kinetics of catalytic oxidation of diesel soot with air under isothermal conditions. Kinetics data were collected in a specially designed mini-semi-batch reactor. Under the high air flow rate assuming pseudo first order reaction the activation energy of soot oxidation was found to be, Ea = 160 kJ/ mol. ©2010 BCREC UNDIP. All rights reserved(Received: 14th June 2010, Revised: 18th July 2010, Accepted: 9th August 2010[How to Cite: R. Prasad, V.R. Bella. (2010. Isothermal Kinetics of Catalyzed Air Oxidation of Diesel Soot. Bulletin of Chemical Reaction Engineering and Catalysis, 5(2: 95-101. doi:10.9767/bcrec.5.2.796.95-101][DOI:http://dx.doi.org/10.9767/bcrec.5.2.796.95-101 || or local:  http://ejournal.undip.ac.id/index.php/bcrec/article/view/796]Cited by in: ACS 1 |

Investigations of Sooting Laminar Coflow Diffusion Flames at Elevated Pressures

KAUST Repository

Steinmetz, Scott A.

2016-12-01

Soot is a common byproduct of hydrocarbon based combustion systems. It poses a risk to human and environmental health, and can negatively or positively affect combustor performance. As a result, there is significant interest in understanding soot formation in order to better control it. More recently, the need to study soot formation in engine relevant conditions has become apparent. One engine relevant parameter that has had little focus is the ambient pressure. This body of work focuses on the formation of soot in elevated pressure environments, and a number of investigations are carried out with this purpose. Laminar coflow diffusion flames are used as steady, simple soot producers. First, a commonly studied flame configuration is further characterized. Coflow flames are frequently used for fundamental flame studies, particularly at elevated pressures. However, they are more susceptible to buoyancy induced instabilities at elevated pressures. The velocity of the coflow is known to have an effect on flame stability and soot formation, though these have not been characterized at elevated pressures. A series of flames are investigated covering a range of flowrates, pressures, and nozzle diameters. The stability limits of coflow flames in this range is investigated. Additionally, an alternative strategy for scaling these flames to elevated pressures is proposed. Finally, the effect of coflow rate on soot formation is evaluated. Identification of fundamental flames for coordinated research can facilitate our understanding of soot formation. The next study of this work focuses on adding soot concentration and particle size information to an existing fundamental flame dataset for the purpose of numerical model validation. Soot volume fraction and average particle diameters are successfully measured in nitrogen-diluted ethylene-air laminar coflow flames at pressures of 4, 8, 12, and 16 atm. An increase in particle size with pressure is found up to 12 atm, where particle

Characterizing Organic Aerosol Processes and Climatically Relevant Properties via Advanced and Integrated Analyses of Aerosol Mass Spectrometry Datasets from DOE Campaigns and ACRF Measurements. Final report for DE-SC0007178

Energy Technology Data Exchange (ETDEWEB)

Zhang, Qi [Univ. of California, Davis, CA (United States)

2017-05-21

Organic aerosols (OA) are an important but poorly characterized component of the earth’s climate system. Enormous complexities commonly associated with OA composition and life cycle processes have significantly complicated the simulation and quantification of aerosol effects. To unravel these complexities and improve understanding of the properties, sources, formation, evolution processes, and radiative properties of atmospheric OA, we propose to perform advanced and integrated analyses of multiple DOE aerosol mass spectrometry datasets, including two high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) datasets from intensive field campaigns on the aerosol life cycle and the Aerosol Chemical Speciation Monitor (ACSM) datasets from long-term routine measurement programs at ACRF sites. In this project, we will focus on 1) characterizing the chemical (i.e., composition, organic elemental ratios), physical (i.e., size distribution and volatility), and radiative (i.e., sub- and super-saturated growth) properties of organic aerosols, 2) examining the correlations of these properties with different source and process regimes (e.g., primary, secondary, urban, biogenic, biomass burning, marine, or mixtures), 3) quantifying the evolutions of these properties as a function of photochemical processing, 4) identifying and characterizing special cases for important processes such as SOA formation and new particle formation and growth, and 5) correlating size-resolved aerosol chemistry with measurements of radiative properties of aerosols to determine the climatically relevant properties of OA and characterize the relationship between these properties and processes of atmospheric aerosol organics. Our primary goal is to improve a process-level understanding of the life cycle of organic aerosols in the Earth’s atmosphere. We will also aim at bridging between observations and models via synthesizing and translating the results and insights generated from this

Intercomparison and closure calculations using measurements of aerosol species and optical properties during the Yosemite Aerosol Characterization Study

Science.gov (United States)

Malm, William C.; Day, Derek E.; Carrico, Christian; Kreidenweis, Sonia M.; Collett, Jeffrey L.; McMeeking, Gavin; Lee, Taehyoung; Carrillo, Jacqueline; Schichtel, Bret

2005-07-01

Physical and optical properties of inorganic aerosols have been extensively studied, but less is known about carbonaceous aerosols, especially as they relate to the non-urban settings such as our nation's national parks and wilderness areas. Therefore an aerosol characterization study was conceived and implemented at one national park that is highly impacted by carbonaceous aerosols, Yosemite. The primary objective of the study was to characterize the physical, chemical, and optical properties of a carbon-dominated aerosol, including the ratio of total organic matter weight to organic carbon, organic mass scattering efficiencies, and the hygroscopic characteristics of a carbon-laden ambient aerosol, while a secondary objective was to evaluate a variety of semi-continuous monitoring systems. Inorganic ions were characterized using 24-hour samples that were collected using the URG and Interagency Monitoring of Protected Visual Environments (IMPROVE) monitoring systems, the micro-orifice uniform deposit impactor (MOUDI) cascade impactor, as well as the semi-continuous particle-into-liquid sampler (PILS) technology. Likewise, carbonaceous material was collected over 24-hour periods using IMPROVE technology along with the thermal optical reflectance (TOR) analysis, while semi-continuous total carbon concentrations were measured using the Rupprecht and Patashnick (R&P) instrument. Dry aerosol number size distributions were measured using a differential mobility analyzer (DMA) and optical particle counter, scattering coefficients at near-ambient conditions were measured with nephelometers fitted with PM10 and PM2.5 inlets, and "dry" PM2.5 scattering was measured after passing ambient air through Perma Pure Nafion® dryers. In general, the 24-hour "bulk" measurements of various aerosol species compared more favorably with each other than with the semi-continuous data. Semi-continuous sulfate measurements correlated well with the 24-hour measurements, but were biased low by

Estimation of Optical Properties for HULIS Aerosols at Anmyeon Island, Korea

Directory of Open Access Journals (Sweden)

Ji Yi Lee

2017-07-01

Full Text Available In this study, the sensitivity of the optical properties of carbonaceous aerosols, especially humic-like substances (HULIS, are investigated based on a one-year measurement of ambient fine atmospheric particulate matter (PM2.5 at a Global Atmospheric Watch (GAW station in South Korea. The extinction, absorption coefficient, and radiative forcing (RF are calculated from the analysis data of water soluble (WSOC and insoluble (WISOC organic aerosols, elemental carbon (EC, and HULIS. The sensitivity of the optical properties on the variations of refractive index, hygroscopicity, and light absorption properties of HULIS as well as the polydispersity of organic aerosols are studied. The results showed that the seasonal absorption coefficient of HULIS varied from 0.09 to 11.64 Mm−1 and EC varied from 0.11 to 3.04 Mm−1 if the geometric mean diameter varied from 0.1 to 1.0 µm and the geometric standard deviation varied from 1.1 to 2.0, with the imaginary refractive index (IRI of HULIS varying from 0.006 to 0.3. Subsequently, this study shows that the RF of HULIS was larger than other constituents, which suggested that HULIS contributed significantly to radiative forcing.

Soot Formation in Laminar Premixed Methane/Oxygen Flames at Atmospheric Pressure

Science.gov (United States)

Xu, F.; Lin, K.-C.; Faeth, G. M.

1998-01-01

Flame structure and soot formation were studied within soot-containing laminar premixed mc1hane/oxygen flames at atmospheric pressure. The following measurements were made: soot volume fractions by laser extinction, soot temperatures by multiline emission, gas temperatures (where soot was absent) by corrected fine-wire thermocouples, soot structure by thermophoretic sampling and transmission electron microscope (TEM), major gas species concentrations by sampling and gas chromatography, and gas velocities by laser velocimetry. Present measurements of gas species concentrations were in reasonably good agreement with earlier measurements due to Ramer et al. as well as predictions based on the detailed mechanisms of Frenklach and co-workers and Leung and Lindstedt: the predictions also suggest that H atom concentrations are in local thermodynamic equilibrium throughout the soot formation region. Using this information, it was found that measured soot surface growth rates could be correlated successfully by predictions based on the hydrogen-abstraction/carbon-addition (HACA) mechanisms of both Frenklach and co-workers and Colket and Hall, extending an earlier assessment of these mechanisms for premixed ethylene/air flames to conditions having larger H/C ratios and acetylene concentrations. Measured primary soot particle nucleation rates were somewhat lower than the earlier observations for laminar premixed ethylene/air flames and were significantly lower than corresponding rates in laminar diffusion flames. for reasons that still must be explained.

Soot formation characteristics of gasoline surrogate fuels in counterflow diffusion flames

KAUST Repository

Choi, Byungchul

2011-01-01

The characteristics of polycyclic aromatic hydrocarbon (PAH) and soot for gasoline surrogate fuels have been investigated in counterflow diffusion flames by adopting laser-induced fluorescence (LIF) and laser-induced incandescence (LII) techniques for both soot formation and soot formation/oxidation flames. Tested fuels were three binary mixtures from the primary reference fuels of n-heptane, iso-octane, and toluene. The result showed that PAH and soot maintained near zero level for all mixtures of n-heptane/iso-octane case under present experimental conditions. For n-heptane/toluene and iso-octane/toluene mixtures, PAH initially increased and then decreased with the toluene ratio, exhibiting a synergistic effect. The soot formation increased monotonically with the toluene ratio, however the effect of toluene on soot formation was minimal for relatively small toluene ratios. These results implied that even though toluene had a dominant role in soot and PAH formations, small amount of toluene had a minimal effect on soot formation. Numerical simulations have also been conducted by adopting recently proposed two kinetic mechanisms. The synergistic behavior of aromatic rings was predicted similar to the experimental PAH measurement, however, the degree of the synergistic effect was over-predicted for the soot formation flame, indicating the need for refinements in the kinetic mechanisms. © 2010 Published by Elsevier Inc. on behalf of The Combustion Institute. All rights reserved.

Strain rate effect on sooting characteristics in laminar counterflow diffusion flames

KAUST Repository

Wang, Yu; Chung, Suk-Ho

2016-01-01

The effects of strain rate, oxygen enrichment and fuel type on the sooting characteristics of counterflow diffusion flames were studied. The sooting structures and relative PAH concentrations were measured with laser diagnostics. Detailed soot

Secondary sulfate is internally mixed with sea spray aerosol and organic aerosol in the winter Arctic

Science.gov (United States)

Kirpes, Rachel M.; Bondy, Amy L.; Bonanno, Daniel; Moffet, Ryan C.; Wang, Bingbing; Laskin, Alexander; Ault, Andrew P.; Pratt, Kerri A.

2018-03-01

Few measurements of aerosol chemical composition have been made during the winter-spring transition (following polar sunrise) to constrain Arctic aerosol-cloud-climate feedbacks. Herein, we report the first measurements of individual particle chemical composition near Utqiaġvik (Barrow), Alaska, in winter (seven sample days in January and February 2014). Individual particles were analyzed by computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM-EDX, 24 847 particles), Raman microspectroscopy (300 particles), and scanning transmission X-ray microscopy with near-edge X-ray absorption fine structure spectroscopy (STXM-NEXAFS, 290 particles). Sea spray aerosol (SSA) was observed in all samples, with fresh and aged SSA comprising 99 %, by number, of 2.5-7.5 µm diameter particles, 65-95 % from 0.5-2.5 µm, and 50-60 % from 0.1-0.5 µm, indicating SSA is the dominant contributor to accumulation and coarse-mode aerosol during the winter. The aged SSA particles were characterized by reduced chlorine content with 94 %, by number, internally mixed with secondary sulfate (39 %, by number, internally mixed with both nitrate and sulfate), indicative of multiphase aging reactions during transport. There was a large number fraction (40 % of 1.0-4.0 µm diameter particles) of aged SSA during periods when particles were transported from near Prudhoe Bay, consistent with pollutant emissions from the oil fields participating in atmospheric processing of aerosol particles. Organic carbon and sulfate particles were observed in all samples and comprised 40-50 %, by number, of 0.1-0.4 µm diameter particles, indicative of Arctic haze influence. Soot was internally mixed with organic and sulfate components. All sulfate was mixed with organic carbon or SSA particles. Therefore, aerosol sources in the Alaskan Arctic and resulting aerosol chemical mixing states need to be considered when predicting aerosol climate effects, particularly cloud

A closure study of aerosol optical properties at a regional background mountainous site in Eastern China

International Nuclear Information System (INIS)

Yuan, Liang; Yin, Yan; Xiao, Hui; Yu, Xingna; Hao, Jian; Chen, Kui

2016-01-01

There is a large uncertainty in evaluating the radiative forcing from aerosol–radiation and aerosol–cloud interactions due to the limited knowledge on aerosol properties. In-situ measurements of aerosol physical and chemical properties were carried out in 2012 at Mt. Huang (the Yellow Mountain), a continental background mountainous site in eastern China. An aerosol optical closure study was performed to verify the model outputs by using the measured aerosol optical properties, in which a spherical Mie model with assumptions of external and core–shell mixtures on the basis of a two-component optical aerosol model and high size-segregated element carbon (EC) ratio was applied. Although the spherical Mie model would underestimate the real scattering with increasing particle diameters, excellent agreement between the calculated and measured values was achieved with correlation coefficients above 0.98. Sensitivity experiments showed that the EC ratio had a negligible effect on the calculated scattering coefficient, but largely influenced the calculated absorption coefficient. The high size-segregated EC ratio averaged over the study period in the closure was enough to reconstruct the aerosol absorption coefficient in the Mie model, indicating EC size resolution was more important than time resolution in retrieving the absorption coefficient in the model. The uncertainties of calculated scattering and absorption coefficients due to the uncertainties of measurements and model assumptions yielded by a Monte Carlo simulation were ± 6% and ± 14% for external mixture and ± 9% and ± 31% for core–shell mixture, respectively. This study provided an insight into the inherent relationship between aerosol optical properties and physicochemical characteristics in eastern China, which could supplement the database of aerosol optical properties for background sites in eastern China and provide a method for regions with similar climate. - Highlights: • A spherical Mie

A closure study of aerosol optical properties at a regional background mountainous site in Eastern China

Energy Technology Data Exchange (ETDEWEB)

Yuan, Liang [Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Key Laboratory for Aerosol–Cloud–Precipitation of China Meteorological Administration, School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing 210044 (China); Yin, Yan, E-mail: yinyan@nuist.edu.cn [Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Key Laboratory for Aerosol–Cloud–Precipitation of China Meteorological Administration, School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing 210044 (China); Xiao, Hui [Key Laboratory for Aerosol–Cloud–Precipitation of China Meteorological Administration, School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing 210044 (China); Yu, Xingna [Collaborative Innovation Center on Forecast and Evaluation of Meteorological Disasters, Nanjing University of Information Science & Technology, Nanjing 210044 (China); Key Laboratory for Aerosol–Cloud–Precipitation of China Meteorological Administration, School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing 210044 (China); Hao, Jian; Chen, Kui [Key Laboratory for Aerosol–Cloud–Precipitation of China Meteorological Administration, School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing 210044 (China); and others

2016-04-15

There is a large uncertainty in evaluating the radiative forcing from aerosol–radiation and aerosol–cloud interactions due to the limited knowledge on aerosol properties. In-situ measurements of aerosol physical and chemical properties were carried out in 2012 at Mt. Huang (the Yellow Mountain), a continental background mountainous site in eastern China. An aerosol optical closure study was performed to verify the model outputs by using the measured aerosol optical properties, in which a spherical Mie model with assumptions of external and core–shell mixtures on the basis of a two-component optical aerosol model and high size-segregated element carbon (EC) ratio was applied. Although the spherical Mie model would underestimate the real scattering with increasing particle diameters, excellent agreement between the calculated and measured values was achieved with correlation coefficients above 0.98. Sensitivity experiments showed that the EC ratio had a negligible effect on the calculated scattering coefficient, but largely influenced the calculated absorption coefficient. The high size-segregated EC ratio averaged over the study period in the closure was enough to reconstruct the aerosol absorption coefficient in the Mie model, indicating EC size resolution was more important than time resolution in retrieving the absorption coefficient in the model. The uncertainties of calculated scattering and absorption coefficients due to the uncertainties of measurements and model assumptions yielded by a Monte Carlo simulation were ± 6% and ± 14% for external mixture and ± 9% and ± 31% for core–shell mixture, respectively. This study provided an insight into the inherent relationship between aerosol optical properties and physicochemical characteristics in eastern China, which could supplement the database of aerosol optical properties for background sites in eastern China and provide a method for regions with similar climate. - Highlights: • A spherical Mie

Use of Multiangle Satellite Observations to Retrieve Aerosol Properties and Ocean Color

Science.gov (United States)

Martonchik, John V.; Diner, David; Khan, Ralph

2005-01-01

A new technique is described for retrieving aerosol over ocean water and the associated ocean color using multiangle satellite observations. Unlike current satellite aerosol retrieval algorithms which only utilize observations at red wavelengths and longer, with the assumption that these wavelengths have a negligible ocean (water-leaving radiance), this new algorithm uses all available spectral bands and simultaneously retrieves both aerosol properties and the spectral ocean color. We show some results of case studies using MISR data, performed over different water conditions (coastal water, blooms, and open water).

Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols

Directory of Open Access Journals (Sweden)

M. O. Andreae

2006-01-01

Full Text Available Although the definition and measurement techniques for atmospheric 'black carbon' ('BC' or 'elemental carbon'' ('EC' have long been subjects of scientific controversy, the recent discovery of light-absorbing carbon that is not black ('brown carbon, Cbrown' makes it imperative to reassess and redefine the components that make up light-absorbing carbonaceous matter (LAC in the atmosphere. Evidence for the atmospheric presence of Cbrown comes from (1 spectral aerosol light absorption measurements near specific combustion sources, (2 observations of spectral properties of water extracts of continental aerosol, (3 laboratory studies indicating the formation of light-absorbing organic matter in the atmosphere, and (4 indirectly from the chemical analogy of aerosol species to colored natural humic substances. We show that brown carbon may severely bias measurements of 'BC' and 'EC' over vast parts of the troposphere, especially those strongly polluted by biomass burning, where the mass concentration of Cbrown is high relative to that of soot carbon. Chemical measurements to determine 'EC' are biased by the refractory nature of Cbrown as well as by complex matrix interferences. Optical measurements of 'BC' suffer from a number of problems: (1 many of the presently used instruments introduce a substantial bias into the determination of aerosol light absorption, (2 there is no unique conversion factor between light absorption and 'EC' or 'BC' concentration in ambient aerosols, and (3 the difference in spectral properties between the different types of LAC, as well as the chemical complexity of Cbrown, lead to several conceptual as well as practical complications. We also suggest that due to the sharply increasing absorption of Cbrown towards the UV, single-wavelength light absorption measurements may not be adequate for the assessment of absorption of solar radiation in the troposphere. We discuss the possible consequences of these effects for our

Effect of aircraft exhaust sulfur emissions on near field plume aerosols

Energy Technology Data Exchange (ETDEWEB)

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

Effect of aircraft exhaust sulfur emissions on near field plume aerosols

Energy Technology Data Exchange (ETDEWEB)

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

1998-12-31

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

Spectral Aerosol Extinction (SpEx): A New Instrument for In situ Ambient Aerosol Extinction Measurements Across the UV/Visible Wavelength Range

Science.gov (United States)

Jordan, C. E.; Anderson, B. E.; Beyersdorf, A. J.; Corr, C. A.; Dibb, J. E.; Greenslade, M. E.; Martin, R. F.; Moore, R. H.; Scheuer, E.; Shook, M. A.;

Cosmic: Carbon Monoxide And Soot In Microgravity Inverse Combustion

Science.gov (United States)

Mikofski, M. A.; Blevins, L. G.; Davis, R. W.; Moore, E. F.; Mulholland, G. W.; Sacksteder, Kurt (Technical Monitor)

2003-01-01

Almost seventy percent of fire related deaths are caused by the inhalation of toxins such as CO and soot that are produced when fires become underventilated.(1) Although studies have established the importance of CO formation during underventilated burning,(2) the formation processes of CO (and soot) in underventilated fires are not well understood. The goal of the COSMIC project is to study the formation processes of CO and soot in underventilated flames. A potential way to study CO and soot production in underventilated flames is the use of inverse diffusion flames (IDFs). An IDF forms between a central air jet and a surrounding fuel jet. IDFs are related to underventilated flames because they may allow CO and soot to escape unoxidized. Experiments and numerical simulations of laminar IDFs of CH4 and C2H4 were conducted in 1-g and micro-g to study CO and soot formation. Laminar flames were studied because turbulent models of underventilated fires are uncertain. Microgravity was used to alter CO and soot pathways. A IDF literature survey, providing background and establishing motivation for this research, was presented at the 5th IWMC.(3) Experimental results from 1-g C2H4 IDFs and comparisons with simulations, demonstrating similarities between IDFs and underventilated fires, were presented at the 6th IWMC.(4) This paper will present experimental results from micro-g and 1-g IDFs of CH4 and C2H4 as well as comparisons with simulations, further supporting the relation between IDFs and underventilated flames.

Investigation of soot morphology and particle size distrib ution in a turbulent nonpremixed flame via Monte Carlo simulations

KAUST Repository

Abdelgadir, Ahmed

2015-03-30

Recently, our group performed a set of direct numerical simulations (DNS) of soot formation and growth in a n-heptane three dimensional non-premixed jet flame [Attili et al., Proc. Comb. Inst, 35, 2015], [Attili et al., Comb. Flame, 161, 2014], [Bisetti et al.,Trans of the Royal Soc, 372, 2014]. The evolution of species relevant to soot formation and growth have been sampled along a large number of Lagrangian trajectories in the DNS. In this work, the DNS results are post-processed to compute the soot evolution along selected Lagrangian trajectories using a Monte Carlo method. An operator splitting approach is adopted to split the deterministic processes (nucleation, surface growth and oxidation) from coagulation, which is treated stochastically. The morphological properties of soot and the particlesize distribution are investigated. For trajectories that experience an early strong nucleation event, the particle size distribution is found to be bimodal, as the soot particles have enough time to coagulate and grow while it is unimodal for trajectories characterized by only late nucleation events. As a results, the average size distribution at two different crosswise positions in the flame is unimodal.

Sensitivity of the Single Particle Soot Photometer to different black carbon types

Science.gov (United States)

Laborde, M.; Mertes, P.; Zieger, P.; Dommen, J.; Baltensperger, U.; Gysel, M.

2012-05-01

Black carbon (BC) is now mainly of anthropogenic origin. It is the dominant light absorbing component of atmospheric aerosols, playing an important role in the earth's radiative balance and therefore relevant to climate change studies. In addition, BC is known to be harmful to human beings making it relevant to policy makers. Nevertheless, the measurement of BC remains biased by the instrument-based definition of BC. The Single Particle Soot Photometer (SP2), allows the measurement of the refractory BC (rBC) mass of individual particles using laser-induced incandescence. However, the SP2 needs an empirical calibration to retrieve the rBC mass from the incandescence signal and the sensitivity of the SP2 differs between different BC types. Ideally, for atmospheric studies, the SP2 should be calibrated using ambient particles containing a known mass of ambient rBC. However, such "ambient BC" calibration particles cannot easily be obtained and thus commercially available BC particles are commonly used for SP2 calibration instead. In this study we tested the sensitivity of the SP2 to different BC types in order to characterize the potential error introduced by using non-ambient BC for calibration. The sensitivity of the SP2 was determined, using an aerosol particle mass analyzer, for rBC from thermodenuded diesel exhaust, wood burning exhaust and ambient particles as well as for commercially available products: Aquadag® and fullerene soot. Thermodenuded, fresh diesel exhaust has been found to be ideal for SP2 calibration for two reasons. First, the small amount of non-BC matter upon emission reduces the risk of bias due to incomplete removal of non-BC matter and second, it is considered to represent atmospheric rBC in urban locations where diesel exhaust is the main source of BC. The SP2 was found to be up to 16% less sensitive to rBC from thermodenuded ambient particles (≤15 fg) than rBC from diesel exhaust, however, at least part of this difference can be explained

Sensitivity of the Single Particle Soot Photometer to different black carbon types

Directory of Open Access Journals (Sweden)

M. Laborde

2012-05-01

Full Text Available Black carbon (BC is now mainly of anthropogenic origin. It is the dominant light absorbing component of atmospheric aerosols, playing an important role in the earth's radiative balance and therefore relevant to climate change studies. In addition, BC is known to be harmful to human beings making it relevant to policy makers. Nevertheless, the measurement of BC remains biased by the instrument-based definition of BC. The Single Particle Soot Photometer (SP2, allows the measurement of the refractory BC (rBC mass of individual particles using laser-induced incandescence. However, the SP2 needs an empirical calibration to retrieve the rBC mass from the incandescence signal and the sensitivity of the SP2 differs between different BC types. Ideally, for atmospheric studies, the SP2 should be calibrated using ambient particles containing a known mass of ambient rBC. However, such "ambient BC" calibration particles cannot easily be obtained and thus commercially available BC particles are commonly used for SP2 calibration instead. In this study we tested the sensitivity of the SP2 to different BC types in order to characterize the potential error introduced by using non-ambient BC for calibration. The sensitivity of the SP2 was determined, using an aerosol particle mass analyzer, for rBC from thermodenuded diesel exhaust, wood burning exhaust and ambient particles as well as for commercially available products: Aquadag^® and fullerene soot.

Thermodenuded, fresh diesel exhaust has been found to be ideal for SP2 calibration for two reasons. First, the small amount of non-BC matter upon emission reduces the risk of bias due to incomplete removal of non-BC matter and second, it is considered to represent atmospheric rBC in urban locations where diesel exhaust is the main source of BC. The SP2 was found to be up to 16% less sensitive to rBC from thermodenuded ambient particles (≤15 fg than rBC from diesel exhaust, however, at least part

Cloud forming properties of ambient aerosol in the Netherlands and resultant shortwave radiative forcing of climate

NARCIS (Netherlands)

Khlystov, A.

1998-01-01

This thesis discusses properties of ambient aerosols in the Netherlands which are controlling the magnitude of the local aerosol radiative forcing. Anthropogenic aerosols influence climate by changing the radiative transfer through the atmosphere via two effects, one is direct and a second

Single Particle Soot Photometer intercomparison at the AIDA chamber

Directory of Open Access Journals (Sweden)

M. Laborde

2012-12-01

Full Text Available Soot particles, consisting of black carbon (BC, organic carbon (OC, inorganic salts, and trace elements, are emitted into the atmosphere during incomplete combustion. Accurate measurements of atmospheric BC are important as BC particles cause adverse health effects and impact the climate.

Unfortunately, the accurate measurement of the properties and mass concentrations of BC particles remains difficult. The Single Particle Soot Photometer (SP2 can contribute to improving this situation by measuring the mass of refractory BC in individual particles as well as its mixing state.

Here, the results of the first detailed SP2 intercomparison, involving 6 SP2s from 6 different research groups, are presented, including the most evolved data products that can presently be calculated from SP2 measurements.

It was shown that a detection efficiency of almost 100% down to 1 fg BC per particle can readily be achieved, and that this limit can be pushed down to ∼0.2 fg BC with optimal SP2 setup. Number and mass size distributions of BC cores agreed within ±5% and ±10%, respectively, in between the SP2s, with larger deviations in the range below 1 fg BC.

The accuracy of the SP2's mass concentration measurement depends on the calibration material chosen. The SP2 has previously been shown to be equally sensitive to fullerene soot and ambient BC from sources where fossil fuel was dominant and less sensitive to fullerene soot than to Aquadag. Fullerene soot was therefore chosen as the standard calibration material by the SP2 user community; however, many data sets rely solely on Aquadag calibration measurements. The difference in SP2 sensitivity was found to be almost equal (fullerene soot to Aquadag response ratio of ∼0.75 at 8.9 fg BC for all SP2s. This allows the calculation of a fullerene soot equivalent calibration curve from a measured Aquadag calibration, when no fullerene soot calibration is available. It could be

Diesel soot oxidation under controlled conditions

OpenAIRE

Song, Haiwen

2003-01-01

This thesis was submitted for the degree of Doctor of Philosophy and awarded by Brunel University, 11/12/2003. In order to improve understanding of diesel soot oxidation, an experimental rig was designed and set up, in which the soot oxidation conditions, such as temperature, oxygen partial pressure, and CO2 partial pressure, could be varied independently of each other. The oxidizing gas flow in the oxidizer was under laminar condition. This test rig comprised a naturally-aspirated single ...

Comprehensive Laser-induced Incandescence (LII) modeling for soot particle sizing

KAUST Repository

Lisanti, Joel

2015-03-30

To evaluate the current state of the art in LII particle sizing, a comprehensive model for predicting the temporal incandescent response of combustion-generated soot to absorption of a pulsed laser is presented. The model incorporates particle heating through laser absorption, thermal annealing, and oxidation at the surface as well as cooling through sublimation and photodesorption, radiation, conduction and thermionic emission. Thermodynamic properties and the thermal accommodation coefficient utilized in the model are temperature dependent. In addition, where appropriate properties are also phase dependent, thereby accounting for annealing effects during laser heating and particle cooling.

In situ airborne measurements of aerosol optical properties during photochemical pollution events

Science.gov (United States)

Mallet, M.; van Dingenen, R.; Roger, J. C.; Despiau, S.; Cachier, H.

2005-02-01

Dry aerosol optical properties (scattering, absorbing coefficients, and single scattering albedo) were derived from in situ airborne measurements during two photochemical pollution events (25 and 26 June) observed during the Experience sur Site pour Contraindre les Modeles de Pollution atmospherique et de Transport d'Emissions (ESCOMPTE) experiment. Two flights were carried out during daytime (one during the morning and one at noon) over a domain, allowing the investigation of how an air pollution event affects the particle optical properties. Both horizontal distribution and vertical profiles are presented. Results from the horizontal mapping show that plumes of enhanced scattering and absorption are formed in the planetary boundary layer (PBL) during the day in the sea breeze-driven outflow of the coastal urban-industrial area of Marseille-Fos de Berre. The domain-averaged scattering coefficient (at 550 nm) over land σs changes from 35 (28) Mm-1 during land breeze to 63 (43) Mm-1 during sea breeze on 25 June (26 June), with local maxima reaching > 100 Mm-1. The increase in the scattering coefficient is associated with new particle formation, indicative of secondary aerosol formation. Simultaneously, the domain-averaged absorption coefficient increases from 5.6 (3.4) Mm-1 to 9.3 (8.0) Mm-1. The pollution plume leads to strong gradients in the single scattering albedo ωo over the domain studied, with local values as low as 0.73 observed inside the pollution plume. The role of photochemistry and secondary aerosol formation during the 25 June case is shown to increase ωo and to make the aerosol more `reflecting' while the plume moves away from the sources. The lower photochemical activity, observed in the 26 June case, induces a relatively higher contribution of black carbon, making the aerosol more absorbing. Results from vertical profiles at a single near-urban location in the domain indicate that the changes in optical properties happen almost entirely within

Aerosol optical properties and direct radiative forcing at Taihu.

Science.gov (United States)

Lü, Rui; Yu, Xingna; Jia, Hailing; Xiao, Sihan

2017-09-01

Ground-based characteristics (optical, type, size, and radiative properties) of aerosols measured between 2005 and 2012 were investigated over the Taihu rim region, which encompasses the cities of Shanghai, Suzhou, Wuxi, and Changzhou. The aerosol optical depth (AOD) showed a distinct seasonal variation with the highest value in summer and the lowest AOD in winter. There was broadest frequency distribution with a multimodal structure in summer. The Ångström exponent (AE) showed high values during spring; the relative frequency of AE in the range of 0-0.8 was 5-10 times greater than that of other seasons. The samples with high AOD 440 and low AE 440-870 were mainly observed in spring, which is attributed to the relative abundance of coarse particles. The monthly aerosol volume size distributions presented a bimodal structure (fine and coarse modes). The coarse mode was dominant during spring, while the fine mode was predominant in other seasons. The main aerosol type over Taihu during all the seasons was the mixed small-particle category, followed by the urban/industrial category. The minimum single scattering albedo (SSA) occurred in winter, suggesting that atmosphere aerosol had a higher absorption. All monthly averaged asymmetry factors (ASY) had positive values and no distinct seasonal variation. Both high real (Re) and imaginary (Im) parts of the refractive index occurred in winter. The atmospheric warming effect of aerosol was more significant in winter compared with other seasons, with the averaged atmosphere aerosol radiative forcing (ARF) and the corresponding atmospheric heating rate up to +69.46  W·m -2 and 1.95  K·day -1 , respectively. There existed a significant positive correlation between AOD and ARF (absolute value), and the correlation coefficients (r) exceeded 0.86 in each season with maximum r in summer. Along with the increasing of the SSA, the aerosol radiative forcing efficiency (absolute value) showed a decreasing trend at the

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.

Empirical estimates of CCN from aerosol optical properties at four remote sites

Directory of Open Access Journals (Sweden)

A. Jefferson

2010-07-01

Full Text Available This study presents an empirical method to estimate the CCN concentration as a function of percent supersaturation. The aerosol optical properties, backscatter fraction and single scatter albedo, function as proxies for the aerosol size and composition in a power law relationship to CCN. This method is tested at four sites with aged aerosol: SGP (Oklahoma, USA, FKB (Black Forest, Germany, HFE (Hefei, China and GRW (Graciosa, Azores. Each site represents a different aerosol type and thus demonstrates the method robustness and limitations. Good agreement was found between the calculated and measured CCN with slopes between 0.81 and 1.03 and correlation coefficients (r² values between 0.59 and 0.67. The fit quality declined at low CCN concentrations.

Properties of aerosol floating in the air in a nuclear power plant workplace environment

International Nuclear Information System (INIS)

Karasawa, H.; Funabashi, M.; Ito, M.

1992-01-01

An investigation was carried out on properties of radioactive aerosol floating in the air at several workplaces in nuclear power plant. The principal results are as follows: the aerosol particle size distributions consisted of two particle groups, whose aerodynamic diameters ranged from 4 to 7 microns and from 0.4 to 0.6 microns; the radioactive aerosol particle size distribution were unimodal. The mean activity median aerodynamic diameter (AMAD) was 6 microns, with geometric standard deviation microns; and, the average density of the aerosol was about 2.2g/cm 3 . (author)

Visibility in the Netherlands during New Year's fireworks: The role of soot and salty aerosol products

Science.gov (United States)

ten Brink, Harry; Henzing, Bas; Otjes, René; Weijers, Ernie

2018-01-01

The visibility on New Year's nights in the Netherlands is low during stagnant weather. This is due to the scattering and absorption of light by the aerosol-smoke from the fireworks. We made an assessment of the responsible aerosol-species. The investigation took place during the New Year's night of 2009. Measurements were made at a regional site in the centre of the country away from specific local sources. An Integrating Nephelometer measured the light-scattering by the inherent compounds after removal of water from the aerosol by drying the air. The actual light-scattering was determined in an open-air scatterometer; it was a factor of five higher than the ;dry; value. The difference in actual and ;dry; light-scattering can only be explained by water-uptake of the salty hygroscopic components of the aerosol. This hypothesis is substantiated by measurements of the composition of the aerosol. The size-dependent concentrations of the salty ionic species were determined on-line with a MARGA-;sizer;. These components were for a large part in particles in the size range that most effectively scatter light. The ;dry; light-scattering was exerted by the inorganic salt components and the sooty carbonaceous material alike. However, the salty products from the fireworks are hygroscopic and take up water at the high relative humidities occurring that night. This explains the fivefold larger light-scattering by the wet ambient aerosol as compared to that by the dry aerosol in the integrating nephelometer. The visibility, which is the inverse of the open-air scattering, is thus indirectly governed by the salty products of the fireworks due to their uptake of water. Under stagnant weather conditions during New Year's nights in the Netherlands both the aerosol concentrations and the relative humidity are high; this implies that the ionic species govern the low visibilities in general, be it via their uptake of water.

Wintertime hygroscopicity and volatility of ambient urban aerosol particles

Directory of Open Access Journals (Sweden)

J. Enroth

2018-04-01

Full Text Available Hygroscopic and volatile properties of atmospheric aerosol particles with dry diameters of (20, 50, 75, 110 and 145 nm were determined in situ by using a volatility–hygroscopicity tandem differential mobility analyser (VH-TDMA system with a relative humidity of 90 % and denuding temperature of 270 °C in central Budapest during 2 months in winter 2014–2015. The probability density function of the hygroscopic growth factor (HGF showed a distinct bimodal distribution. One of the modes was characterised by an overall mean HGF of approximately 1.07 (this corresponds to a hygroscopicity parameter κ of 0.033 independently of the particle size and was assigned to nearly hydrophobic (NH particles. Its mean particle number fraction was large, and it decreased monotonically from 69 to 41 % with particle diameter. The other mode showed a mean HGF increasing slightly from 1.31 to 1.38 (κ values from 0.186 to 0.196 with particle diameter, and it was attributed to less hygroscopic (LH particles. The mode with more hygroscopic particles was not identified. The probability density function of the volatility GF (VGF also exhibited a distinct bimodal distribution with an overall mean VGF of approximately 0.96 independently of the particle size, and with another mean VGF increasing from 0.49 to 0.55 with particle diameter. The two modes were associated with less volatile (LV and volatile (V particles. The mean particle number fraction for the LV mode decreased from 34 to 21 % with particle diameter. The bimodal distributions indicated that the urban atmospheric aerosol contained an external mixture of particles with a diverse chemical composition. Particles corresponding to the NH and LV modes were assigned mainly to freshly emitted combustion particles, more specifically to vehicle emissions consisting of large mass fractions of soot likely coated with or containing some water-insoluble organic compounds such as non

The Measurement of Aerosol Optical Properties Using Continuous Wave Cavity Ring-Down Techniques

Science.gov (United States)

Strawa, A. W.; Owano, T.; Castaneda, R.; Baer, D. S.; Paldus, B. A.; Gore, Warren J. (Technical Monitor)

2002-01-01

Large uncertainties in the effects that aerosols have on climate require improved in-situ measurements of extinction coefficient and single-scattering albedo. This abstract describes the use of continuous wave cavity ring-down (CW-CRD) technology to address this problem. The innovations in this instrument are the use of CW-CRD to measure aerosol extinction coefficient, the simultaneous measurement of scattering coefficient, and small size suitable for a wide range of aircraft applications. Our prototype instrument measures extinction and scattering coefficient at 690 nm and extinction coefficient at 1550 nm. The instrument itself is small (60 x 48 x 15 cm) and relatively insensitive to vibrations. The prototype instrument has been tested in our lab and used in the field. While improvements in performance are needed, the prototype has been shown to make accurate and sensitive measurements of extinction and scattering coefficients. Combining these two parameters, one can obtain the single-scattering albedo and absorption coefficient, both important aerosol properties. The use of two wavelengths also allows us to obtain a quantitative idea of the size of the aerosol through the Angstrom exponent. Minimum sensitivity of the prototype instrument is 1.5 x 10(exp -6)/m (1.5/Mm). Validation of the measurement of extinction coefficient has been accomplished by comparing the measurement of calibration spheres with Mie calculations. This instrument and its successors have potential to help reduce uncertainty currently associated with aerosol optical properties and their spatial and temporal variation. Possible applications include studies of visibility, climate forcing by aerosol, and the validation of aerosol retrieval schemes from satellite data.

Phototransformation rate constants of PAHs associated with soot particles

International Nuclear Information System (INIS)

Kim, Daekyun; Young, Thomas M.; Anastasio, Cort

2013-01-01

Photodegradation is a key process governing the residence time and fate of polycyclic aromatic hydrocarbons (PAHs) in particles, both in the atmosphere and after deposition. We have measured photodegradation rate constants of PAHs in bulk deposits of soot particles illuminated with simulated sunlight. The photodegradation rate constants at the surface (k p 0 ), the effective diffusion coefficients (D eff ), and the light penetration depths (z 0.5 ) for PAHs on soot layers of variable thickness were determined by fitting experimental data with a model of coupled photolysis and diffusion. The overall disappearance rates of irradiated low molecular weight PAHs (with 2–3 rings) on soot particles were influenced by fast photodegradation and fast diffusion kinetics, while those of high molecular weight PAHs (with 4 or more rings) were apparently controlled by either the combination of slow photodegradation and slow diffusion kinetics or by very slow diffusion kinetics alone. The value of z 0.5 is more sensitive to the soot layer thickness than the k p 0 value. As the thickness of the soot layer increases, the z 0.5 values increase, but the k p 0 values are almost constant. The effective diffusion coefficients calculated from dark experiments are generally higher than those from the model fitting method for illumination experiments. Due to the correlation between k p 0 and z 0.5 in thinner layers, D eff should be estimated by an independent method for better accuracy. Despite some limitations of the model used in this study, the fitted parameters were useful for describing empirical results of photodegradation of soot-associated PAHs. - Highlights: ► PAHs on soot were evaluated by a model of coupled photolysis and diffusion. ► Photodegradation rate at the surface, diffusion coefficient, and light penetration path were determined. ► Low MW PAHs were influenced by fast photodegradation and fast diffusion. ► High MW PAHs were controlled either by slow

Beyond the Alphabet Soup: Molecular Properties of Aerosol Components Influence Optics. (Invited)

Science.gov (United States)

Thompson, J. E.

2013-12-01

Components within atmospheric aerosols exhibit almost every imaginable model of chemical bonding and physical diversity. The materials run the spectrum from crystalline to amorphous, covalent to ionic, and have varying viscosities, phase, and hygroscopicity. This seminar will focus on the molecular properties of materials that influence the optical behavior of aerosols. Special focus will be placed on the polarizability of materials, hygroscopic growth, and particle phase.

Analysis of CCN activity of Remote and Combustion Aerosol over the South East Pacific during autumn 2008 and links to Sc cloud properties

Science.gov (United States)

Freitag, S.; Clarke, A. D.; Howell, S. G.; Twohy, C. H.; Snider, J. R.; Toohey, D. W.; Shank, L.; McNaughton, C. S.; Brekhovskikh, V.; Kapustin, V.

2013-12-01

The earth's most extensive Stratocumulus (Sc) deck, situated off the coast of Northern Chile and Southern Peru, strongly influences the radiation budget and climate over the South East Pacific (SEP) by enhancing solar reflection. This feature makes Sc clouds an important constituent for climate modeling, yet these clouds are poorly represented in models. A large uncertainty in understanding the variability in these low cloud fields arises from our deficit in understanding the role of aerosol. Hence, a major goal of the VOCALS (www.eol.ucar.edu/projects/vocals) campaign in 2008 was to further explore and assess interactions of natural and anthropogenic aerosol with Sc clouds in both the more polluted coastal environment and west of 80W where we encountered nearly pristine boundary layer clouds often exposed to cloud-top entrainment of pollution aerosol from the free troposphere. Extensive airborne measurements of size-resolved aerosol volatility and chemical composition collected aboard the NCAR C-130 were analyzed with an aerosol mass spectrometer (AMS) and a single particle soot photometer (SP2) to calculate aerosol hygroscopicity (κ) and predict cloud condensation nuclei (CCN) concentration for all observed air mass types above and below cloud utilizing estimated Sc cloud supersaturations deduced from cloud-processed aerosol size distribution information. The predicted CCN agree to within 10% to measured CCN. Results from this analysis are presented here and CCN variability observed along VOCALS flight tracks is discussed in conjunction with size-resolved cloud droplet information. This includes assessing the impact of aerosol perturbations on the shape of the cloud droplet size distribution parameterized in models and satellite algorithms such as cloud top effective radius retrievals. We will further discuss cloud droplet residual composition collected using a counterflow virtual impactor (CVI) and analyzed with the AMS and SP2. Size resolved variations in

Connecting Organic Aerosol Climate-Relevant Properties to Chemical Mechanisms of Sources and Processing

Energy Technology Data Exchange (ETDEWEB)

Thornton, Joel [Univ. of Washington, Seattle, WA (United States)

2015-01-26

The research conducted on this project aimed to improve our understanding of secondary organic aerosol (SOA) formation in the atmosphere, and how the properties of the SOA impact climate through its size, phase state, and optical properties. The goal of this project was to demonstrate that the use of molecular composition information to mechanistically connect source apportionment and climate properties can improve the physical basis for simulation of SOA formation and properties in climate models. The research involved developing and improving methods to provide online measurements of the molecular composition of SOA under atmospherically relevant conditions and to apply this technology to controlled simulation chamber experiments and field measurements. The science we have completed with the methodology will impact the simulation of aerosol particles in climate models.

Experimental study of the interaction of HO2 radicals with soot surface.

Science.gov (United States)

Bedjanian, Yuri; Lelièvre, Stéphane; Le Bras, Georges

2005-01-21

The reaction of HO2 with toluene and kerosene flame soot was studied over the temperature range 240-350 K and at P = 0.5-5 Torr of helium using a discharge flow reactor coupled to a modulated molecular beam mass spectrometer. A flat-flame burner was used for the preparation and deposition of soot samples from premixed flames of liquid fuels under well controlled and adjustable combustion conditions. The independent of temperature in the range 240-350 K value of gamma = (7.5 +/- 1.5) x 10(-2) (calculated with geometric surface area) was found for the uptake coefficient of HO2 on kerosene and toluene soot. No significant deactivation of soot surface during its reaction with HO2 was observed. Experiments on soot ageing under ambient conditions showed that the reactivity of aged soot is similar to that of freshly prepared soot samples. The results show that the HO2 + soot reaction could be a significant loss process for HOx in the urban atmosphere with a potential impact on photochemical ozone formation. In contrast this process will be negligible in the upper troposphere even in flight corridors.

Fractal-like dimension of nanometer Diesel soot particles

Energy Technology Data Exchange (ETDEWEB)

Skillas, G.; Baltensperger, U. [Paul Scherrer Inst. (PSI), Villigen (Switzerland); Siegmann, K. [Eidgenoessische Technische Hochschule, Zurich (Switzerland)

1997-11-01

Measurements with a low-pressure impactor and a differential mobility analyser were conducted for Diesel soot at various engine loads. By means of these measurements a fractal-like dimension of Diesel soot particles, with diameters ranging from 55 up to 260 nm, was established. (author) 2 figs., 7 refs.

Long-term variability of aerosol optical properties and radiative effects in Northern Finland

Science.gov (United States)

Lihavainen, Heikki; Hyvärinen, Antti; Asmi, Eija; Hatakka, Juha; Viisanen, Yrjö

2017-04-01

We introduce long term dataset of aerosol scattering and absorption properties and combined aerosol optical properties measured in Pallas Atmosphere-Ecosystem Supersite in Norhern Finland. The station is located 170 km north of the Arctic Circle. The station is affected by both pristine Arctic air masses as well as long transported air pollution from northern Europe. We studied the optical properties of aerosols and their radiative effects in continental and marine air masses, including seasonal cycles and long-term trends. The average (median) scattering coefficient, backscattering fraction, absorption coefficient and single scattering albedo at the wavelength of 550 nm were 7.9 (4.4) 1/Mm, 0.13 (0.12), 0.74 (0.35) 1/Mm and 0.92 (0.93), respectively. We observed clear seasonal cycles in these variables, the scattering coefficient having high values during summer and low in fall, and absorption coefficient having high values during winter and low in fall. We found that the high values of the absorption coefficient and low values of the single scattering albedo were related to continental air masses from lower latitudes. These aerosols can induce an additional effect on the surface albedo and melting of snow. We observed the signal of the Arctic haze in marine (northern) air masses during March and April. The haze increased the value of the absorption coefficient by almost 80% and that of the scattering coefficient by about 50% compared with the annual-average values. We did not observe any long-term trend in the scattering coefficient, while our analysis showed a clear decreasing trend in the backscattering fraction and scattering Ångström exponent during winter. We also observed clear relationship with temperature and aerosol scattering coefficient. We will present also how these different features affects to aerosol direct radiative forcing.

Chemical Composition Based Aerosol Optical Properties According to Size Distribution and Mixture Types during Smog and Asian Dust Events in Seoul, Korea

Science.gov (United States)

Jung, Chang Hoon; Lee, Ji Yi; Um, Junshik; Lee, Seung Soo; Kim, Yong Pyo

2018-02-01

This study investigated the optical properties of aerosols involved in different meteorological events, including smog and Asian dust days. Carbonaceous components and inorganic species were measured in Seoul, Korea between 25 and 31 March 2012. Based on the measurements, the optical properties of aerosols were calculated by considering composition, size distribution, and mixing state of aerosols. To represent polydisperse size distributions of aerosols, a lognormal size distribution with a wide range of geometric mean diameters and geometric standard deviations was used. For the optical property calculations, the Mie theory was used to compute single-scattering properties of aerosol particles with varying size and composition. Analysis of the sampled data showed that the water-soluble components of organic matter increased on smog days, whereas crustal elements increased on dust days. The water content significantly influenced the optical properties of aerosols during the smog days as a result of high relative humidity and an increase in the water-soluble component. The absorption coefficients depended on the aerosol mixture type and the aerosol size distributions. Therefore, to improve our knowledge on radiative impacts of aerosols, especially the regional impacts of aerosols in East Asia, accurate measurements of aerosols, such as size distribution, composition, and mixture type, under different meteorological conditions are required.

AKTIS Nr. 12: To better understand radioactive aerosol deposit in order to better measure it; Radio-induced lesions: a new step towards healing; Modelling the collapse of an immersed grain column; To better model soot deposit; Towards the prediction of the leakage rate of containment enclosures

International Nuclear Information System (INIS)

Benderitter, Marc; Perales, Frederic; Monerie, Yann; Maro, Denis; Boyer, Patrick; Lemaitre, Pascal; Porcheron, Emmanuel; Depuydt, Guillaume; Masson, Olivier; Gensdarmes, Francois

2013-04-01

This publication presents the main results of researches undertaken by the IRSN in the field of radiation protection, nuclear safety and security. The topics herein addressed are: radio-induced lesions as a new step towards healing (case of injection mesenchymal stem cells for the treatment of induced severe colorectal lesions), the modelling of the collapse of an immersed grain column (to study the nuclear fuel behaviour in an accidental situation through a modelling of fluid-grain interactions), a better understanding of radioactive aerosol deposit (to study particle or aerosol deposits after radioactive releases in the atmosphere in case of accident), a better modelling of soot deposits (in case of fire), the prediction of leakage rates of containment enclosures (ageing phenomena of installations, systems and equipment, with the case of cracks due to material ageing and resulting in confinement losses which could thus be quantified)

Catalytic oxidation of soot over alkaline niobates

International Nuclear Information System (INIS)

Pecchi, G.; Cabrera, B.; Buljan, A.; Delgado, E.J.; Gordon, A.L.; Jimenez, R.

2013-01-01

Highlights: ► No previous reported studies about alkaline niobates as catalysts for soot oxidation. ► NaNbO 3 and KNbO 3 perovskite-type oxides show lower activation energy than other lanthanoid perovskite-type oxides. ► The alkaline niobate does not show deactivation by metal loss. - Abstract: The lack of studies in the current literature about the assessment of alkaline niobates as catalysts for soot oxidation has motivated this research. In this study, the synthesis, characterization and assessment of alkaline metal niobates as catalysts for soot combustion are reported. The solids MNbO 3 (M = Li, Na, K, Rb) are synthesized by a citrate method, calcined at 450 °C, 550 °C, 650 °C, 750 °C, and characterized by AAS, N 2 adsorption, XRD, O 2 -TPD, FTIR and SEM. All the alkaline niobates show catalytic activity for soot combustion, and the activity depends basically on the nature of the alkaline metal and the calcination temperature. The highest catalytic activity, expressed as the temperature at which combustion of carbon black occurs at the maximum rate, is shown by KNbO 3 calcined at 650 °C. At this calcination temperature, the catalytic activity follows an order dependent on the atomic number, namely: KNbO 3 > NaNbO 3 > LiNbO 3 . The RbNbO 3 solid do not follow this trend presumably due to the perovskite structure was not reached. The highest catalytic activity shown by of KNbO 3 , despite the lower apparent activation energy of NaNbO 3 , stress the importance of the metal nature and suggests the hypothesis that K + ions are the active sites for soot combustion. It must be pointed out that alkaline niobate subjected to consecutive soot combustion cycles does not show deactivation by metal loss, due to the stabilization of the alkaline metal inside the perovskite structure.

Analysis of aerosol absorption properties and transport over North Africa and the Middle East using AERONET data

Directory of Open Access Journals (Sweden)

A. Farahat

2016-11-01

Full Text Available In this paper particle categorization and absorption properties were discussed to understand transport mechanisms at different geographic locations and possible radiative impacts on climate. The long-term Aerosol Robotic Network (AERONET data set (1999–2015 is used to estimate aerosol optical depth (AOD, single scattering albedo (SSA, and the absorption Ångström exponent (αabs at eight locations in North Africa and the Middle East. Average variation in SSA is calculated at four wavelengths (440, 675, 870, and 1020 nm, and the relationship between aerosol absorption and physical properties is used to infer dominant aerosol types at different locations. It was found that seasonality and geographic location play a major role in identifying dominant aerosol types at each location. Analyzing aerosol characteristics among different sites using AERONET Version 2, Level 2.0 data retrievals and the Hybrid Single Particle Lagrangian Integrated Trajectory model (HYSPLIT backward trajectories shows possible aerosol particle transport among different locations indicating the importance of understanding transport mechanisms in identifying aerosol sources.

Effects of multiple scattering on radiative properties of soot fractal aggregates

International Nuclear Information System (INIS)

Yon, Jérôme; Liu, Fengshan; Bescond, Alexandre; Caumont-Prim, Chloé; Rozé, Claude; Ouf, François-Xavier; Coppalle, Alexis

2014-01-01

The in situ optical characterization of smokes composed of soot particles relies on light extinction, angular static light scattering (SLS), or laser induced incandescence (LII). These measurements are usually interpreted by using the Rayleigh–Debye–Gans theory for Fractal Aggregates (RDG-FA). RDG-FA is simple to use but it completely neglects the impact of multiple scattering (MS) within soot aggregates. In this paper, based on a scaling approach that takes into account MS effects, an extended form of the RDG-FA theory is proposed in order to take into account these effects. The parameters of this extended theory and their dependency on the number of primary sphere inside the aggregate (1 p <1006) and on the wavelength (266nm<λ<1064nm) are evaluated thanks to rigorous calculations based on discrete dipole approximation (DDA) and generalized multi-sphere Mie-solution (GMM) calculations. This study shows that size determination by SLS is not distorted by MS effect. On the contrary, it is shown that fractal dimension can be misinterpreted by light scattering experiments, especially at short wavelengths. MS effects should be taken into account for the interpretation of absorption measurements that are involved in LII or extinction measurements. -- Highlights: • We incorporate multiple scattering effects in a scaling approach for fractal aggregates. • A generalized structure factor is introduced for implementation in RDG-FA theory. • Forward scattering is affected by multiple scattering as well as power law regime. • Absorption cross sections are affected by multiple scattering. • Absorption cross sections are 11% higher than that for forward scattering

Analysis of intensive aerosol optical properties measured at the Jungfraujoch station

Energy Technology Data Exchange (ETDEWEB)

Li, F.; Nyeki, S.; Baltensperger, U.; Weingartner, E.; Lugauer, M. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

1997-09-01

Characterisation of atmospheric aerosol optical properties at the Jungfraujoch has been conducted to deliver basic data for comparison with those from NOAA baseline atmospheric monitoring stations. (author) 2 figs., 2 refs.

Molecular mechanics and quantum mechanical modeling of hexane soot structure and interactions with pyrene

Directory of Open Access Journals (Sweden)

Kubicki JD

2000-09-01

Full Text Available Molecular simulations (energy minimizations and molecular dynamics of an n-hexane soot model developed by Smith and co-workers (M. S. Akhter, A. R. Chughtai and D. M. Smith, Appl. Spectrosc., 1985, 39, 143; ref. 1 were performed. The MM+ (N. L. Allinger, J. Am. Chem. Soc., 1977, 395, 157; ref. 2 and COMPASS (H. Sun, J. Phys. Chem., 1998, 102, 7338; ref. 3 force fields were tested for their ability to produce realistic soot nanoparticle structure. The interaction of pyrene with the model soot was simulated. Quantum mechanical calculations on smaller soot fragments were carried out. Starting from an initial 2D structure, energy minimizations are not able to produce the observed layering within soot with either force field. Results of molecular dynamics simulations indicate that the COMPASS force field does a reasonably accurate job of reproducing observations of soot structure. Increasing the system size from a 683 to a 2732 atom soot model does not have a significant effect on predicted structures. Neither does the addition of water molecules surrounding the soot model. Pyrene fits within the soot structure without disrupting the interlayer spacing. Polycyclic aromatic hydrocarbons (PAH, such as pyrene, may strongly partition into soot and have slow desorption kinetics because the PAH-soot bonding is similar to soot–soot interactions. Diffusion of PAH into soot micropores may allow the PAH to be irreversibly adsorbed and sequestered so that they partition slowly back into an aqueous phase causing dis-equilibrium between soil organic matter and porewater.

Synergy of Satellite-Surface Observations for Studying the Properties of Absorbing Aerosols in Asia

Science.gov (United States)

Tsay, Si-Chee

2010-01-01

Through interaction with clouds and alteration of the Earth's radiation budget, atmospheric aerosols significantly influence our weather and climate. Monsoon rainfalls, for example, sustain the livelihood of more than half of the world's population. Thus, understanding the mechanism that drives the water cycle and freshwater distribution is high-lighted as one of the major near-term goals in NASA's Earth Science Enterprise Strategy. Every cloud droplet/ice-crystal that serves as an essential element in portraying water cycle and distributing freshwater contains atmospheric aerosols at its core. In addition, the spatial and temporal variability of atmospheric aerosol properties is complex due to their dynamic nature. In fact, the predictability of the tropical climate system is much reduced during the boreal spring, which is associated with the peak season of biomass burning activities and regional/long-range transport of dust aerosols. Therefore, to accurately assess the impact of absorbing aerosols on regional-to-global climate requires not only modeling efforts but also continuous observations from satellites, aircraft, networks of ground-based instruments and dedicated field experiments. Since 1997 NASA has been successfully launching a series of satellites the Earth Observing System - to intensively study, and gain a better understanding of, the Earth as an integrated system. Through participation in many satellite remote-sensing/retrieval and validation projects over the years, we have gradually developed and refined the SMART (Surface-sensing Measurements for Atmospheric Radiative Transfer) and COMMIT (Chemical, Optical & Microphysical Measurements of In-situ Troposphere) mobile observatories, a suite of surface remote sensing and in-situ instruments that proved to be vital in providing high temporal measurements, which complement the satellite observations. In this talk, we will present SMART-COMMIT which has played key roles, serving as network or supersite

Diurnal Cycles of Aerosol Optical Properties at Pico Tres Padres, Mexico City: Evidences for Changes in Particle Morphology and Secondary Aerosol Formation

Science.gov (United States)

Mazzoleni, C.; Dubey, M.; Chakrabarty, R.; Moosmuller, H.; Onasch, T.; Zavala, M.; Herndon, S.; Kolb, C.

2007-12-01

Aerosol optical properties affect planetary radiative balance and depend on chemical composition, size distribution, and morphology. During the MILAGRO field campaign, we measured aerosol absorption and scattering in Mexico City using the Los Alamos aerosol photoacoustic (LAPA) instrument operating at 781 nm. The LAPA was mounted on-board the Aerodyne Research Inc. mobile laboratory, which hosted a variety of gaseous and aerosol instruments. During the campaign, the laboratory was moved to different sites, capturing spatial and temporal variability. Additionally, we collected ambient aerosols on Nuclepore filters for scanning electron microscopy (SEM) analysis. SEM images of selected filters were taken to study particle morphology. Between March 7th and 19th air was sampled at the top of Pico Tres Padres, a mountain on the north side of Mexico City. Aerosol absorption and scattering followed diurnal patterns related to boundary layer height and solar insulation. We report an analysis of aerosol absorption, scattering, and morphology for three days (9th, 11th and 12th of March 2006). The single scattering albedo (SSA, ratio of scattering to total extinction) showed a drop in the tens-of-minutes-to-hour time frame after the boundary layer grew above the sampling site. Later in the day the SSA rose steadily reaching a maximum in the afternoon. The SEM images showed a variety of aerosol shapes including fractal-like aggregates, spherical particles, and other shapes. The absorption correlated with the CO2 signal and qualitatively with the fraction of fractal-like particles to the total particle count. In the afternoon the SSA qualitatively correlated with a relative increase in spherical particles and total particle count. These observed changes in optical properties and morphology can be explained by the dominant contribution of freshly emitted particles in the morning and by secondary particle formation in the afternoon. SSA hourly averaged values ranged from ~0.63 in

Evaluation of simulated aerosol properties with the aerosol-climate model ECHAM5-HAM using observations from the IMPACT field campaign

Directory of Open Access Journals (Sweden)

G.-J. Roelofs

2010-08-01

Full Text Available In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the associated aerosol optical thickness (AOT for the campaign period. Synoptic scale meteorology is represented realistically through nudging of the vorticity, the divergence, the temperature and the surface pressure. Simulated concentrations of aerosol sulfate and organics at the surface are generally within a factor of two from observed values. The monthly averaged AOT from the model is 0.33, about 20% larger than observed. For selected periods of the month with relatively dry and moist conditions discrepancies are approximately −30% and +15%, respectively. Discrepancies during the dry period are partly caused by inaccurate representation of boundary layer (BL dynamics by the model affecting the simulated AOT. The model simulates too strong exchange between the BL and the free troposphere, resulting in weaker concentration gradients at the BL top than observed for aerosol and humidity, while upward mixing from the surface layers into the BL appears to be underestimated. The results indicate that beside aerosol sulfate and organics also aerosol ammonium and nitrate significantly contribute to aerosol water uptake. The simulated day-to-day variability of AOT follows synoptic scale advection of humidity rather than particle concentration. Even for relatively dry conditions AOT appears to be strongly influenced by the diurnal cycle of RH in the lower boundary layer, further enhanced by uptake and release of nitric acid and ammonia by aerosol water.

Numerical Investigation of Soot Formation in Non-premixed Flames

KAUST Repository

Abdelgadir, Ahmed Gamaleldin

2017-01-01

Soot is a carbon particulate formed as a result of the combustion of fossil fuels. Due to the health hazard posed by the carbon particulate, government agencies have applied strict regulations to control soot emissions from road vehicles, airplanes

Modeling LIDAR Detection of Biological Aerosols to Determine Optimum Implementation Strategy

Energy Technology Data Exchange (ETDEWEB)

Sheen, David M.; Aker, Pam M.

2007-09-19

This report summarizes work performed for a larger multi-laboratory project named the Background Interferent Measurement and Standards project. While originally tasked to develop algorithms to optimize biological warfare agent detection using UV fluorescence LIDAR, the current uncertainties in the reported fluorescence profiles and cross sections the development of any meaningful models. It was decided that a better approach would be to model the wavelength-dependent elastic backscattering from a number of ambient background aerosol types, and compare this with that generated from representative sporulated and vegetative bacterial systems. Calculations in this report show that a 266, 355, 532 and 1064 nm elastic backscatter LIDAR experiment will allow an operator to immediately recognize when sulfate, VOC-based or road dust (silicate) aerosols are approaching, independent of humidity changes. It will be more difficult to distinguish soot aerosols from biological aerosols, or vegetative bacteria from sporulated bacteria. In these latter cases, the elastic scattering data will most likely have to be combined with UV fluorescence data to enable a more robust categorization.

Airborne measurements of aerosol optical properties related to early spring transport of mid-latitude sources into the Arctic

Directory of Open Access Journals (Sweden)

R. A. de Villiers

2010-06-01

Full Text Available Airborne lidar and in-situ measurements of the aerosol properties were conducted between Svalbard Island and Scandinavia in April 2008. Evidence of aerosol transport from Europe and Asia is given. The analysis of the aerosol optical properties based on a multiwavelength lidar (355, 532, 1064 nm including volume depolarization at 355 nm aims at distinguishing the role of the different aerosol sources (Siberian wild fires, Eastern Asia and European anthropogenic emissions. Combining, first aircraft measurements, second FLEXPART simulations with a calculation of the PBL air fraction originating from the three different mid-latitude source regions, and third level-2 CALIPSO data products (i.e. backscatter coefficient 532 nm,volume depolarization and color ratio between 1064 and 532 nm in aerosol layers along the transport pathways, appears a valuable approach to identify the role of the different aerosol sources even after a transport time larger than 4 days. Optical depth of the aerosol layers are always rather small (<4% while transported over the Arctic and ratio of the total attenuated backscatter (i.e. including molecular contribution provide more stable result than conventional aerosol backscatter ratio. Above Asia, CALIPSO data indicate more depolarization (up to 15% and largest color ratio (>0.5 for the northeastern Asia emissions (i.e. an expected mixture of Asian pollution and dust, while low depolarization together with smaller and quasi constant color ratio (≈0.3 are observed for the Siberian biomass burning emissions. A similar difference is visible between two layers observed by the aircraft above Scandinavia. The analysis of the time evolution of the aerosol optical properties revealed by CALIPSO between Asia and Scandinavia shows a gradual decrease of the aerosol backscatter, depolarization ratio and color ratio which suggests the removal of the largest particles in the accumulation mode. A similar study conducted for a European

Morphology, Composition, and Mixing State of Individual Aerosol Particles in Northeast China during Wintertime

Directory of Open Access Journals (Sweden)

Liang Xu

2017-02-01

Full Text Available Northeast China is located in a high latitude area of the world and undergoes a cold season that lasts six months each year. Recently, regional haze episodes with high concentrations of fine particles (PM2.5 have frequently been occurring in Northeast China during the heating period, but little information has been available. Aerosol particles were collected in winter at a site in a suburban county town (T1 and a site in a background rural area (T2. Morphology, size, elemental composition, and mixing state of individual aerosol particles were characterized by transmission electron microscopy (TEM. Aerosol particles were mainly composed of organic matter (OM and S-rich and certain amounts of soot and K-rich. OM represented the most abundant particles, accounting for 60.7% and 53.5% at the T1 and T2 sites, respectively. Abundant spherical OM particles were likely emitted directly from coal-burning stoves. Soot decreased from 16.9% at the T1 site to 4.6% at the T2 site and sulfate particles decrease from 35.9% at the T2 site to 15.7% at the T1 site, suggesting that long-range transport air masses experienced more aging processes and produced more secondary particles. Based on our investigations, we proposed that emissions from coal-burning stoves in most rural areas of the west part of Northeast China can induce regional haze episodes.

Measurement of Soot Deposition in Automotive Components Using Neutron Radiography

Energy Technology Data Exchange (ETDEWEB)

Zekveld, David; Liu, Liaohui [AMEC NSS, 700 University Ave, Toronto, Ontario, M5G 1X6 (Canada); UOIT, 2000 Simcoe Street North, Oshawa, Ontario, L1H 7K4 (Canada); Harrison, Andrew; Gill, Spencer; Harvel, Glenn [UOIT, 2000 Simcoe Street North, Oshawa, Ontario, L1H 7K4 (Canada); Chang, Jen-Shih [McMaster University, 1280 Main Street West, Hamilton, Ontario, L8S 4L8 (Canada)

2008-07-01

About 40% of air pollution is generated by vehicles and transportation. The particulate matter (PM) emission significantly impacts human health. Fine particles below 2.5 {mu}m (PM2.5) can enter the lungs and lead to respiratory problems. These particles not only influence human health, but also reduce the capability of many automobile exhaust heat exchanging devices. Neutron radiography is a non-destructive method of analyzing carbonaceous PM. While neutron radiography has been demonstrated for soot measurement in the past, the application has not considered the presence of unburned hydrocarbons, significant amounts of moisture nor examined complex geometrical configurations. The purpose of this work is to study a reliable non-destructive testing methodology using neutron radiography for measurement of soot distribution in automotive components. A soot standard (aluminium target) was designed and manufactured as a calibration tool. The standard is radiographed and used to measure the differences between various soot thickness and compositions. The radiograph images are analyzed to determine a calibration curve based upon the composition of the materials which can then be used for analysis of the automotive components. Experiments are performed using a diesel engine to produce soot deposits on exhaust piping. Soot distribution on exhaust piping is measured using neutron radiography. (authors)

Measurement of Soot Deposition in Automotive Components Using Neutron Radiography

International Nuclear Information System (INIS)

Zekveld, David; Liu, Liaohui; Harrison, Andrew; Gill, Spencer; Harvel, Glenn; Chang, Jen-Shih

2008-01-01

About 40% of air pollution is generated by vehicles and transportation. The particulate matter (PM) emission significantly impacts human health. Fine particles below 2.5 μm (PM2.5) can enter the lungs and lead to respiratory problems. These particles not only influence human health, but also reduce the capability of many automobile exhaust heat exchanging devices. Neutron radiography is a non-destructive method of analyzing carbonaceous PM. While neutron radiography has been demonstrated for soot measurement in the past, the application has not considered the presence of unburned hydrocarbons, significant amounts of moisture nor examined complex geometrical configurations. The purpose of this work is to study a reliable non-destructive testing methodology using neutron radiography for measurement of soot distribution in automotive components. A soot standard (aluminium target) was designed and manufactured as a calibration tool. The standard is radiographed and used to measure the differences between various soot thickness and compositions. The radiograph images are analyzed to determine a calibration curve based upon the composition of the materials which can then be used for analysis of the automotive components. Experiments are performed using a diesel engine to produce soot deposits on exhaust piping. Soot distribution on exhaust piping is measured using neutron radiography. (authors)

Optical properties of aerosols over a tropical rain forest in Xishuangbanna, South Asia

Science.gov (United States)

Ma, Yongjing; Xin, Jinyuan; Zhang, Wenyu; Wang, Yuesi

2016-09-01

Observation and analysis of the optical properties of atmospheric aerosols in a South Asian tropical rain forest showed that the annual mean aerosol optical depth (AOD) and aerosol Ångström exponent (α) at 500 nm were 0.47 ± 0.30 (± value represents the standard deviation) and 1.35 ± 0.32, respectively, from 2012 to 2014, similar with that of Amazon region. Aerosol optical properties in this region varied significantly between the dry and wet seasons. The mean AOD and α were 0.50 ± 0.32 and 1.41 ± 0.28, respectively, in the dry season and 0.41 ± 0.20 and 1.13 ± 0.41 in the wet season. Because of the combustion of the rich biomass in the dry season, fine modal smoke aerosols increased, which led to a higher AOD and smaller aerosol control mode than in the wet season. The average atmospheric humidity in the wet season was 85.50%, higher than the 79.67% during the dry season. In the very damp conditions of the wet season, the aerosol control mode was relatively larger, while AOD appeared to be lower because of the effect of aerosol hygroscopic growth and wet deposition. The trajectories were similar both in dry and wet, but with different effects on the aerosol concentration. The highest AOD values 0.66 ± 0.34 (in dry) and 0.45 ± 0.21 (in wet) both occurred in continental air masses, while smaller (0.38-0.48 in dry and 0.30-0.35 in wet) in oceanic air masses. The range of AOD values during the wet season was relatively narrow (0.30-0.45), but the dry season range was wider (0.38-0.66). For the Ångström exponent, the range in the wet season (0.74-1.34) was much greater than that in the dry season (1.33-1.54).

The pH-dependent adsorption of tributyltin to charcoals and soot

International Nuclear Information System (INIS)

Fang Liping; Borggaard, Ole K.; Marcussen, Helle; Holm, Peter E.; Bruun Hansen, Hans Christian

2010-01-01

Widespread use of tributyltin (TBT) poses a serious environmental problem. Adsorption by black carbon (BC) may strongly affect its behavior. The adsorption of TBT to well characterized soot and two charcoals with specific surface area in the range of 62-111 m 2 g -1 have been investigated with main focus on pH effects. The charcoals but not soot possess acidic functional groups. TBT adsorption reaches maximum at pH 6-7 for charcoals, and at pH > 6 for soot. Soot has between 1.5 and 15 times higher adsorption density (0.09-1.77 μmol m -2 ) than charcoals, but charcoals show up to 17 times higher sorption affinities than soot. TBT adsorption is successfully described by a new pH-dependent dual Langmuir model considering electrostatic and hydrophobic adsorption, and pH effects on TBT speciation and BC surface charge. It is inferred that strong sorption of the TBTOH species to BC may affect TBT toxicity. - Tributyltin adsorption to black carbon increases at increasing pH but charcoal exhibits electrostatic and hydrophobic adsorption, whereas soot only adsorbs hydrophobically.

Using the OMI aerosol index and absorption aerosol optical depth to evaluate the NASA MERRA Aerosol Reanalysis

Science.gov (United States)

Buchard, V.; da Silva, A. M.; Colarco, P. R.; Darmenov, A.; Randles, C. A.; Govindaraju, R.; Torres, O.; Campbell, J.; Spurr, R.

2015-05-01

A radiative transfer interface has been developed to simulate the UV aerosol index (AI) from the NASA Goddard Earth Observing System version 5 (GEOS-5) aerosol assimilated fields. The purpose of this work is to use the AI and aerosol absorption optical depth (AAOD) derived from the Ozone Monitoring Instrument (OMI) measurements as independent validation for the Modern Era Retrospective analysis for Research and Applications Aerosol Reanalysis (MERRAero). MERRAero is based on a version of the GEOS-5 model that is radiatively coupled to the Goddard Chemistry, Aerosol, Radiation, and Transport (GOCART) aerosol module and includes assimilation of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS) sensor. Since AI is dependent on aerosol concentration, optical properties and altitude of the aerosol layer, we make use of complementary observations to fully diagnose the model, including AOD from the Multi-angle Imaging SpectroRadiometer (MISR), aerosol retrievals from the AErosol RObotic NETwork (AERONET) and attenuated backscatter coefficients from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) mission to ascertain potential misplacement of plume height by the model. By sampling dust, biomass burning and pollution events in 2007 we have compared model-produced AI and AAOD with the corresponding OMI products, identifying regions where the model representation of absorbing aerosols was deficient. As a result of this study over the Saharan dust region, we have obtained a new set of dust aerosol optical properties that retains consistency with the MODIS AOD data that were assimilated, while resulting in better agreement with aerosol absorption measurements from OMI. The analysis conducted over the southern African and South American biomass burning regions indicates that revising the spectrally dependent aerosol absorption properties in the near-UV region improves the modeled-observed AI comparisons

Evaluation and application of passive and active optical remote sensing methods for the measurement of atmospheric aerosol properties

Energy Technology Data Exchange (ETDEWEB)

Mielonen, T.

2010-07-01

Atmospheric aerosol particles affect the atmosphere's radiation balance by scattering and absorbing sunlight. Moreover, the particles act as condensation nuclei for clouds and affect their reflectivity. In addition, aerosols have negative health effects and they reduce visibility. Aerosols are emitted into the atmosphere from both natural and anthropogenic sources. Different types of aerosols have different effects on the radiation balance, thus global monitoring and typing of aerosols is of vital importance. In this thesis, several remote sensing methods used in the measurement of atmospheric aerosols are evaluated. Remote sensing of aerosols can be done with active and passive instruments. Passive instruments measure radiation emitted by the sun and the Earth while active instruments have their own radiation source, for example a black body radiator or laser. The instruments utilized in these studies were sun photometers (PFR, Cimel), lidars (POLLYXT, CALIOP), transmissiometer (OLAF) and a spectroradiometer (MODIS). Retrieval results from spaceborne instruments (MODIS, CALIOP) were evaluated with ground based measurements (PFR, Cimel). In addition, effects of indicative aerosol model assumptions on the calculated radiative transfer were studied. Finally, aerosol particle mass at the ground level was approximated from satellite measurements and vertical profiles of aerosols measured with a lidar were analyzed. For the evaluation part, these studies show that the calculation of aerosol induced attenuation of radiation based on aerosol size distribution measurements is not a trivial task. In addition to dry aerosol size distribution, the effect of ambient relative humidity on the size distribution and the optical properties of the aerosols need to be known in order to achieve correct results from the calculations. Furthermore, the results suggest that aerosol size parameters retrieved from passive spaceborne measurements depend heavily on surgace reflectance

Contrasting aerosol optical and radiative properties between dust and urban haze episodes in megacities of Pakistan

Science.gov (United States)

Iftikhar, Muhammad; Alam, Khan; Sorooshian, Armin; Syed, Waqar Adil; Bibi, Samina; Bibi, Humera

2018-01-01

Satellite and ground based remote sensors provide vital information about aerosol optical and radiative properties. Analysis of aerosol optical and radiative properties during heavy aerosol loading events in Pakistan are limited and, therefore, require in-depth examination. This work examines aerosol properties and radiative forcing during Dust Episodes (DE) and Haze Episodes (HE) between 2010 and 2014 over mega cities of Pakistan (Karachi and Lahore). Episodes having the daily averaged values of Aerosol Optical Depth (AOD) exceeding 1 were selected. DE were associated with high AOD and low Ångström Exponent (AE) over Karachi and Lahore while high AOD and high AE values were associated with HE over Lahore. Aerosol volume size distributions (AVSD) exhibited a bimodal lognormal distribution with a noticeable coarse mode peak at a radius of 2.24 μm during DE, whereas a fine mode peak was prominent at a radius 0.25 μm during HE. The results reveal distinct differences between HE and DE for spectral profiles of several parameters including Single Scattering Albedo (SSA), ASYmmetry parameter (ASY), and the real and imaginary components of refractive index (RRI and IRI). The AOD-AE correlation revealed that dust was the dominant aerosol type during DE and that biomass burning and urban/industrial aerosol types were pronounced during HE. Aerosol radiative forcing (ARF) was estimated using the Santa Barbra DISORT Atmospheric Radiative Transfer (SBDART) model. Calculations revealed a negative ARF at the Top Of the Atmosphere (ARFTOA) and at the Bottom Of the Atmosphere (ARFBOA), with positive ARF within the Atmosphere (ARFATM) during both DE and HE over Karachi and Lahore. Furthermore, estimations of ARFATM by SBDART were shown to be in good agreement with values derived from AERONET data for DE and HE over Karachi and Lahore.

Optical properties and source analysis of aerosols over a desert area in Dunhuang, Northwest china

Science.gov (United States)

Ma, Yongjing; Xin, Jinyuan; Ma, Yining; Kong, Lingbin; Zhang, Kequan; Zhang, Wenyu; Wang, Yuesi; Wang, Xiuqin; Zhu, Yongfeng

2017-08-01

Aerosol observational data for 2012 obtained from Dunhuang Station of CARE-China (Campaign on Atmospheric Aerosol Research Network of China) were analyzed to achieve in-depth knowledge of aerosol optical properties over Dunhuang region. The results showed that the annual average aerosol optical depth (AOD) at 500 nm was 0.32±0.06, and the Ångström exponent ( α) was 0.73 ± 0.27. Aerosol optical properties revealed significant seasonal characteristics. Frequent sandstorms in MAM (March-April-May) resulted in the seasonal maximum AOD, 0.41 ± 0.04, and a relatively smaller α value, 0.44±0.04. The tourism seasons, JJA (June-July-August) and SON (September-October-November) coincide with serious emissions of small anthropogenic aerosols. While in DJF (December-January-February), the composition of the atmosphere was a mixture of dust particles and polluted aerosols released by domestic heating; the average AOD and α were 0.29 ± 0.02 and 0.66 ± 0.17, respectively. Different air masses exhibited different degrees of influence on the aerosol concentration over Dunhuang in different seasons. During MAM, ranges of AOD (0.11-1.18) and α (0.06-0.82) were the largest under the dust influence of northwest-short-distance air mass in the four trajectories. Urban aerosols transported by northwest-short-distance air mass accounted for a very large proportion in JJA and the mixed aerosols observed in SON were mainly conveyed by air masses from the west. In DJF, the similar ranges of AOD and α under the three air mass demonstrated the analogous diffusion effects on regional pollutants over Dunhuang.

Soot modeling of counterflow diffusion flames of ethylene-based binary mixture fuels

KAUST Repository

Wang, Yu; Raj, Abhijeet Dhayal; Chung, Suk-Ho

2015-01-01

of ethylene and its binary mixtures with methane, ethane and propane based on the method of moments. The soot model has 36 soot nucleation reactions from 8 PAH molecules including pyrene and larger PAHs. Soot surface growth reactions were based on a modified

A computational study of soot formation in opposed-flow diffusion flame interacting with vortices

KAUST Repository

Selvaraj, Prabhu

2017-01-05

The flame-vortex interaction enables the study of basic phenomena that control the coupling between combustion and turbulence. Employing a gas phase reaction mechanism considering polycyclic aromatic hydrocarbons (PAH), a two dimensional counterflow ethylene-air flame is simulated. A reduced mechanism with PAH pathways that includes until coronene and method of moments with interpolative closure (MOMIC) has been employed to calculate the soot characteristics. Interaction of sooting flame with a prescribed decaying random velocity field is being investigated. Counterflow nonpremixed flames at low strain rate sooting conditions are considered. Effects of vortices are studied on the flame structures and its sensitivity on the soot formation characteristics. As the vortex rolls up the flame, integrated soot volume fraction is found to be larger for the air-side vortex. A detailed analysis on the flame structure and its influence on the formation of soot were carried out. The results indicate that the larger PAH species contributes to the soot formation in the airside perturbation regimes, whereas the soot formation is dominated by the soot transport in fuel-side perturbation.

Effect of Dimethyl Ether Mixing on Soot Size Distribution in Premixed Ethylene Flame

KAUST Repository

Li, Zepeng

2016-01-01

As a byproduct of incomplete combustion, soot attracts increasing attentions as extensive researches exploring serious health and environmental effects from soot particles. Soot emission reduction requires a comprehensive understanding

Characterization of Dust Properties during ACE-Asia and PRIDE: A Column Satellite-Surface Perspective

Science.gov (United States)

Lau, William K. M. (Technical Monitor); Tsay, Si-Chee; Hsu, N. Christina; Herman, Jay R.; Ji, Q. Jack

2002-01-01

Many recent field experiments are designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally occurring aerosols, which often exist in high concentration over particular pathways around the globe. For example, the ACE-Asia (Aerosol Characterization Experiment-Asia) was conducted from March-May 2001 in the vicinity of the Taklimakan and Gobi deserts, East Coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). The PRIDE (Puerto RIco Dust Experiment, July 2000) was designed to measure the properties of Saharan dust transported across the Atlantic Ocean to the Caribbean. Dust particles typically originate in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of dust aerosols is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the ocean. During ACE-Asia and PRIDE we had measured aerosol physical/optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from ground-based remote sensing. The inclusion of flux measurements permits the determination of aerosol radiative flux in addition to measurements of loading and optical depth. At the time of the Terra/MODIS, SeaWiFS, TOMS and other satellite overpasses, these ground-based observations can provide valuable data to compare with satellite retrievals over land. We will present the results and discuss their implications in regional climatic effects.

Biomass burning plumes and the aging of black carbon aerosols in the tropopause region observed with the CARIBIC single particle soot photometer

Science.gov (United States)

Ditas, J.; Ma, N.; Zhang, Y.; Assmann, D. N.; Neumaier, M.; Wang, S.; Wang, J.; Zahn, A.; Hermann, M.; Brenninkmeijer, C. A. M.; Poeschl, U.; Su, H.; Cheng, Y.

2017-12-01

Biomass burning (BB) events can release large amounts of refractory black carbon (rBC) into the upper troposphere and lowermost stratosphere (UT/LMS) (Dahlkötter et al., 2014). To explore this effect, a Single Particle Soot Photometer (SP2) was added to the scientific payload of the instrumented CARIBIC container that is installed monthly in the cargo bay of a passenger aircraft (the IAGOS-CARIBIC atmospheric observatory, www.iagos.org). Regular measurement flights with different destinations are performed, covering an area of about 120°W to 120°E and 75°N to 30°S. A wide range of in situ measurements (CO, O3, greenhouse gases, aerosol particles and volatile organic compounds) is combined with a collection of air and aerosol samples for laboratory analyses. Since August 2014, the SP2 measures BC number and mass concentration at altitudes between 8 and 12 km. More than 600 BC measurement hours show a strong impact of BB emissions on the lowermost stratosphere. The BB plumes are identified with the help of concurrent carbon monoxide and acetonitrile measurements showing substantially increased concentrations compared to their background level. Transported into the lowermost stratosphere, BB smoke can be transported over long distances and the BC particles can stay in the atmosphere up to one year. The monthly missions of four consecutive CARIBIC flights sometimes enable to revisit a certain air mass, as was the case during a measurement flight to San Francisco in August 2014, with a stopover time of 2h. The revisited biomass burning plume located over the Altlantic ocean near Greenland was traced back by backward and forward trajectories to open fires in Canada (upper Fig.). The transit time of the smoke plume was estimated to 16 - 19h which perfectly matches our flight time difference ( 18h). Based on the LEO-fit method (Leading Edge Only fit) from Gao et al. (2007), the mixing state of the BC particles within the BB plume was calculated. Our unique data set

Implementation of two-equation soot flamelet models for laminar diffusion flames

Energy Technology Data Exchange (ETDEWEB)

Carbonell, D.; Oliva, A.; Perez-Segarra, C.D. [Centre Tecnologic de Transferencia de Calor (CTTC), Universitat Politecnica de Catalunya (UPC), ETSEIAT, Colom 11, E-08222, Terrassa (Barcelona) (Spain)

2009-03-15

The two-equation soot model proposed by Leung et al. [K.M. Leung, R.P. Lindstedt, W.P. Jones, Combust. Flame 87 (1991) 289-305] has been derived in the mixture fraction space. The model has been implemented using both Interactive and Non-Interactive flamelet strategies. An Extended Enthalpy Defect Flamelet Model (E-EDFM) which uses a flamelet library obtained neglecting the soot formation is proposed as a Non-Interactive method. The Lagrangian Flamelet Model (LFM) is used to represent the Interactive models. This model uses direct values of soot mass fraction from flamelet calculations. An Extended version (E-LFM) of this model is also suggested in which soot mass fraction reaction rates are used from flamelet calculations. Results presented in this work show that the E-EDFM predict acceptable results. However, it overpredicts the soot volume fraction due to the inability of this model to couple the soot and gas-phase mechanisms. It has been demonstrated that the LFM is not able to predict accurately the soot volume fraction. On the other hand, the extended version proposed here has been shown to be very accurate. The different flamelet mathematical formulations have been tested and compared using well verified reference calculations obtained solving the set of the Full Transport Equations (FTE) in the physical space. (author)

Wintertime Arctic Ocean sea water properties and primary marine aerosol concentrations

Directory of Open Access Journals (Sweden)

J. Zábori

2012-11-01

Full Text Available Sea spray aerosols are an important part of the climate system through their direct and indirect effects. Due to the diminishing sea ice, the Arctic Ocean is one of the most rapidly changing sea spray aerosol source areas. However, the influence of these changes on primary particle production is not known.

In laboratory experiments we examined the influence of Arctic Ocean water temperature, salinity, and oxygen saturation on primary particle concentration characteristics. Sea water temperature was identified as the most important of these parameters. A strong decrease in sea spray aerosol production with increasing water temperature was observed for water temperatures between −1°C and 9°C. Aerosol number concentrations decreased from at least 1400 cm⁻³ to 350 cm⁻³. In general, the aerosol number size distribution exhibited a robust shape with one mode close to dry diameter D_p 0.2 μm with approximately 45% of particles at smaller sizes. Changes in sea water temperature did not result in pronounced change of the shape of the aerosol size distribution, only in the magnitude of the concentrations. Our experiments indicate that changes in aerosol emissions are most likely linked to changes of the physical properties of sea water at low temperatures. The observed strong dependence of sea spray aerosol concentrations on sea water temperature, with a large fraction of the emitted particles in the typical cloud condensation nuclei size range, provide strong arguments for a more careful consideration of this effect in climate models.

Aerosol generation from Kerosene fires

International Nuclear Information System (INIS)

Jordan, S.; Lindner, W.

1981-01-01

The course of solvent surface fires is dependent on the surface area on fire; depth of pool and solvent composition do not influence the fire rate. But the fire rate increases rapidly with the burning area. The residual oxygen concentration after a fire in a closed container is dependent on the violence of the fire, i.e. on the burning surface. Moreover the ending of the fire is influenced by the TBP-concentration of the solvent. With sufficient supply of solvent the TBP-concentration changes only slightly during the fire, so that a fire at 14% O 2 -concentration is extinguished within the container. With the TBP-concentration changing considerably, i.e. little mass, a fire with a similar burning surface is already extinguished at an O 2 -content of 18%. The aerosol generation depends on the fire rate, and so it is higher in free atmosphere than in closed containers. The soot production in the mixture fire (kerosene /TBP 70/30) is higher by a factor 7 than in the pure kerosene fire. Primary soot-particles have a diameter of approximately 0,05 μm and agglomerate rapidly into aggregates of 0,2-0,4 μm. (orig.) [de

Fog-induced variations in aerosol optical and physical properties over the Indo-Gangetic Basin and impact to aerosol radiative forcing

Directory of Open Access Journals (Sweden)

S. K. Das

2008-06-01

Full Text Available A detailed study on the changes in aerosol physical and optical properties during fog events were made in December 2004 at Hissar (29.13° N, 75.70° E, a city located in the Indo-Gangetic basin. The visible aerosol optical depth was relatively low (0.3 during the initial days, which, however, increased (0.86 as the month progressed. The increasing aerosol amount, the decreasing surface temperature and a higher relative humidity condition were found favoring the formation of fog. The fog event is also found to alter the aerosol size distribution. An increase in the number concentration of the nucleation mode (radius<0.1 μm particles, along with a decrease in the mode radius showed the formation of freshly nucleated aerosols. In the case of accumulation mode (0.1 μmaerosol optical depth spectra are model fitted to infer the aerosol components which are further used to compute the aerosol radiative forcing. The top of the atmosphere forcing is found to increase during foggy days due to large backscattering of radiation back to space. It is also shown that during foggy days, as the day progresses the RH value decreases, which reduces the forcing value while the increasing solar elevation increases the forcing value. Thus the fog event which prolongs longer into the daytime has a stronger effect on the diurnally averaged aerosol radiative forcing than those events which are confined only to the early morning hours.

Fog-induced variations in aerosol optical and physical properties over the Indo-Gangetic Basin and impact to aerosol radiative forcing

Energy Technology Data Exchange (ETDEWEB)

Das, S.K.; Misra, A. [Physical Research Lab., Ahmedabad (India); Jayaraman, A. [National Atmospheric Research Lab., Gadanki (India)

2008-07-01

A detailed study on the changes in aerosol physical and optical properties during fog events were made in December 2004 at Hissar (29.13 N, 75.70 E), a city located in the Indo-Gangetic basin. The visible aerosol optical depth was relatively low (0.3) during the initial days, which, however, increased (0.86) as the month progressed. The increasing aerosol amount, the decreasing surface temperature and a higher relative humidity condition were found favoring the formation of fog. The fog event is also found to alter the aerosol size distribution. An increase in the number concentration of the nucleation mode (radius<0.1 {mu}m) particles, along with a decrease in the mode radius showed the formation of freshly nucleated aerosols. In the case of accumulation mode (0.1 {mu}maerosol optical depth spectra are model fitted to infer the aerosol components which are further used to compute the aerosol radiative forcing. The top of the atmosphere forcing is found to increase during foggy days due to large backscattering of radiation back to space. It is also shown that during foggy days, as the day progresses the RH value decreases, which reduces the forcing value while the increasing solar elevation increases the forcing value. Thus the fog event which prolongs longer into the daytime has a stronger effect on the diurnally averaged aerosol radiative forcing than those events which are confined only to the early morning hours. (orig.)

Size distributions and chemical properties of aerosol at Ny Ålesund, Svalbard

Science.gov (United States)

Covert, David S.; Heintzenberg, Jost

Physical and chemical parameters of the arctic aerosol were investigated at Ny Ålesund, Svalbard, in March and April 1989 in connection with the third Arctic Gas and Aerosol Project (AGASP III). The number size distribution of the particles was measured over the range of 0.02-1.0 μm. Filter samples were analysed for elemental composition and two integral chemical properties, hygroscopic growth and volatility, were measured. Along with the latter measurements, the distribution of these properties at specific particle sizes, i.e. the degree of internal mixing, was determined. Both clean, marine conditions and "arctic haze" episodes were included in the series of measurements. The number size distribution indicated that the aerosol was well aged based on its narrowness and the relative low concentration of nuclei mode particles. It had a number mode at 0.22 μm diameter and geometric standard deviation of 1.4. Generally the particles exhibited uniform hygroscopic growth properties, i.e. they were largely internally mixed. The growth factor was 1.45 at 90% relative humidity. Approximately 40% of the overall particulate mass was volatile at a temperature of 50°C. The volatile fraction varied form particle to particle, i.e. the particles were externally mixed with respect to volatility.

Role of Fluid-Dynamics in Soot Formation and Microstructure in Acetylene-Air Laminar Diffusion Flames

Directory of Open Access Journals (Sweden)

Praveen Pandey

2015-03-01

Full Text Available Residence time and thermo-chemical environment are important factors in the soot-formation process in flames. Studies have revealed that flow-dynamics plays a dominant role in soot formation process. For understanding the effect of flow dynamics on soot formation and physical structure of the soot formed in different combustion environments two types of laminar diffusion flames of Acetylene and air, a normal diffusion flame (NDF and an inverse diffusion flame (IDF have been investigated. The fuel and air supply in the reaction zone in two flame types were kept constant but the interchange of relative position of fuel and air altered the burner exit Reynolds and Froude numbers of gases, fuel/air velocity ratio and flame shape. Soot samples were collected using thermophoretic sampling on transmission electron microscope (TEM grids at different flame heights and were analyzed off-line in a Transmission Electron Microscope. Soot primary particle size, soot aggregate size and soot volume fraction were measured using an image analysis software. In NDF the maximum flame temperature was about 1525 K and 1230 K for IDF. The soot primary particles are distinctly smaller in size in IDF (between 19 – 26 nm compared to NDF (between 29–34 nm. Both NDF and IDF show chainlike branched structure of soot agglomerate with soot particles of a nearly spherical shape. The average number of soot primary particles per aggregate in NDF was in the range of 24 to 40 and in IDF it varied between 16 to 24. Soot volume fraction was between 0.6 to 1.5 ppm in NDF where as it was less than 0.2 ppm in IDF. The change in sooting characteristics of the two flame types is attributed to changed fuel/air velocity ratio, entrainment of gas molecules and thermophoresis on soot particles.

Aerosol properties over the Arabian Sea during the north east monsoon

Digital Repository Service at National Institute of Oceanography (India)

Suresh, T.; Dulac, F.; Leon, G.F.; Desa, E.

Knowledge of the variations of the aerosol properties is essential for the development of the satellite atmospheric correction algorithms. The measurements were carried-out during a cruise using a six channel spectral sun photometer at wavelengths...

Sun and aureole spectrometer for airborne measurements to derive aerosol optical properties.

Science.gov (United States)

Asseng, Hagen; Ruhtz, Thomas; Fischer, Jürgen

2004-04-01

We have designed an airborne spectrometer system for the simultaneous measurement of the direct Sun irradiance and aureole radiance. The instrument is based on diffraction grating spectrometers with linear image sensors. It is robust, lightweight, compact, and reliable, characteristics that are important for airborne applications. The multispectral radiation measurements are used to derive optical properties of tropospheric aerosols. We extract the altitude dependence of the aerosol volume scattering function and of the aerosol optical depth by using flight patterns with descents and ascents ranging from the surface level to the top of the boundary layer. The extinction coefficient and the product of single scattering albedo and phase function of separate layers can be derived from the airborne measurements.

The pH-dependent adsorption of tributyltin to charcoals and soot

Energy Technology Data Exchange (ETDEWEB)

Fang Liping, E-mail: fang@life.ku.d [Department of Basic Sciences and Environment, Faculty of Life Sciences, University of Copenhagen, Thorvaldsensvej 40, DK-1871 Frederiksberg C (Denmark); Borggaard, Ole K.; Marcussen, Helle; Holm, Peter E.; Bruun Hansen, Hans Christian [Department of Basic Sciences and Environment, Faculty of Life Sciences, University of Copenhagen, Thorvaldsensvej 40, DK-1871 Frederiksberg C (Denmark)

2010-12-15

Widespread use of tributyltin (TBT) poses a serious environmental problem. Adsorption by black carbon (BC) may strongly affect its behavior. The adsorption of TBT to well characterized soot and two charcoals with specific surface area in the range of 62-111 m{sup 2} g{sup -1} have been investigated with main focus on pH effects. The charcoals but not soot possess acidic functional groups. TBT adsorption reaches maximum at pH 6-7 for charcoals, and at pH > 6 for soot. Soot has between 1.5 and 15 times higher adsorption density (0.09-1.77 {mu}mol m{sup -2}) than charcoals, but charcoals show up to 17 times higher sorption affinities than soot. TBT adsorption is successfully described by a new pH-dependent dual Langmuir model considering electrostatic and hydrophobic adsorption, and pH effects on TBT speciation and BC surface charge. It is inferred that strong sorption of the TBTOH species to BC may affect TBT toxicity. - Tributyltin adsorption to black carbon increases at increasing pH but charcoal exhibits electrostatic and hydrophobic adsorption, whereas soot only adsorbs hydrophobically.

Biomass Burning Research Using DOE ARM Single-Particle Soot Photometer (SP2) Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Onasch, Timothy B [Aerodyne Research, Inc., Billerica, MA (United States); Sedlacek, Arthur J [Brookhaven National Lab. (BNL), Upton, NY (United States); Lewis, Ernie [Brookhaven National Lab. (BNL), Upton, NY (United States)

2017-03-01

The focus of this laboratory study was to investigate the chemical and optical properties, and the detection efficiencies, of tar balls generated in the laboratory using the same instruments deployed on the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility Gulfstream-1 (G-1) aircraft during the 2013 Biomass Burning Observation Project (BBOP) field study, during which tar balls were observed in wildland biomass burning particulate emissions. Key goals of this laboratory study were: (a) measuring the chemical composition of tar balls to provide insights into the atmospheric processes that form (evaporation/oxidation) and modify them in biomass burning plumes, (b) identifying whether tar balls contain refractory black carbon, (c) determining the collection efficiencies of tar balls impacting on the 600oC heated tungsten vaporizer in the Aerodyne Soot Particle Aerosol Mass Spectrometer (SP-AMS) (i.e., given the observed low volatilities, AMS measurements might underestimate organic biomass burning plume loadings), and (d) measuring the wavelength-dependent, mass-specific absorption cross-sections of brown carbon components of tar balls. This project was funded primarily by the DOE Atmospheric System Research (ASR) program, and the ARM Facility made their single-particle soot photometer (SP2) available for September 1-September 31, 2016 in the Aerodyne laboratories. The ARM mentor (Dr. Sedlacek) requested no funds for mentorship or data reduction. All ARM SP2 data collected as part of this project are archived in the ARM Data Archive in accordance with established protocols. The main objectives of the ARM Biomass Burning Observation Period (BBOP, July-October, 2013) field campaign were to (1) assess the impact of wildland fires in the Pacific Northwest on climate, through near-field and regional intensive measurement campaigns, and (2) investigate agricultural burns to determine how those biomass burn plumes differ from

Does variation in mineral composition alter the short-wave light scattering properties of desert dust aerosol?

International Nuclear Information System (INIS)

Smith, Andrew J.A.; Grainger, Roy G.

2014-01-01

Mineral dust aerosol is a major component of natural airborne particulates. Using satellite measurements from the visible and near-infrared, there is insufficient information to retrieve a full microphysical and chemical description of an aerosol distribution. As such, refractive index is one of many parameters that must be implicitly assumed in order to obtain an optical depth retrieval. This is essentially a proxy for the dust mineralogy. Using a global soil map, it is shown that as long as a reasonable refractive index for dust is assumed, global dust variability is unlikely to cause significant variation in the optical properties of a dust aerosol distribution in the short-wave, and so should not greatly affect retrievals of mineral dust aerosol from space by visible and near-infrared radiometers. Errors in aerosol optical depth due to this variation are expected to be ≲1%. The work is framed around the ORAC AATSR aerosol retrieval, but is equally applicable to similar satellite retrievals. In this case, variations in the top-of-atmosphere reflectance caused by mineral variation are within the noise limits of the instrument. -- Highlights: • Global variation in dust aerosol refractive index is quantified using soil maps. • Resulting visible light scattering properties have limited variability. • Satellite aerosol retrievals do not need to account for varying dust refractive indices

Diesel/biodiesel soot oxidation with ceo2 and ceo2-zro2-modified cordierites: a facile way of accounting for their catalytic ability in fuel combustion processes

Directory of Open Access Journals (Sweden)

Rodrigo F. Silva

2011-01-01

Full Text Available CeO2 and mixed CeO2-ZrO2 nanopowders were synthesized and efficiently deposited onto cordierite substrates, with the evaluation of their morphologic and structural properties through XRD, SEM, and FTIR. The modified substrates were employed as outer heterogeneous catalysts for reducing the soot originated from the diesel and diesel/biodiesel blends incomplete combustion. Their activity was evaluated in a diesel stationary motor, and a comparative analysis of the soot emission was carried out through diffuse reflectance spectroscopy. The analyses have shown that the catalyst-impregnated cordierite samples are very efficient for soot oxidation, being capable of reducing the soot emission in more than 60%.

Monthly and seasonal variations of aerosol optical properties and direct radiative forcing over Zanjan, Iran

Science.gov (United States)

Gharibzadeh, Maryam; Alam, Khan; Abedini, Yousefali; Bidokhti, Abbasali Aliakbari; Masoumi, Amir

2017-11-01

Aerosol optical properties and radiative forcing over Zanjan in northwest of Iran has been analyzed during 2010-2013. The aerosol optical and radiative properties are less studied over Zanjan, and therefore, require a careful and in depth analysis. The optical properties like Aerosol Optical Depth (AOD), Ångström Exponent (AE), ASYmmetry parameter (ASY), Single Scattering Albedo (SSA), and Aerosol Volume Size Distribution (AVSD) have been evaluated using the ground-based AErosol RObotic NETwork (AERONET) data. Higher AOD while relatively lower AE were observed in the spring and summer, which showed the presence of coarse mode particles in these seasons. An obvious increase of coarse mode particles in AVSD distribution, as well as a higher value of SSA represented considerable addition of coarse mode particles like dust into the atmosphere of Zanjan in these two seasons. Increase in AE, while a decrease in AOD was detected in the winter and fall. The presence of fine particles indicates the dominance of particles like urban-industrial aerosols from local sources especially in the winter. The Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model was utilized to calculate the Aerosol Radiative Forcing (ARF) at the Top of the Atmosphere (TOA), earth's surface and within the atmosphere. The annual averaged ARF values were -13.47 W m-2 and -36.1 W m-2 at the TOA and earth's surface, respectively, which indicate a significant cooling effect. Likewise, the ARF efficiencies at the TOA and earth's surface were -65.08 W m-2 and -158.43 W m-2, respectively. The annual mean atmospheric ARF and heating rate within the atmosphere were 22.63 W m-2 and 0.27 Kday-1 respectively, represented the warming effect within the atmosphere. Finally, a good agreement was found between AERONET retrieved ARF and SBDART simulated ARF.

Molecular Characterization of the Gas-Particle Interface of Soot Sampled from a Diesel Engine Using a Titration Method.

Science.gov (United States)

Tapia, A; Salgado, M S; Martín, María Pilar; Lapuerta, M; Rodríguez-Fernández, J; Rossi, M J; Cabañas, B

2016-03-15

Surface functional groups of two different types of combustion aerosols, a conventional diesel (EN 590) and a hydrotreated vegetable oil (HVO) soot, have been investigated using heterogeneous chemistry (i.e., gas-particle surface reactions). A commercial sample of amorphous carbon (Printex XE2-B) was analyzed as a reference substrate. A Knudsen flow reactor was used to carry out the experiments under molecular flow conditions. The selected gases for the titration experiments were: N(CH3)3 for the identification of acidic sites, NH2OH for the presence of carbonyl groups, CF3COOH and HCl for basic sites of different strength, and O3 and NO2 for reducing groups. Reactivity with N(CH3)3 indicates a lower density of acidic functionalities for Printex XE2-B in relation to diesel and HVO soot. Results for NH2OH experiments indicates that commercial amorphous carbon exhibits a lower abundance of available carbonyl groups at the interface compared to the results from diesel and HVO soot, the latter being the one with the largest abundance of carbonyl functions. Reactions with acids indicate the presence of weak basic oxides on the particle surface that preferentially interact with the strong acid CF3COOH. Finally, reactions with O3 and NO2 reveal that diesel and especially HVO have a significantly higher reactivity with both oxidizers compared to that of Printex XE2-B because they have more reducing sites by roughly a factor of 10 and 30, respectively. The kinetics of titration reactions have also been investigated.

Characterization of Dust Properties at the Source Region During ACE-Asia

Science.gov (United States)

Tsay, Si-Chee; Lau, William (Technical Monitor)

2001-01-01

ACE (Aerosol Characterization Experiment)-Asia is designed to study the compelling variability in spatial and temporal scale of both pollution-derived and naturally-occurring aerosols, which often exist in high concentrations over eastern Asia and along the rim of the western Pacific. The phase-I of ACE-Asia was conducted from March-May 2001 in the vicinity of the Gobi desert, east coast of China, Yellow Sea, Korea, and Japan, along the pathway of Kosa (severe events that blanket East Asia with yellow desert dust, peaked in the Spring season). Asian dust typically originates in desert areas far from polluted urban regions. During transport, dust layers can interact with anthropogenic sulfate and soot aerosols from heavily polluted urban areas. Added to the complex effects of clouds and natural marine aerosols, dust particles reaching the marine environment can have drastically different properties than those from the source. Thus, understanding the unique temporal and spatial variations of Asian dust is of special importance in regional-to-global climate issues such as radiative forcing, the hydrological cycle, and primary biological productivity in the mid-Pacific Ocean. During ACE-Asia we have measured continuously aerosol optical/radiative properties, column precipitable water amount, and surface reflectivity over homogeneous areas from surface. The inclusion of flux measurements permits the determination of dust aerosol radiative flux in addition to measurements of loading and optical thickness. At the time of the Terra/MODIS overpass, these ground-based observations can provide valuable data to compare with MODIS retrievals over land. Preliminary results will be presented and discussed their implications in regional climatic effects.

Optimal estimation retrieval of aerosol microphysical properties from SAGE II satellite observations in the volcanically unperturbed lower stratosphere

Directory of Open Access Journals (Sweden)

T. Deshler

2010-05-01

Full Text Available Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003. An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities, even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal size

Optimal estimation retrieval of aerosol microphysical properties from SAGE~II satellite observations in the volcanically unperturbed lower stratosphere

Science.gov (United States)

Wurl, D.; Grainger, R. G.; McDonald, A. J.; Deshler, T.

2010-05-01

Stratospheric aerosol particles under non-volcanic conditions are typically smaller than 0.1 μm. Due to fundamental limitations of the scattering theory in the Rayleigh limit, these tiny particles are hard to measure by satellite instruments. As a consequence, current estimates of global aerosol properties retrieved from spectral aerosol extinction measurements tend to be strongly biased. Aerosol surface area densities, for instance, are observed to be about 40% smaller than those derived from correlative in situ measurements (Deshler et al., 2003). An accurate knowledge of the global distribution of aerosol properties is, however, essential to better understand and quantify the role they play in atmospheric chemistry, dynamics, radiation and climate. To address this need a new retrieval algorithm was developed, which employs a nonlinear Optimal Estimation (OE) method to iteratively solve for the monomodal size distribution parameters which are statistically most consistent with both the satellite-measured multi-wavelength aerosol extinction data and a priori information. By thus combining spectral extinction measurements (at visible to near infrared wavelengths) with prior knowledge of aerosol properties at background level, even the smallest particles are taken into account which are practically invisible to optical remote sensing instruments. The performance of the OE retrieval algorithm was assessed based on synthetic spectral extinction data generated from both monomodal and small-mode-dominant bimodal sulphuric acid aerosol size distributions. For monomodal background aerosol, the new algorithm was shown to fairly accurately retrieve the particle sizes and associated integrated properties (surface area and volume densities), even in the presence of large extinction uncertainty. The associated retrieved uncertainties are a good estimate of the true errors. In the case of bimodal background aerosol, where the retrieved (monomodal) size distributions naturally

Studies of dry deposition of trace elements and diesel soot onto Lake Michigan and the Chesapeake Bay

International Nuclear Information System (INIS)

Ondov, J.M.; Caffrey, P.F.; Suarez, A.E.; Han, M.; Borgoul, P.V.

1995-01-01

As part of the Atmospheric Exchange Over Lakes and Oceans Study (AEOLOS) study, the University of Maryland participated in four intensive field campaigns, three on Lake Michigan (LM) and one on the Chesapeake Bay (CB), to determine the size distributions of potentially toxic elemental aerosol constituents, determine their sources, and their dry deposition loadings to surface waters. The work further seeks to elucidate the relative importance of constituents of fine- and coarse particles, as differentiation of these modes is essential to the eventual formation of control strategies. Unique components of the UMCP studies include (1) resolution of toxic elemental components of aerosol particles depositing to LM and CB by particle size and by source and (2) a Lake-wide evaluation of the importance of fine and coarse particle deposition to inorganic contamination of LM surface waters. In addition, a unique component of the Baltimore Study was the application of a sensitive iridium tracer to intentionally tag emissions form the City of Baltimore's sanitation truck fleet to tag the Baltimore urban plume and to determine the atmospheric behavior of diesel soot particles, a major source of urban carbon aerosol and the principle carrier of toxic polynuclear aromatic hydrocarbons. The work encompasses results for >40 elements by X-ray fluorescence and instrumental neutron activation analyses of more than 700 individual size-segregated aerosol, deposition, urban dust, and surface-water-suspended particulate samples. An overview of the results of these studies will be presented

Development and implementation of Intelligent Soot Blowing Optimization System for TNB Janamanjung

Directory of Open Access Journals (Sweden)

Sundaram Taneshwaren

2017-01-01

Full Text Available With an ever increasing demand for energy, Malaysia has become a nation that thrives on solid power generation sector to meet the energy demand and supply market. In a coal fired power plant, soot blowing operation is commonly used as a cleaning mechanism inside the boiler. There are many types of sequence available for this soot blowing operation. Hence, there is no efficient ways in utilizing the soot blowing operation to enhance the efficiency of boiler. Soot blowing optimization requires specific set of data preparation and simulation in order to achieve the best modal. Computational Fluid Dynamics (CFD is used to model a 700MW super-critical boiler, whereby parameters with effect to soot blowing operation is studied. Two different boiler condition is studied to analyze parameters in a clean and faulty boiler. Artificial Neural Network (ANN is used to train neural network modal with back propagation method to determine the best modal that will be used to predict soot blowing operation. Combination of neural network different number of neurons, hidden layers, training algorithm, and training functions is trained to find the modal with lowest error. By improving soot blowing sequence, efficiency of boiler can be improved by providing best parameter and model. This model is then used as a reference for advisory tool whereby a Neural Network Predictive Tool is suggested to the station to predict the soot blowing operation that occurs.

Effect of diluents on soot precursor formation and temperature in ethylene laminar diffusion flames

KAUST Repository

Abhinavam Kailasanathan, Ranjith Kumar

2013-03-01

Soot precursor species concentrations and flame temperature were measured in a diluted laminar co-flow jet diffusion flame at pressures up to eight atmospheres while varying diluent type. The objective of this study was to gain a better understanding of soot production and oxidation mechanisms, which could potentially lead to a reduction in soot emissions from practical combustion devices. Gaseous samples were extracted from the centerline of an ethylene-air laminar diffusion flame, which was diluted individually with four diluents (argon, helium, nitrogen, and carbon dioxide) to manipulate flame temperature and transport properties. The diluted fuel and co-flow exit velocities (top-hat profiles) were matched at all pressures to minimize shear-layer effects, and the mass fluxes were fixed over the pressure range to maintain constant Reynolds number. The flame temperature was measured using a fine gauge R-type thermocouple at pressures up to four atmospheres. Centerline concentration profiles of major non-fuel hydrocarbons collected via extractive sampling with a quartz microprobe and quantification using GC/MS+FID are reported within. The measured hydrocarbon species concentrations are vary dramatically with pressure and diluent, with the helium and carbon dioxide diluted flames yielding the largest and smallest concentrations of soot precursors, respectively. In the case of C2H2 and C6H6, two key soot precursors, helium diluted flames had concentrations more than three times higher compared with the carbon dioxide diluted flame. The peak flame temperature vary with diluents tested, as expected, with carbon dioxide diluted flame being the coolest, with a peak temperature of 1760K at 1atm, and the helium diluted flame being the hottest, with a peak temperature of 2140K. At four atmospheres, the helium diluted flame increased to 2240K, but the CO2 flame temperature increased more, decreasing the difference to approximately 250K. © 2012 The Combustion Institute.

Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B

Science.gov (United States)

Shinozuka, Y.; Clarke, A. D.; Decarlo, P. F.; Jimenez, J. L.; Dunlea, E. J.; Roberts, G. C.; Tomlinson, J. M.; Collins, D. R.; Howell, S. G.; Kapustin, V. N.; McNaughton, C. S.; Zhou, J.

2009-09-01

Remote sensing of cloud condensation nuclei (CCN) would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100 nm particles decreased with increasing organic fraction of non-refractory mass of submicron particles (OMF) as 0.34-0.20×OMF over Central Mexico and 0.47-0.43×OMF over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(-1/3), within measurement uncertainty (~20%). The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0-0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as -0.70×OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust). Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemical composition and CCN activity over Central Mexico.

Application of the direct simulation Monte Carlo method to nanoscale heat transfer between a soot particle and the surrounding gas

International Nuclear Information System (INIS)

Yang, M.; Liu, F.; Smallwood, G.J.

2004-01-01

Laser-Induced Incandescence (LII) technique has been widely used to measure soot volume fraction and primary particle size in flames and engine exhaust. Currently there is lack of quantitative understanding of the shielding effect of aggregated soot particles on its conduction heat loss rate to the surrounding gas. The conventional approach for this problem would be the application of the Monte Carlo (MC) method. This method is based on simulation of the trajectories of individual molecules and calculation of the heat transfer at each of the molecule/molecule collisions and the molecule/particle collisions. As the first step toward calculating the heat transfer between a soot aggregate and the surrounding gas, the Direct Simulation Monte Carlo (DSMC) method was used in this study to calculate the heat transfer rate between a single spherical aerosol particle and its cooler surrounding gas under different conditions of temperature, pressure, and the accommodation coefficient. A well-defined and simple hard sphere model was adopted to describe molecule/molecule elastic collisions. A combination of the specular reflection and completely diffuse reflection model was used to consider molecule/particle collisions. The results obtained by DSMC are in good agreement with the known analytical solution of heat transfer rate for an isolated, motionless sphere in the free-molecular regime. Further the DSMC method was applied to calculate the heat transfer in the transition regime. Our present DSMC results agree very well with published DSMC data. (author)

Flame experiments at the advanced light source: new insights into soot formation processes.

Science.gov (United States)

Hansen, Nils; Skeen, Scott A; Michelsen, Hope A; Wilson, Kevin R; Kohse-Höinghaus, Katharina

2014-05-26

The following experimental protocols and the accompanying video are concerned with the flame experiments that are performed at the Chemical Dynamics Beamline of the Advanced Light Source (ALS) of the Lawrence Berkeley National Laboratory(1-4). This video demonstrates how the complex chemical structures of laboratory-based model flames are analyzed using flame-sampling mass spectrometry with tunable synchrotron-generated vacuum-ultraviolet (VUV) radiation. This experimental approach combines isomer-resolving capabilities with high sensitivity and a large dynamic range(5,6). The first part of the video describes experiments involving burner-stabilized, reduced-pressure (20-80 mbar) laminar premixed flames. A small hydrocarbon fuel was used for the selected flame to demonstrate the general experimental approach. It is shown how species' profiles are acquired as a function of distance from the burner surface and how the tunability of the VUV photon energy is used advantageously to identify many combustion intermediates based on their ionization energies. For example, this technique has been used to study gas-phase aspects of the soot-formation processes, and the video shows how the resonance-stabilized radicals, such as C3H3, C3H5, and i-C4H5, are identified as important intermediates(7). The work has been focused on soot formation processes, and, from the chemical point of view, this process is very intriguing because chemical structures containing millions of carbon atoms are assembled from a fuel molecule possessing only a few carbon atoms in just milliseconds. The second part of the video highlights a new experiment, in which an opposed-flow diffusion flame and synchrotron-based aerosol mass spectrometry are used to study the chemical composition of the combustion-generated soot particles(4). The experimental results indicate that the widely accepted H-abstraction-C2H2-addition (HACA) mechanism is not the sole molecular growth process responsible for the formation

Aerosol Optical Properties at the Ground Sites during the 2010 CARES Field Campaign

Science.gov (United States)

Atkinson, D. B.; Radney, J. G.; Harworth, J. W.

2010-12-01

Preliminary results from the ground sites at the 2010 CARES field campaign (T0 near Sacramento, CA and T1 near Cool, CA) will be presented. A number of aerosol optical properties were measured at high time resolution for the four week study period using custom instruments. The aerosol extinction coefficient was measured at T0 using a cavity ring-down transmissometer (CRDT) at two wavelengths (532 and 1064 nm) and the aerosol scattering coefficient was measured at 532 nm using a Radiance Research M903 nephelometer. At T1, a new CRDT instrument was deployed that measured the extinction coefficient at three wavelengths (355, 532, and 1064 nm) for sub-10 μm (nominal) and sub-2.5 μm aerosols at ambient, elevated, and reduced relative humidity. A new type of custom nephelometer that measures the aerosol scattering coefficient at 532 nm using an array detector was also deployed at T1.

Changes in the physico-chemical properties of Amazonian aerosols from background conditions due to urban impacts in Central Amazonia.

Science.gov (United States)

Artaxo, P.; Barbosa, H. M.; Brito, J.; Carbone, S.; Fiorese, C.; Andre, B.; Rizzo, L. V.; Ditas, F.; Pöhlker, C.; Pöhlker, M. L.; Saturno, J.; Holanda, B. A.; Wang, J.; Souza, R. A. F. D.; Machado, L.; Andreae, M. O.; Martin, S. T.

2016-12-01

The GoAmazon 2014/15 experiment (Observations and Modeling of the Green Ocean Amazon) was a great opportunity to study how urbanization can change aerosol properties under pristine conditions in a tropical rain forest. The experiment took place from January 2014 to December 2015 in the vicinity of Manaus, Brazil, where several sampling stations were operated. Natural biogenic aerosol properties were studied in 3 sampling stations upwind of Manaus (ATTO (T0a), ZF2 (T0z) and EMBRAPA (T0e)). Urban impacted aerosols were analysed in two downwind sampling stations at Tiwa (T2) and Manacapuru (T3). Properties analysed were size distribution, scattering and absorption, composition, vertical profiles and others. Remote sensing measurements were done using AERONET and MODIS, while extensive ground based measurements were done in all sampling stations. Remote sensing measurements shows important changes in aerosol optical depth (AOD), especially in the aerosol absorption component. It was also observed a reduction in cloud droplet size downwind of Manaus for liquid phase clouds. Changes in particle number and size were also very significant, that reflected in changes in the aerosol radiative forcing (RF) before and after Manaus plume. In the dry season, an average RF of -24 w/m² was observed upwind, while -17 w/m² was observed downwind, due to large scale biomass burning aerosols. Single scattering albedo (SSA) at 550 nm changed from a high value of 0.96 upwind to 0.84 downwind due to the increase in absorbing aerosols in the wet season. In the dry season, SSA at 550nm changed from 0.95 to 0.87. Aerosol composition showed a large dominance of organic aerosols for all sites, accounting for 65-75% of PM1 non refractory aerosol. Most of these were secondary organic aerosol (SOA), with very low sulfate and nitrate concentrations. The influence of the Manaus plume on aerosol properties was more intense during the wet season, because in the dry season a significant amount of

Effect of NO2 and water on the catalytic oxidation of soot

DEFF Research Database (Denmark)

Christensen, Jakob Munkholt; Grunwaldt, Jan-Dierk; Jensen, Anker Degn

2017-01-01

The influence of adding NO2 to 10 vol% O2/N2 on non-catalytic soot oxidation and soot oxidation in intimate or loose contact with a catalyst has been investigated. In non-catalytic soot oxidation the oxidation rate is increased significantly at lower temperatures by NO2. For soot oxidation in tig...... exhibited a volcano-curve dependence on the heat of oxygen chemisorption, and among the tested pure metals and oxides Cr2O3 was the most active catalyst. Further improvements were achieved with a FeaCrbOx binary oxide catalyst....

Characterization of Diesel Soot Aggregates by Scattering and Extinction Methods

Science.gov (United States)

Kamimoto, Takeyuki

2006-07-01

Characteristics of diesel soot particles sampled from diesel exhaust of a common-rail turbo-charged diesel engine are quantified by scattering and extinction diagnostics using newly build two laser-based instruments. The radius of gyration representing the aggregates size is measured by the angular distribution of scattering intensity, while the soot mass concentration is measured by a two-wavelength extinction method. An approach to estimate the refractive index of diesel soot by an analysis of the extinction and scattering data using an aggregates scattering theory is proposed.

Characterization of Diesel Soot Aggregates by Scattering and Extinction Methods

International Nuclear Information System (INIS)

Kamimoto, Takeyuki

2006-01-01

Characteristics of diesel soot particles sampled from diesel exhaust of a common-rail turbo-charged diesel engine are quantified by scattering and extinction diagnostics using newly build two laser-based instruments. The radius of gyration representing the aggregates size is measured by the angular distribution of scattering intensity, while the soot mass concentration is measured by a two-wavelength extinction method. An approach to estimate the refractive index of diesel soot by an analysis of the extinction and scattering data using an aggregates scattering theory is proposed

Vertical Profiles of Aerosol Optical Properties Over Central Illinois and Comparison with Surface and Satellite Measurements

Science.gov (United States)

Sheridan P. J.; Andrews, E.; Ogren, J A.; Tackett, J. L.; Winker, D. M.

2012-01-01

Between June 2006 and September 2009, an instrumented light aircraft measured over 400 vertical profiles of aerosol and trace gas properties over eastern and central Illinois. The primary objectives of this program were to (1) measure the in situ aerosol properties and determine their vertical and temporal variability and (2) relate these aircraft measurements to concurrent surface and satellite measurements. Underflights of the CALIPSO satellite show reasonable agreement in a majority of retrieved profiles between aircraft-measured extinction at 532 nm (adjusted to ambient relative humidity) and CALIPSO-retrieved extinction, and suggest that routine aircraft profiling programs can be used to better understand and validate satellite retrieval algorithms. CALIPSO tended to overestimate the aerosol extinction at this location in some boundary layer flight segments when scattered or broken clouds were present, which could be related to problems with CALIPSO cloud screening methods. The in situ aircraft-collected aerosol data suggest extinction thresholds for the likelihood of aerosol layers being detected by the CALIOP lidar. These statistical data offer guidance as to the likelihood of CALIPSO's ability to retrieve aerosol extinction at various locations around the globe.

Investigations of the long-term effects of LII on soot and bath gas

KAUST Repository

Cenker, Emre

2017-08-24

A combination of high-repetition rate imaging, laser extinction measurements, two-colour soot pyrometry imaging, and high-resolution transmission electron microscopy of thermophoretically sampled soot is used to investigate the long-term and permanent effects of rapid heating of in-flame soot during laser-induced incandescence (LII). Experiments are carried out on a laminar non-premixed co-annular ethylene/air flame with various laser fluences. The high-repetition rate images clearly show that the heated and the neighbouring laser-border zones undergo a permanent transformation after the laser pulse, and advect vertically with the flow while the permanent marking is preserved. The soot volume fraction at the heated zone reduces due to the sublimation of soot and the subsequent enhanced oxidation. At the laser-border zones, however, optical thickness increases that may be due to thermophoretic forces drawing hot particles towards relatively cooler zones and the rapid compression of the bath gas induced by the pressure waves created by the expansion of the desorbed carbon clusters. Additionally sublimed carbon clusters can condense onto existing particles and contribute to increase of the optical thickness. Time-resolved two-colour pyrometry imaging show that the increased temperature of soot both in the heated and neighbouring laser-border zones persists for several milliseconds. This can be associated to the increase in the bath-gas temperature, and a change in the wavelength-dependent emissivity of soot particles induced by the thermal annealing of soot. Ex-situ analysis show that the lattice structure of the soot sampled at the laser-border zones tend to change and soot becomes more graphitic. This may be attributed to thermal annealing induced by elevated temperature.

Soot reduction under DC electric fields in counterflow non-premixed laminar ethylene flames

KAUST Repository

Park, Daegeun

2014-04-23

The effects of DC electric fields on non-premixed ethylene flames in a counterflow burner were studied experimentally with a focus on the reduction of soot particles. The experiment was conducted by connecting a high voltage terminal and a ground terminal to a lower (fuel) and upper (oxidizer) nozzle, respectively. We applied direct current (DC) potentials in a range of -5 kV < Vdc < 5 kV. Uniform electric fields were then generated in the gap between the two nozzles. The experimental conditions were selected to cover both soot formation (SF) and soot formation oxidation (SFO) flames. The flames subjected to the negative electric fields moved toward the fuel nozzle because of an ionic wind due to the Lorentz force acting on the positive ions in the flames. In addition, the yellow luminosity significantly decreased, indicating changes in the sooting characteristics. To analyze the sooting characteristics under the electric fields, planar laser induced incandescence (PLII) and fluorescence (PLIF) techniques were used to visualize the soot, polycyclic aromatic hydrocarbons (PAHs), and OH radicals. The sooting limits in terms of the fuel and oxygen mole fractions were measured. No substantial soot formation due to the effects of the DC electric fields for the tested range of voltages and reactant mole fractions could be identified. The detailed flame behaviors and sooting characteristics under the DC electric fields are discussed. Copyright © Taylor & Francis Group, LLC.

Source identification of individual soot agglomerates in Arctic air by transmission electron microscopy

Science.gov (United States)

Weinbruch, S.; Benker, N.; Kandler, K.; Schütze, K.; Kling, K.; Berlinger, B.; Thomassen, Y.; Drotikova, T.; Kallenborn, R.

2018-01-01

Individual soot agglomerates collected at four different locations on the Arctic archipelago Svalbard (Norway) were characterised by transmission electron microscopy and energy-dispersive X-ray microanalysis. For source identification of the ambient soot agglomerates, samples from different local sources (coal burning power plants in Longyearbyen and Barentsburg, diesel and oil burning for power generation in Sveagruva and Ny Ålesund, cruise ship) as well as from other sources which may contribute to Arctic soot concentrations (biomass burning, aircraft emissions, diesel engines) were investigated. Diameter and graphene sheet separation distance of soot primary particles were found to be highly variable within each source and are not suited for source identification. In contrast, concentrations of the minor elements Si, P, K, Ca and Fe showed significant differences which can be used for source attribution. The presence/absence of externally mixed particle groups (fly ashes, tar balls, mercury particles) gives additional hints about the soot sources. Biomass/wood burning, ship emissions and coal burning in Barentsburg can be excluded as major source for ambient soot at Svalbard. The coal power plant in Longyearbyen is most likely a major source of soot in the settlement of Longyearbyen but does not contribute significantly to soot collected at the Global Atmosphere Watch station Zeppelin Mountain near Ny Ålesund. The most probable soot sources at Svalbard are aircraft emissions and diesel exhaust as well as long range transport of coal burning emissions.

Role of soot in the transport of chlorine in hydrocarbon-air diffusion flames

International Nuclear Information System (INIS)

Venkatesh, S.; Saito, K.; Stencel, J.M.; Majidi, V.; Owens, M.

1991-01-01

Soot is an inevitable product of incomplete combustion in many practical combustion systems such as automobiles, incinerators and furnaces. Recent studies on chlorinated hydrocarbon combustion have shown that soot and other praticulates (eg. fly ash) play an important role in secondary reactions leading to the formation of chlorine substituted polyaromatic hydrocarbons (PAHs). In order to attain very high destruction efficiencies the fundamental chemical and physical processes that are associated with combustion, and post-combustion cleanup must be well understood. In order to understand the effect of chlorine on the soot formed in a combustion system, fundamental studies using a coflow laminar hydrocarbon-air diffusion flame have been carried out. Phenomenological studies have revealed the effect of chlorine on the visible structure of the flame. Soot inception activation energies were estimated for methane, ethane and ethylene diffusion flames for the case of with and without chlorine addition. No significant difference in the activation energy was estimated for either case. The effect of chlorine on the soot escape rate of an acetylene diffusion flame was estimated. The soot formed in these diffusion flames was analyzed for chlorine using scanning electron microscopy with energy dispersive spectroscopy (SEM/EDS) and by laser induced plasma spectroscopy (LIPS). REsults from these techniques indicate the presence of chlorine in the soot formed. In this paper a chemical scheme to explain the chlorine found in the soot is proposed based on known theories of soot formation

Aerosol optical properties in a rural environment near the mega-city Guangzhou, China: implications for regional air pollution, radiative forcing and remote sensing

Directory of Open Access Journals (Sweden)

Y. H. Zhang

2008-09-01

Full Text Available The scattering and absorption of solar radiation by atmospheric aerosols is a key element of the Earth's radiative energy balance and climate. The optical properties of aerosol particles are, however, highly variable and not well characterized, especially near newly emerging mega-cities. In this study, aerosol optical properties were measured at a rural site approximately 60 km northwest of the mega-city Guangzhou in southeast China. The measurements were part of the PRIDE-PRD2006 intensive campaign, covering the period of 1–30 July 2006. Scattering and absorption coefficients of dry aerosol particles with diameters up to 10 μm (PM₁₀ were determined with a three-wavelength integrating nephelometer and with a photoacoustic spectrometer, respectively.

Averaged over the measurement campaign (arithmetic mean ± standard deviation, the total scattering coefficients were 200±133 Mm⁻¹ (450 nm, 151±103 Mm⁻¹ (550 nm and 104±72 Mm⁻¹ (700 nm and the absorption coefficient was 34.3±26.5 Mm⁻¹ (532 nm. The average Ångström exponent was 1.46±0.21 (450 nm/700 nm and the average single scattering albedo was 0.82±0.07 (532 nm with minimum values as low as 0.5. The low single scattering albedo values indicate a high abundance, as well as strong sources, of light absorbing carbon (LAC. The ratio of LAC to CO concentration was highly variable throughout the campaign, indicating a complex mix of different combustion sources. The scattering and absorption coefficients, as well as the Ångström exponent and single scattering albedo, exhibited pronounced diurnal cycles, which can be attributed to boundary layer mixing effects and enhanced nighttime emissions of LAC (diesel soot from regulated truck traffic. The daytime average mid-visible single scattering albedo of 0.87 appears to be more suitable for climate modeling purposes than the 24-h average of 0.82, as the latter value is

Vertical profiles of aerosol optical properties over central Illinois and comparison with surface and satellite measurements

Directory of Open Access Journals (Sweden)

P. J. Sheridan

2012-12-01

Full Text Available Between June 2006 and September 2009, an instrumented light aircraft measured over 400 vertical profiles of aerosol and trace gas properties over eastern and central Illinois. The primary objectives of this program were to (1 measure the in situ aerosol properties and determine their vertical and temporal variability and (2 relate these aircraft measurements to concurrent surface and satellite measurements. The primary profile location was within 15 km of the NOAA/ESRL surface aerosol monitoring station near Bondville, Illinois. Identical instruments at the surface and on the aircraft ensured that the data from both platforms would be directly comparable and permitted a determination of how representative surface aerosol properties were of the lower column. Aircraft profiles were also conducted occasionally at two other nearby locations to increase the frequency of A-Train satellite underflights for the purpose of comparing in situ and satellite-retrieved aerosol data. Measurements of aerosol properties conducted at low relative humidity over the Bondville site compare well with the analogous surface aerosol data and do not indicate any major sampling issues or that the aerosol is radically different at the surface compared with the lowest flyby altitude of ~ 240 m above ground level. Statistical analyses of the in situ vertical profile data indicate that aerosol light scattering and absorption (related to aerosol amount decreases substantially with increasing altitude. Parameters related to the nature of the aerosol (e.g., single-scattering albedo, Ångström exponent, etc., however, are relatively constant throughout the mixed layer, and do not vary as much as the aerosol amount throughout the profile. While individual profiles often showed more variability, the median in situ single-scattering albedo was 0.93–0.95 for all sampled altitudes. Several parameters (e.g., submicrometer scattering fraction, hemispheric backscattering fraction, and

Comparative Study of Different Methods for Soot Sensing and Filter Monitoring in Diesel Exhausts

Science.gov (United States)

Feulner, Markus; Hagen, Gunter; Hottner, Kathrin; Redel, Sabrina; Müller, Andreas; Moos, Ralf

2017-01-01

Due to increasingly tighter emission limits for diesel and gasoline engines, especially concerning particulate matter emissions, particulate filters are becoming indispensable devices for exhaust gas after treatment. Thereby, for an efficient engine and filter control strategy and a cost-efficient filter design, reliable technologies to determine the soot load of the filters and to measure particulate matter concentrations in the exhaust gas during vehicle operation are highly needed. In this study, different approaches for soot sensing are compared. Measurements were conducted on a dynamometer diesel engine test bench with a diesel particulate filter (DPF). The DPF was monitored by a relatively new microwave-based approach. Simultaneously, a resistive type soot sensor and a Pegasor soot sensing device as a reference system measured the soot concentration exhaust upstream of the DPF. By changing engine parameters, different engine out soot emission rates were set. It was found that the microwave-based signal may not only indicate directly the filter loading, but by a time derivative, the engine out soot emission rate can be deduced. Furthermore, by integrating the measured particulate mass in the exhaust, the soot load of the filter can be determined. In summary, all systems coincide well within certain boundaries and the filter itself can act as a soot sensor. PMID:28218700

Comparative Study of Different Methods for Soot Sensing and Filter Monitoring in Diesel Exhausts.

Science.gov (United States)

Feulner, Markus; Hagen, Gunter; Hottner, Kathrin; Redel, Sabrina; Müller, Andreas; Moos, Ralf

2017-02-18

Due to increasingly tighter emission limits for diesel and gasoline engines, especially concerning particulate matter emissions, particulate filters are becoming indispensable devices for exhaust gas after treatment. Thereby, for an efficient engine and filter control strategy and a cost-efficient filter design, reliable technologies to determine the soot load of the filters and to measure particulate matter concentrations in the exhaust gas during vehicle operation are highly needed. In this study, different approaches for soot sensing are compared. Measurements were conducted on a dynamometer diesel engine test bench with a diesel particulate filter (DPF). The DPF was monitored by a relatively new microwave-based approach. Simultaneously, a resistive type soot sensor and a Pegasor soot sensing device as a reference system measured the soot concentration exhaust upstream of the DPF. By changing engine parameters, different engine out soot emission rates were set. It was found that the microwave-based signal may not only indicate directly the filter loading, but by a time derivative, the engine out soot emission rate can be deduced. Furthermore, by integrating the measured particulate mass in the exhaust, the soot load of the filter can be determined. In summary, all systems coincide well within certain boundaries and the filter itself can act as a soot sensor.

Comparative Study of Different Methods for Soot Sensing and Filter Monitoring in Diesel Exhausts

Directory of Open Access Journals (Sweden)

Markus Feulner

2017-02-01

Full Text Available Due to increasingly tighter emission limits for diesel and gasoline engines, especially concerning particulate matter emissions, particulate filters are becoming indispensable devices for exhaust gas after treatment. Thereby, for an efficient engine and filter control strategy and a cost-efficient filter design, reliable technologies to determine the soot load of the filters and to measure particulate matter concentrations in the exhaust gas during vehicle operation are highly needed. In this study, different approaches for soot sensing are compared. Measurements were conducted on a dynamometer diesel engine test bench with a diesel particulate filter (DPF. The DPF was monitored by a relatively new microwave-based approach. Simultaneously, a resistive type soot sensor and a Pegasor soot sensing device as a reference system measured the soot concentration exhaust upstream of the DPF. By changing engine parameters, different engine out soot emission rates were set. It was found that the microwave-based signal may not only indicate directly the filter loading, but by a time derivative, the engine out soot emission rate can be deduced. Furthermore, by integrating the measured particulate mass in the exhaust, the soot load of the filter can be determined. In summary, all systems coincide well within certain boundaries and the filter itself can act as a soot sensor.

[Optical properties of aerosol during haze-fog episodes in Beijing].

Science.gov (United States)

Yu, Xing-Na; Li, Xin-Mei; Deng, Zen-Grandeng; De, Qing-Yangzong; Yuan, Shuai

2012-04-01

The purpose of this study is to investigate the optical properties of aerosol during haze-fog episodes in Beijing. The aerosol optical depth (AOD), Angstrom exponent (alpha), size distribution and single scattering albedo (omega) during haze-fog episodes were analyzed between 2002 and 2008 using AERONENT data. During haze-fog episodes, the aerosol optical depth showed a decreasing trend with wavelengths, and showed high values with an average 1.34 at 440 nm. The magnitude of Angstrom exponent was relatively high during haze-fog episodes and the mean values reached 1.11. The frequency distribution of alpha was up to 94% when alpha > 0.9, indicating the predominance of fine particles during haze-fog episodes in Beijing. The aerosol volume size distributions presented a bimodal structure (fine and coarse modes). The maxima (peaks) radius of fine mode showed an increasing trend with AOD, however, those of coarse mode showed a decreasing trend with AOD. The size distribution showed a distinct difference in dominant mode for the different AOD. The single scattering albedo showed an increasing trend with AOD during haze-fog episodes in Beijing. The mean value of omega was 0.89 at the four wavelengths and the omega exhibited a low sensitivity to wavelengths.

Facile synthesis of nano cauliflower and nano broccoli like hierarchical superhydrophobic composite coating using PVDF/carbon soot particles via gelation technique.

Science.gov (United States)

Sahoo, Bichitra Nanda; Balasubramanian, Kandasubramanian

2014-12-15

We have elucidated a cost effective fabrication technique to produce superhydrophobic polyvinylidene fluoride (PVDF/DMF/candle soot particle and PVDF/DMF/camphor soot particle composite) porous materials. The water repellent dry composite was formed by the interaction of non-solvent (methanol) into PVDF/carbon soot particles suspension in N,N-dimethylformamide (DMF). It is seen that longer quenching time effectively changes the surface morphology of dry composites. The nano broccoli like hierarchical microstructure with micro or nano scaled roughen surface was obtained for PVDF/DMF/camphor soot particle, which reveals water contact angle of 172° with roll off angle of 2°. However, composite coating of PVDF/DMF/candle soot particle shows nano cauliflower like hierarchical, which illustrates water contact angle of 169° with roll off angle of 3°. To elucidate the enhancement of water repellent property of PVDF composites, we further divulge the evolution mechanism of nano cauliflower and nano broccoli structure. In order to evaluate the water contact angle of PVDF composites, surface diffusion of water inside the pores is investigated. Furthermore, the addition of small amount of carbon soot particles in composite not only provides the crystallization of PVDF, but also leads to dramatical amendment of surface morphology which increases the surface texture and roughness for superhydrophobicity. Copyright © 2014 Elsevier Inc. All rights reserved.

Asymptotic analysis soot model and experiment for a directed injection engine

Science.gov (United States)

Liu, Yongfeng; Pei, Pucheng; Xiong, Qinghui; Lu, Yong

2012-09-01

The existing soot models are either too complex and can not be applied to the internal combustion engine, or too simple to make calculation errors. Exploring the soot model becomes the pursuit of the goal of many researchers within the error range in the current computer speed. On the basis of the latest experimental results, TP (temperature phases) model is presented as a new soot model to carry out optimization calculation for a high-pressure common rail diesel engine. Temperature and excess air factor are the most important two parameters in this model. When zone temperature T0.6, only the soot precursors—polycyclic aromatic hydrocarbons(PAH) is created and there is no soot emission. When zone temperature T ⩾ 1 500 K and excess air factor Φinjection time, variation of rail pressure and variation of speed among TP models. The experimental results indicate that the TP model can carry out optimization and computational fluid dynamics can be a tool to calculate for a high-pressure common rail directed injection diesel engine. The TP model result is closer than the use of the original KIVA-3V results of soot model accuracy by about 50% and TP model gives a new method for engine researchers.

Facile Fabrication and Characterization of a PDMS-Derived Candle Soot Coated Stable Biocompatible Superhydrophobic and Superhemophobic Surface.

Science.gov (United States)

Iqbal, R; Majhy, B; Sen, A K

2017-09-13

We report a simple, inexpensive, rapid, and one-step method for the fabrication of a stable and biocompatible superhydrophobic and superhemophobic surface. The proposed surface comprises candle soot particles embedded in a mixture of PDMS+n-hexane serving as the base material. The mechanism responsible for the superhydrophobic behavior of the surface is explained, and the surface is characterized based on its morphology and elemental composition, wetting properties, mechanical and chemical stability, and biocompatibility. The effect of %n-hexane in PDMS, the thickness of the PDMS+n-hexane layer (in terms of spin coating speed) and sooting time on the wetting property of the surface is studied. The proposed surface exhibits nanoscale surface asperities (average roughness of 187 nm), chemical compositions of soot particles, very high water and blood repellency along with excellent mechanical and chemical stability and excellent biocompatibility against blood sample and biological cells. The water contact angle and roll-off angle is measured as 160° ± 1° and 2°, respectively, and the blood contact angle is found to be 154° ± 1°, which indicates that the surface is superhydrophobic and superhemophobic. The proposed superhydrophobic and superhemophobic surface offers significantly improved (>40%) cell viability as compared to glass and PDMS surfaces.

Empirical soot formation and oxidation model

Directory of Open Access Journals (Sweden)

Boussouara Karima

2009-01-01

Full Text Available Modelling internal combustion engines can be made following different approaches, depending on the type of problem to be simulated. A diesel combustion model has been developed and implemented in a full cycle simulation of a combustion, model accounts for transient fuel spray evolution, fuel-air mixing, ignition, combustion, and soot pollutant formation. The models of turbulent combustion of diffusion flame, apply to diffusion flames, which one meets in industry, typically in the diesel engines particulate emission represents one of the most deleterious pollutants generated during diesel combustion. Stringent standards on particulate emission along with specific emphasis on size of emitted particulates have resulted in increased interest in fundamental understanding of the mechanisms of soot particulate formation and oxidation in internal combustion engines. A phenomenological numerical model which can predict the particle size distribution of the soot emitted will be very useful in explaining the above observed results and will also be of use to develop better particulate control techniques. A diesel engine chosen for simulation is a version of the Caterpillar 3406. We are interested in employing a standard finite-volume computational fluid dynamics code, KIVA3V-RELEASE2.

Physicochemical properties of fine aerosols at Plan d'Aups during ESCOMPTE

Science.gov (United States)

Marinoni, Angela; Laj, Paolo; Deveau, Pierre Alexandre; Marino, Federica; Ghermandi, Grazia; Aulagnier, Fabien; Cachier, Hélène

2005-03-01

The physical and chemical properties of aerosol particles were investigated at Plan d'Aups, one of the ESCOMPTE sites located in the St. Baume mountain area (700 m a.s.l.), 50 km east of Marseilles (France). The site is ideally located for assessing the vertical and horizontal extent of the pollution plume from the Marseilles-Berre area. Our study showed that polluted air masses from the Marseilles-Berre area are advected to Plan d'Aups in the early afternoon. Average daily concentration of particles reaches up to 40 μg m -3 while 1-h average particle number concentration is greater than 30,000 cm -3. Most of the particle mass is composed of SO 42- and organic carbon (OC). The chemical properties of the particles revealed that an additional source, possibly from the industrial area of Gardanne, contributes to the aerosol mass. This last source is characterised by significant emissions of elements, such as Zn, V, Al and Si. In addition to transport, we found that gas-to-particle conversion takes place at the interface between the free troposphere and the boundary layer. We estimated that on average, 30% of the particle number is accounted for by direct nucleation. This is potentially a major aerosol source to the free troposphere.